The reformation of catalyst: From a trial-and-error synthesis to rational design

Yang, J. R.; Li, W. H.; Tang, H. T.; Pan, Y. M.; Wang, D. S.; Li, Y. D. CO₂-mediated organocatalytic chlorine evolution under industrial conditions. Nature 2023, 617, 519–523.

Smil, V. Detonator of the population explosion. Nature 1999, 400, 415–415.

Morawetz, H. Difficulties in the emergence of the polymer concept-an essay. Angew. Chem., Int. Ed. 1987, 26, 93–97.

Mülhaupt, R. Hermann staudinger and the origin of macromolecular chemistry. Angew. Chem., Int. Ed. 2004, 43, 1054–1063.

Wang, L. G.; Wang, D. S.; Li, Y. D. Single-atom catalysis for carbon neutrality. Carbon Energy 2022, 4, 1021–1079.

Baláž, P.; Achimovičová, M.; Baláž, M.; Billik, P.; Cherkezova-Zheleva, Z.; Criado, J. M.; Delogu, F.; Dutková, E.; Gaffet, E.; Gotor, F. J. et al. Hallmarks of mechanochemistry: From nanoparticles to technology. Chem. Soc. Rev. 2013, 42, 7571–7637.

Tan, C. L.; Cao, X. H.; Wu, X. J.; He, Q. Y.; Yang, J.; Zhang, X.; Chen, J. Z.; Zhao, W.; Han, S. K.; Nam, G. H. et al. Recent advances in ultrathin two-dimensional nanomaterials. Chem. Rev. 2017, 117, 6225–6331.

Wang, X.; Zhuang, J.; Peng, Q.; Li, Y. D. A general strategy for nanocrystal synthesis. Nature 2005, 437, 121–124.

Shi, Y. M.; Zhang, B. Recent advances in transition metal phosphide nanomaterials: Synthesis and applications in hydrogen evolution reaction. Chem. Soc. Rev. 2016, 45, 1529–1541.

Gao, J. H.; Gu, H. W.; Xu, B. Multifunctional magnetic nanoparticles: Design, synthesis, and biomedical applications. Acc. Chem. Res. 2009, 42, 1097–1107.

Gao, M. R.; Xu, Y. F.; Jiang, J.; Yu, S. H. Nanostructured metal chalcogenides: Synthesis, modification, and applications in energy conversion and storage devices. Chem. Soc. Rev. 2013, 42, 2986–3017.

Guo, S. J.; Dong, S. J. Graphene nanosheet: Synthesis, molecular engineering, thin film, hybrids, and energy and analytical applications. Chem. Soc. Rev. 2011, 40, 2644–2672.

Wang, G. F.; Peng, Q.; Li, Y. D. Lanthanide-doped nanocrystals: Synthesis, optical-magnetic properties, and applications. Acc. Chem. Res. 2011, 44, 322–332.

Xu, H. X.; Zeiger, B. W.; Suslick, K. S. Sonochemical synthesis of nanomaterials. Chem. Soc. Rev. 2013, 42, 2555–2567.

Qiao, B. T.; Wang, A. Q.; Yang, X. F.; Allard, L. F.; Jiang, Z.; Cui, Y. T.; Liu, J. Y.; Li, J.; Zhang, T. Single-atom catalysis of CO oxidation using Pt₁/FeO_x. Nat. Chem. 2011, 3, 634–641.

Wang, A. Q.; Li, J.; Zhang, T. Heterogeneous single-atom catalysis. Nat. Rev. Chem. 2018, 2, 65–81.

Wang, S. W.; Wang, L. G.; Wang, D. S.; Li, Y. D. Recent advances of single-atom catalysts in CO₂ conversion. Energy Environ. Sci. 2023, 16, 2759–2803.

Liang, X.; Fu, N. H.; Yao, S. C.; Li, Z.; Li, Y. D. The progress and outlook of metal single-atom-site catalysis. J. Am. Chem. Soc. 2022, 144, 18155–18174.

Xu, Q.; Guo, C. X.; Li, B. B.; Zhang, Z. D.; Qiu, Y. J.; Tian, S. B.; Zheng, L. R.; Gu, L.; Yan, W. S.; Wang, D. S. et al. Al³⁺ dopants induced Mg²⁺ vacancies stabilizing single-atom Cu catalyst for efficient free-radical hydrophosphinylation of alkenes. J. Am. Chem. Soc. 2022, 144, 4321–4326.

Chen, Y. J.; Jiang, B.; Hao, H. G.; Li, H. J.; Qiu, C. Y.; Liang, X.; Qu, Q. Y.; Zhang, Z. D.; Gao, R.; Duan, D. M. et al. Atomic-level regulation of cobalt single-atom nanozymes: Engineering high-efficiency catalase mimics. Angew. Chem., Int. Ed. 2023, 62, e202301879.

Ji, S. F.; Chen, Y. J.; Wang, X. L.; Zhang, Z. D.; Wang, D. S.; Li, Y. D. Chemical synthesis of single atomic site catalysts. Chem. Rev. 2020, 120, 11900–11955.

Chen, Y. J.; Ji, S. F.; Chen, C.; Peng, Q.; Wang, D. S.; Li, Y. D. Single-atom catalysts: Synthetic strategies and electrochemical applications. Joule 2018, 2, 1242–1264.

Lang, R.; Du, X. R.; Huang, Y. K.; Jiang, X. Z.; Zhang, Q.; Guo, Y. L.; Liu, K. P.; Qiao, B. T.; Wang, A. Q.; Zhang, T. Single-atom catalysts based on the metal-oxide interaction. Chem. Rev. 2020, 120, 11986–12043.

Zhuo, H. Y.; Zhang, X.; Liang, J. X.; Yu, Q.; Xiao, H.; Li, J. Theoretical understandings of graphene-based metal single-atom catalysts: Stability and catalytic performance. Chem. Rev. 2020, 120, 12315–12341.

Gao, C.; Low, J.; Long, R.; Kong, T. T.; Zhu, J. F.; Xiong, Y. J. Heterogeneous single-atom photocatalysts: Fundamentals and applications. Chem. Rev. 2020, 120, 12175–12216.

Wei, Y. S.; Zhang, M.; Zou, R. Q.; Xu, Q. Metal-organic framework-based catalysts with single metal sites. Chem. Rev. 2020, 120, 12089–12174.

Qin, R. X.; Liu, K. L.; Wu, Q. Y.; Zheng, N. F. Surface coordination chemistry of atomically dispersed metal catalysts. Chem. Rev. 2020, 120, 11810–11899.

Kaiser, S. K.; Chen, Z. P.; Akl, D. F.; Mitchell, S.; Pérez-Ramírez, J. Single-atom catalysts across the periodic table. Chem. Rev. 2020, 120, 11703–11809.

Seh, Z. W.; Kibsgaard, J.; Dickens, C. F.; Chorkendorff, I.; Nørskov, J. K.; Jaramillo, T. F. Combining theory and experiment in electrocatalysis: Insights into materials design. Science 2017, 355, eaad4998.

Suen, N. T.; Hung, S. F.; Quan, Q.; Zhang, N.; Xu, Y. J.; Chen, H. M. Electrocatalysis for the oxygen evolution reaction: Recent development and future perspectives. Chem. Soc. Rev. 2017, 46, 337–365.

Shao, M. H.; Chang, Q. W.; Dodelet, J. P.; Chenitz, R. Recent advances in electrocatalysts for oxygen reduction reaction. Chem. Rev. 2016, 116, 3594–3657.

Hong, W. T.; Risch, M.; Stoerzinger, K. A.; Grimaud, A.; Suntivich, J.; Shao-Horn, Y. Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis. Energy Environ. Sci. 2015, 8, 1404–1427.

Wang, Y.; Zheng, M.; Li, Y. R.; Ye, C. L.; Chen, J.; Ye, J. Y.; Zhang, Q. H.; Li, J.; Zhou, Z. Y.; Fu, X. Z. et al. p-d orbital hybridization induced by a monodispersed Ga site on a Pt₃Mn nanocatalyst boosts ethanol electrooxidation. Angew. Chem., Int. Ed. 2022, 61, e202115735.

Hoffmann, M. R.; Martin, S. T.; Choi, W.; Bahnemann, D. W. Environmental applications of semiconductor photocatalysis. Chem. Rev. 1995, 95, 69–96.

Asahi, R.; Morikawa, T.; Ohwaki, T.; Aoki, K.; Taga, Y. Visible-light photocatalysis in nitrogen-doped titanium oxides. Science 2001, 293, 269–271.

Ong, W. J.; Tan, L. L.; Ng, Y. H.; Yong, S. T.; Chai, S. P. Graphitic carbon nitride (g-C₃N₄)-based photocatalysts for artificial photosynthesis and environmental remediation: Are we a step closer to achieving sustainability. Chem. Rev. 2016, 116, 7159–7329.

Fox, M. A.; Dulay, M. T. Heterogeneous photocatalysis. Chem. Rev. 1993, 93, 341–357.

Wang, G.; Chen, Z.; Wang, T.; Wang, D. S.; Mao, J. J. P and Cu dual sites on graphitic carbon nitride for photocatalytic CO₂ reduction to hydrocarbon fuels with high C₂H₆ evolution. Angew. Chem., Int. Ed. 2022, 61, e202210789.

Wang, G.; Wu, Y.; Li, Z. J.; Lou, Z. Z.; Chen, Q. Q.; Li, Y. F.; Wang, D. S.; Mao, J. J. Engineering a copper single-atom electron bridge to achieve efficient photocatalytic CO₂ conversion. Angew. Chem., Int. Ed. 2023, 62, e202218460.

Tackett, B. M.; Gomez, E.; Chen, J. G. Net reduction of CO₂ via its thermocatalytic and electrocatalytic transformation reactions in standard and hybrid processes. Nat. Catal. 2019, 2, 381–386.

Meng, X. G.; Cui, X. J.; Rajan, N. P.; Yu, L.; Deng, D. H.; Bao, X. H. Direct methane conversion under mild condition by thermo-, electro-, or photocatalysis. Chem 2019, 5, 2296–2325.

Zhang, F. F.; Zhu, Y. L.; Lin, Q.; Zhang, L.; Zhang, X. W.; Wang, H. T. Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis. Energy Environ. Sci. 2021, 14, 2954–3009.

Meng, G.; Lan, W.; Zhang, L. L.; Wang, S. B.; Zhang, T. H.; Zhang, S.; Xu, M.; Wang, Y.; Zhang, J.; Yue, F. X. et al. Synergy of single atoms and lewis acid sites for efficient and selective lignin disassembly into monolignol derivatives. J. Am. Chem. Soc. 2023, 145, 12884–12893.

Ning, S. B.; Ou, H. H.; Li, Y. G.; Lv, C. C.; Wang, S. F.; Wang, D. S.; Ye, J. H. Co⁰–Co^δ+ interface double-site-mediated C–C coupling for the photothermal conversion of CO₂ into light olefins. Angew. Chem., Int. Ed. 2023, 62, e202302253.

Ling, C. Y.; Cui, Y.; Lu, S. H.; Bai, X. W.; Wang, J. L. How computations accelerate electrocatalyst discovery. Chem 2022, 8, 1575–1610.

Chun, H.; Lee, E.; Nam, K.; Jang, J. H.; Kyoung, W.; Noh, S. H.; Han, B. First-principle-data-integrated machine-learning approach for high-throughput searching of ternary electrocatalyst toward oxygen reduction reaction. Chem Catal. 2021, 1, 855–869.

Yang, J. R.; Li, W. H.; Wang, D. S. Machine learning: The trends of developing high-efficiency single-atom materials. Chem Catal. 2021, 1, 24–26.

Tang, B. J.; Lu, Y. H.; Zhou, J. D.; Chouhan, T.; Wang, H.; Golani, P.; Xu, M. Z.; Xu, Q.; Guan, C. T.; Liu, Z. Machine learning-guided synthesis of advanced inorganic materials. Mater. Today 2020, 41, 72–80.

Raccuglia, P.; Elbert, K. C.; Adler, P. D. F.; Falk, C.; Wenny, M. B.; Mollo, A.; Zeller, M.; Friedler, S. A.; Schrier, J.; Norquist, A. J. Machine-learning-assisted materials discovery using failed experiments. Nature 2016, 533, 73–76.

Brent, J. R.; Savjani, N.; O'Brien, P. Synthetic approaches to two-dimensional transition metal dichalcogenide nanosheets. Prog. Mater. Sci. 2017, 89, 411–478.

Chen, Y.; Fan, Z. X.; Zhang, Z. C.; Niu, W. X.; Li, C. L.; Yang, N. L.; Chen, B.; Zhang, H. Two-dimensional metal nanomaterials: Synthesis, properties, and applications. Chem. Rev. 2018, 118, 6409–6455.

Li, J.; Jing, X. C.; Li, Q. Q.; Li, S. W.; Gao, X.; Feng, X.; Wang, B. Bulk COFs and COF nanosheets for electrochemical energy storage and conversion. Chem. Soc. Rev. 2020, 49, 3565–3604.

Dong, R. H.; Zhang, T.; Feng, X. L. Interface-assisted synthesis of 2D materials: Trend and challenges. Chem. Rev. 2018, 118, 6189–6235.

Feinle, A.; Elsaesser, M. S.; Hüsing, N. Sol-gel synthesis of monolithic materials with hierarchical porosity. Chem. Soc. Rev. 2016, 45, 3377–3399.

Ma, R. Z.; Sasaki, T. Nanosheets of oxides and hydroxides: Ultimate 2D charge-bearing functional crystallites. Adv. Mater. 2010, 22, 5082–5104.

Mei, J.; Liao, T.; Kou, L. Z.; Sun, Z. Q. Two-dimensional metal oxide nanomaterials for next-generation rechargeable batteries. Adv. Mater. 2017, 29, 1700176.

Nicolosi, V.; Chhowalla, M.; Kanatzidis, M. G.; Strano, M. S.; Coleman, J. N. Liquid exfoliation of layered materials. Science 2013, 340, 1226419.

Coleman, J. N.; Lotya, M.; O’Neill, A.; Bergin, S. D.; King, P. J.; Khan, U.; Young, K.; Gaucher, A.; De, S.; Smith, R. J. et al. Two-dimensional nanosheets produced by liquid exfoliation of layered materials. Science 2011, 331, 568–571.

Abid, N.; Khan, A. M.; Shujait, S.; Chaudhary, K.; Ikram, M.; Imran, M.; Haider, J.; Khan, M.; Khan, Q.; Maqbool, M. Synthesis of nanomaterials using various top-down and bottom-up approaches, influencing factors, advantages, and disadvantages: A review. Adv. Colloid Interface Sci. 2022, 300, 102597.

Schiøtz, J.; Di Tolla, F. D.; Jacobsen, K. W. Softening of nanocrystalline metals at very small grain sizes. Nature 1998, 391, 561–563.

Pietryga, J. M.; Park, Y. S.; Lim, J.; Fidler, A. F.; Bae, W. K.; Brovelli, S.; Klimov, V. I. Spectroscopic and device aspects of nanocrystal quantum dots. Chem. Rev. 2016, 116, 10513–10622.

Melnychuk, C.; Guyot-Sionnest, P. Multicarrier dynamics in quantum dots. Chem. Rev. 2021, 121, 2325–2372.

Xia, Y.; Chen, W.; Zhang, P.; Liu, S. S.; Wang, K.; Yang, X. K.; Tang, H. D.; Lian, L. Y.; He, J. G.; Liu, X. X. et al. Facet control for trap-state suppression in colloidal quantum dot solids. Adv. Funct. Mater. 2020, 30, 2000594.

Xia, Y.; Liu, S. S.; Wang, K.; Yang, X. K.; Lian, L. Y.; Zhang, Z. M.; He, J. G.; Liang, G. J.; Wang, S.; Tan, M. L. et al. Cation-exchange synthesis of highly monodisperse PbS quantum dots from ZnS nanorods for efficient infrared solar cells. Adv. Funct. Mater. 2020, 30, 1907379.

Fan, J. Z.; Andersen, N. T.; Biondi, M.; Todorović, P.; Sun, B.; Ouellette, O.; Abed, J.; Sagar, L. K.; Choi, M. J.; Hoogland, S. et al. Mixed lead halide passivation of quantum dots. Adv. Mater. 2019, 31, 1904304.

Wang, R. L.; Wu, X.; Xu, K. M.; Zhou, W. J.; Shang, Y. Q.; Tang, H. Y.; Chen, H.; Ning, Z. J. Highly efficient inverted structural quantum dot solar cells. Adv. Mater. 2018, 30, 1704882.

Yang, J.; Ling, T.; Wu, W. T.; Liu, H.; Gao, M. R.; Ling, C.; Li, L.; Du, X. W. A top-down strategy towards monodisperse colloidal lead sulphide quantum dots. Nat. Commun. 2013, 4, 1695.

Tavakoli, M. M.; Dastjerdi, H. T.; Yadav, P.; Prochowicz, D.; Si, H. Y.; Tavakoli, R. Ambient stable and efficient monolithic tandem perovskite/PbS quantum dots solar cells via surface passivation and light management strategies. Adv. Funct. Mater. 2021, 31, 2010623.

Wang, Y.; Liu, X. Q.; Liu, J.; Han, B.; Hu, X. Q.; Yang, F.; Xu, Z. W.; Li, Y. C.; Jia, S. R.; Li, Z. et al. Carbon quantum dot implanted graphite carbon nitride nanotubes: Excellent charge separation and enhanced photocatalytic hydrogen evolution. Angew. Chem., Int. Ed. 2018, 57, 5765–5771.

Jin, Y. C.; Hu, C. G.; Dai, Q. B.; Xiao, Y.; Lin, Y.; Connell, J. W.; Chen, F. Y.; Dai, L. M. High-performance Li-CO₂ batteries based on metal-free carbon quantum dot/holey graphene composite catalysts. Adv. Funct. Mater. 2018, 28, 1804630.

Younis, A.; Hu, L.; Sharma, P.; Lin, C. H.; Mi, Y.; Guan, X. W.; Zhang, D. W.; Wang, Y. T.; He, T. Y.; Liu, X. F. et al. Enhancing resistive switching performance and ambient stability of hybrid perovskite single crystals via embedding colloidal quantum dots. Adv. Funct. Mater. 2020, 30, 2002948.

Arancibia, V.; Valderrama, M.; Silva, K.; Tapia, T. Determination of chromium in urine samples by complexation-supercritical fluid extraction and liquid or gas chromatography. J. Chromatogr. B 2003, 785, 303–309.

Bottini, M.; Balasubramanian, C.; Dawson, M. I.; Bergamaschi, A.; Bellucci, S.; Mustelin, T. Isolation and characterization of fluorescent nanoparticles from pristine and oxidized electric arc-produced single-walled carbon nanotubes. J. Phys. Chem. B 2006, 110, 831–836.

Lim, S. Y.; Shen, W.; Gao, Z. Q. Carbon quantum dots and their applications. Chem. Soc. Rev. 2015, 44, 362–381.

Bouzas-Ramos, D.; Canga, J. C.; Mayo, J. C.; Sainz, R. M.; Encinar, J. R.; Costa-Fernandez, J. M. Carbon quantum dots codoped with nitrogen and lanthanides for multimodal imaging. Adv. Funct. Mater. 2019, 29, 1903884.

Zhang, G.; Ji, Q. H.; Wu, Z.; Wang, G. C.; Liu, H. J.; Qu, J. H.; Li, J. H. Facile “spot-heating” synthesis of carbon dots/carbon nitride for solar hydrogen evolution synchronously with contaminant decomposition. Adv. Funct. Mater. 2018, 28, 1706462.

Zhou, S. J.; Tang, R.; Yin, L. W. Slow-photon-effect-induced photoelectrical-conversion efficiency enhancement for carbon-quantum-dot-sensitized inorganic CsPbBr₃ inverse opal perovskite solar cells. Adv. Mater. 2017, 29, 1703682.

Wang, Z. F.; Yuan, F. L.; Li, X. H.; Li, Y. C.; Zhong, H. Z.; Fan, L. Z.; Yang, S. H. 53% efficient red emissive carbon quantum dots for high color rendering and stable warm white-light-emitting diodes. Adv. Mater. 2017, 29, 1702910.

Li, W. D.; Liu, Y.; Wu, M.; Feng, X. L.; Redfern, S. A. T.; Shang, Y.; Yong, X.; Feng, T. L.; Wu, K. F.; Liu, Z. Y. et al. Carbon-quantum-dots-loaded ruthenium nanoparticles as an efficient electrocatalyst for hydrogen production in alkaline media. Adv. Mater. 2018, 30, 1800676.

Hills, G.; Lau, C.; Wright, A.; Fuller, S.; Bishop, M. D.; Srimani, T.; Kanhaiya, P.; Ho, R.; Amer, A.; Stein, Y. et al. Modern microprocessor built from complementary carbon nanotube transistors. Nature 2019, 572, 595–602.

Bai, Y. X.; Zhang, R. F.; Ye, X.; Zhu, Z. X.; Xie, H. H.; Shen, B. Y.; Cai, D. L.; Liu, B. F.; Zhang, C. X.; Jia, Z. et al. Carbon nanotube bundles with tensile strength over 80 GPa. Nat. Nanotechnol. 2018, 13, 589–595.

Yang, F.; Wang, X.; Zhang, D. Q.; Yang, J.; Luo, D.; Xu, Z. W.; Wei, J. K.; Wang, J. Q.; Xu, Z.; Peng, F. et al. Chirality-specific growth of single-walled carbon nanotubes on solid alloy catalysts. Nature 2014, 510, 522–524.

Zhuang, T. T.; Li, Y.; Gao, X. Q.; Wei, M. Y.; De Arquer, F. P. G.; Todorović, P.; Tian, J.; Li, G. P.; Zhang, C.; Li, X. Y. et al. Regioselective magnetization in semiconducting nanorods. Nat. Nanotechnol. 2020, 15, 192–197.

Zhou, G. M.; Xu, L.; Hu, G. W.; Mai, L.; Cui, Y. Nanowires for electrochemical energy storage. Chem. Rev. 2019, 119, 11042–11109.

Wang, D. F.; Bao, D. L.; Zheng, Q.; Wang, C. T.; Wang, S. Y.; Fan, P.; Mishra, S.; Tao, L.; Xiao, Y.; Huang, L. et al. Twisted bilayer zigzag-graphene nanoribbon junctions with tunable edge states. Nat. Commun. 2023, 14, 1018.

Christoff-Tempesta, T.; Cho, Y.; Kim, D. Y.; Geri, M.; Lamour, G.; Lew, A. J.; Zuo, X. B.; Lindemann, W. R.; Ortony, J. H. Self-assembly of aramid amphiphiles into ultra-stable nanoribbons and aligned nanoribbon threads. Nat. Nanotechnol. 2021, 16, 447–454.

Cheung, K. Y.; Watanabe, K.; Segawa, Y.; Itami, K. Synthesis of a zigzag carbon nanobelt. Nat. Chem. 2021, 13, 255–259.

Iijima, S. Helical microtubules of graphitic carbon. Nature 1991, 354, 56–58.

Iijima, S.; Ichihashi, T. Single-shell carbon nanotubes of 1-nm diameter. Nature 1993, 363, 603–605.

Journet, C.; Maser, W. K.; Bernier, P.; Loiseau, A.; De La Chapelle, M. L.; Lefrant, S.; Deniard, P.; Lee, R.; Fischer, J. E. Large-scale production of single-walled carbon nanotubes by the electric-arc technique. Nature 1997, 388, 756–758.

Gwyther, R. E. A.; Nekrasov, N. P.; Emelianov, A. V.; Nasibulin, A. G.; Ramakrishnan, K.; Bobrinetskiy, I.; Jones, D. D. Differential bio-optoelectronic gating of semiconducting carbon nanotubes by varying the covalent attachment residue of a green fluorescent protein. Adv. Funct. Mater. 2022, 32, 2112374.

Liao, Y. P.; Jiang, H.; Wei, N.; Laiho, P.; Zhang, Q.; Khan, S. A.; Kauppinen, E. I. Direct synthesis of colorful single-walled carbon nanotube thin films. J. Am. Chem. Soc. 2018, 140, 9797–9800.

Guo, Y. F.; Shi, E. Z.; Zhu, J. D.; Shen, P. C.; Wang, J. T.; Lin, Y. X.; Mao, Y. W.; Deng, S. B.; Li, B. N.; Park, J. H. et al. Soft-lock drawing of super-aligned carbon nanotube bundles for nanometre electrical contacts. Nat. Nanotechnol. 2022, 17, 278–284.

Qian, L.; Xie, Y.; Yu, Y.; Wang, S. S.; Zhang, S. C.; Zhang, J. Growth of single-walled carbon nanotubes with controlled structure: Floating carbide solid catalysts. Angew. Chem., Int. Ed. 2020, 59, 10884–10887.

Zhang, S. C.; Kang, L. X.; Wang, X.; Tong, L. M.; Yang, L. W.; Wang, Z. Q.; Qi, K.; Deng, S. B.; Li, Q. W.; Bai, X. D. et al. Arrays of horizontal carbon nanotubes of controlled chirality grown using designed catalysts. Nature 2017, 543, 234–238.

Jin, Q.; Jiang, S.; Zhao, Y.; Wang, D.; Qiu, J. H.; Tang, D. M.; Tan, J.; Sun, D. M.; Hou, P. X.; Chen, X. Q. et al. Flexible layer-structured Bi₂Te₃ thermoelectric on a carbon nanotube scaffold. Nat. Mater. 2019, 18, 62–68.

Sett, D.; Basak, D. Highly enhanced H₂ gas sensing characteristics of Co: ZnO nanorods and its mechanism. Sensor. Actuat. B Chem. 2017, 243, 475–483.

Tian, H. L.; Fan, H. Q.; Li, M. M.; Ma, L. T. Zeolitic imidazolate framework coated ZnO nanorods as molecular sieving to improve selectivity of formaldehyde gas sensor. ACS Sens. 2016, 1, 243–250.

Yaghmour, S. J.; Mahmoud, W. E. Synthesis and characterization of self-assembly silver sulfide nanorods prepared by squalene assisted microwave technique. Mater. Lett. 2013, 109, 55–57.

Lee, J.; Kim, Y.; Kim, J. K.; Kim, S.; Min, D. H.; Jang, D. J. Highly efficient photocatalytic performances of SnO₂-deposited ZnS nanorods based on interfacial charge transfer. Appl. Catal. B Environ. 2017, 205, 433–442.

Zhang, H. Ultrathin two-dimensional nanomaterials. ACS Nano 2015, 9, 9451–9469.

Geim, A. K.; Novoselov, K. S. The rise of graphene. Nat. Mater. 2007, 6, 183–191.

Geim, A. K. Graphene: Status and prospects. Science 2009, 324, 1530–1534.

Raccichini, R.; Varzi, A.; Passerini, S.; Scrosati, B. The role of graphene for electrochemical energy storage. Nat. Mater. 2015, 14, 271–279.

Dou, Y. H.; Zhang, L.; Xu, X.; Sun, Z. Q.; Liao, T.; Dou, S. X. Atomically thin non-layered nanomaterials for energy storage and conversion. Chem. Soc. Rev. 2017, 46, 7338–7373.

Shahzad, F.; Alhabeb, M.; Hatter, C. B.; Anasori, B.; Hong, S. M.; Koo, C. M.; Gogotsi, Y. Electromagnetic interference shielding with 2D transition metal carbides (MXenes). Science 2016, 353, 1137–1140.

Neto, A. H. C.; Guinea, F.; Peres, N. M. R.; Novoselov, K. S.; Geim, A. K. The electronic properties of graphene. Rev. Mod. Phys. 2009, 81, 109–162.

Jariwala, D.; Sangwan, V. K.; Lauhon, L. J.; Marks, T. J.; Hersam, M. C. Carbon nanomaterials for electronics, optoelectronics, photovoltaics, and sensing. Chem. Soc. Rev. 2013, 42, 2824–2860.

Sun, Y. Q.; Wu, Q.; Shi, G. Q. Graphene based new energy materials. Energy Environ. Sci. 2011, 4, 1113–1132.

Liu, Y. X.; Dong, X. C.; Chen, P. Biological and chemical sensors based on graphene materials. Chem. Soc. Rev. 2012, 41, 2283–2307.

Novoselov, K. S.; Geim, A. K.; Morozov, S. V.; Jiang, D.; Zhang, Y.; Dubonos, S. V.; Grigorieva, I. V.; Firsov, A. A. Electric field effect in atomically thin carbon films. Science 2004, 306, 666–669.

Zhou, S. Y.; Gweon, G. H.; Fedorov, A. V.; First, P. N.; De Heer, W. A.; Lee, D. H.; Guinea, F.; Neto, A. H. C.; Lanzara, A. Substrate-induced bandgap opening in epitaxial graphene. Nat. Mater. 2007, 6, 770–775.

Huang, Y.; Sutter, E.; Shi, N. N.; Zheng, J. B.; Yang, T. Z.; Englund, D.; Gao, H. J.; Sutter, P. Reliable exfoliation of large-area high-quality flakes of graphene and other two-dimensional materials. ACS Nano 2015, 9, 10612–10620.

Naguib, M.; Mashtalir, O.; Carle, J.; Presser, V.; Lu, J.; Hultman, L.; Gogotsi, Y.; Barsoum, M. W. Two-dimensional transition metal carbides. ACS Nano 2012, 6, 1322–1331.

Liu, K. K.; Zhang, W. J.; Lee, Y. H.; Lin, Y. C.; Chang, M. T.; Su, C. Y.; Chang, C. S.; Li, H.; Shi, Y. M.; Zhang, H. et al. Growth of large-area and highly crystalline MoS₂ thin layers on insulating substrates. Nano Lett. 2012, 12, 1538–1544.

Song, F.; Hu, X. L. Exfoliation of layered double hydroxides for enhanced oxygen evolution catalysis. Nat. Commun. 2014, 5, 4477.

Georgakilas, V.; Otyepka, M.; Bourlinos, A. B.; Chandra, V.; Kim, N.; Kemp, K. C.; Hobza, P.; Zboril, R.; Kim, K. S. Functionalization of graphene: Covalent and non-covalent approaches, derivatives and applications. Chem. Rev. 2012, 112, 6156–6214.

Kong, X. K.; Chen, C. L.; Chen, Q. W. Doped graphene for metal-free catalysis. Chem. Soc. Rev. 2014, 43, 2841–2857.

Choi, C. H.; Chung, M. W.; Kwon, H. C.; Park, S. H.; Woo, S. I. B, N- and P, N-doped graphene as highly active catalysts for oxygen reduction reactions in acidic media. J. Mater. Chem. A 2013, 1, 3694–3699.

Ding, H. M.; Li, Y. B.; Li, M.; Chen, K.; Liang, K.; Chen, G. X.; Lu, J.; Palisaitis, J.; Persson, P. O. Å.; Eklund, P. et al. Chemical scissor-mediated structural editing of layered transition metal carbides. Science 2023, 379, 1130–1135.

Zhang, X.; Lai, Z. C.; Tan, C. L.; Zhang, H. Solution-processed two-dimensional MoS₂ nanosheets: Preparation, hybridization, and applications. Angew. Chem., Int. Ed. 2016, 55, 8816–8838.

Fu, Q.; Han, J. C.; Wang, X. J.; Xu, P.; Yao, T.; Zhong, J.; Zhong, W. W.; Liu, S. W.; Gao, T. L.; Zhang, Z. H. et al. 2D transition metal dichalcogenides: Design, modulation, and challenges in electrocatalysis. Adv. Mater. 2021, 33, 1907818.

Xie, J. F.; Zhang, H.; Li, S.; Wang, R. X.; Sun, X.; Zhou, M.; Zhou, J. F.; Lou, X. W. D.; Xie, Y. Defect-rich MoS₂ ultrathin nanosheets with additional active edge sites for enhanced electrocatalytic hydrogen evolution. Adv. Mater. 2013, 25, 5807–5813.

Kibsgaard, J.; Chen, Z. B.; Reinecke, B. N.; Jaramillo, T. F. Engineering the surface structure of MoS₂ to preferentially expose active edge sites for electrocatalysis. Nat. Mater. 2012, 11, 963–969.

Gao, M. R.; Chan, M. K. Y.; Sun, Y. G. Edge-terminated molybdenum disulfide with a 9.4-Å interlayer spacing for electrochemical hydrogen production. Nat. Commun. 2015, 6, 7493.

Rao, T. K.; Wang, H. D.; Zeng, Y. J.; Guo, Z. N.; Zhang, H.; Liao, W. G. Phase transitions and water splitting applications of 2D transition metal dichalcogenides and metal phosphorous trichalcogenides. Adv. Sci. (Weinh. ) 2021, 8, 2002284.

Faraji, M.; Yousefi, M.; Yousefzadeh, S.; Zirak, M.; Naseri, N.; Jeon, T. H.; Choi, W.; Moshfegh, A. Z. Two-dimensional materials in semiconductor photoelectrocatalytic systems for water splitting. Energy Environ. Sci. 2019, 12, 59–95.

Qiu, B. C.; Zhu, Q. H.; Du, M. M.; Fan, L. G.; Xing, M. Y.; Zhang, J. L. Efficient solar light harvesting CdS/Co₉S₈ hollow cubes for Z-scheme photocatalytic water splitting. Angew. Chem., Int. Ed. 2017, 56, 2684–2688.

Haque, F.; Daeneke, T.; Kalantar-Zadeh, K.; Ou, J. Z. Two-dimensional transition metal oxide and chalcogenide-based photocatalysts. Nano-Micro Lett. 2018, 10, 23.

Chang, K.; Mei, Z. W.; Wang, T.; Kang, Q.; Ouyang, S. X.; Ye, J. H. MoS₂/graphene cocatalyst for efficient photocatalytic H₂ evolution under visible light irradiation. ACS Nano 2014, 8, 7078–7087.

Pumera, M.; Sofer, Z.; Ambrosi, A. Layered transition metal dichalcogenides for electrochemical energy generation and storage. J. Mater. Chem. A 2014, 2, 8981–8987.

Chhowalla, M.; Shin, H. S.; Eda, G.; Li, L. J.; Loh, K. P.; Zhang, H. The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. Nat. Chem. 2013, 5, 263–275.

Yun, Q. B.; Li, L. X.; Hu, Z. N.; Lu, Q. P.; Chen, B.; Zhang, H. Layered transition metal dichalcogenide-based nanomaterials for electrochemical energy storage. Adv. Mater. 2020, 32, 1903826.

Sun, Z. Q.; Liao, T.; Dou, Y. H.; Hwang, S. M.; Park, M. S.; Jiang, L.; Kim, J. H.; Dou, S. X. Generalized self-assembly of scalable two-dimensional transition metal oxide nanosheets. Nat. Commun. 2014, 5, 3813.

Wang, X.; Chen, W. X.; Zhang, L.; Yao, T.; Liu, W.; Lin, Y.; Ju, H. X.; Dong, J. C.; Zheng, L. R.; Yan, W. S. et al. Uncoordinated amine groups of metal-organic frameworks to anchor single Ru sites as chemoselective catalysts toward the hydrogenation of quinoline. J. Am. Chem. Soc. 2017, 139, 9419–9422.

Chen, Y. J.; Ji, S. F.; Wang, Y. G.; Dong, J. C.; Chen, W. X.; Li, Z.; Shen, R. A.; Zheng, L. R.; Zhuang, Z. B.; Wang, D. S. et al. Isolated single iron atoms anchored on N-doped porous carbon as an efficient electrocatalyst for the oxygen reduction reaction. Angew. Chem., Int. Ed. 2017, 56, 6937–6941.

Liu, Y. W.; Li, Z.; Yu, Q. Y.; Chen, Y. F.; Chai, Z. W.; Zhao, G. F.; Liu, S. J.; Cheong, W. C.; Pan, Y.; Zhang, Q. H. et al. A general strategy for fabricating isolated single metal atomic site catalysts in Y zeolite. J. Am. Chem. Soc. 2019, 141, 9305–9311.

Zhao, C. S.; Zhang, H. T.; Si, W. J.; Wu, H. Mass production of two-dimensional oxides by rapid heating of hydrous chlorides. Nat. Commun. 2016, 7, 12543.

Corma, A.; Concepción, P.; Boronat, M.; Sabater, M. J.; Navas, J.; Yacaman, M. J.; Larios, E.; Posadas, A.; López-Quintela, M. A.; Buceta, D. et al. Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity. Nat. Chem. 2013, 5, 775–781.

Ortalan, V.; Uzun, A.; Gates, B. C.; Browning, N. D. Direct imaging of single metal atoms and clusters in the pores of dealuminated HY zeolite. Nat. Nanotechnol. 2010, 5, 506–510.

Kistler, J. D.; Chotigkrai, N.; Xu, P. H.; Enderle, B.; Praserthdam, P.; Chen, C. Y.; Browning, N. D.; Gates, B. C. A single-site platinum CO oxidation catalyst in zeolite KLTL: Microscopic and spectroscopic determination of the locations of the platinum atoms. Angew. Chem., Int. Ed. 2014, 53, 8904–8907.

Luo, E. G.; Zhang, H.; Wang, X.; Gao, L. Q.; Gong, L. Y.; Zhao, T.; Jin, Z.; Ge, J. J.; Jiang, Z.; Liu, C. P. et al. Single-atom Cr-N₄ sites designed for durable oxygen reduction catalysis in acid media. Angew. Chem., Int. Ed. 2019, 58, 12469–12475.

Li, J. Z.; Chen, M. J.; Cullen, D. A.; Hwang, S.; Wang, M. Y.; Li, B. Y.; Liu, K. X.; Karakalos, S.; Lucero, M.; Zhang, H. G. et al. Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells. Nat. Catal. 2018, 1, 935–945.

Zhong, W. F.; Sa, R.; Li, L. Y.; He, Y. J.; Li, L. Y.; Bi, J. H.; Zhuang, Z. Y.; Yu, Y.; Zou, Z. G. A covalent organic framework bearing single Ni sites as a synergistic photocatalyst for selective photoreduction of CO₂ to CO. J. Am. Chem. Soc. 2019, 141, 7615–7621.

Chen, Y. J.; Ji, S. F.; Sun, W. M.; Chen, W. X.; Dong, J. C.; Wen, J. F.; Zhang, J.; Li, Z.; Zheng, L. R.; Chen, C. et al. Discovering partially charged single-atom Pt for enhanced anti-markovnikov alkene hydrosilylation. J. Am. Chem. Soc. 2018, 140, 7407–7410.

Zhang, E. H.; Tao, L.; An, J. K.; Zhang, J. W.; Meng, L. Z.; Zheng, X. B.; Wang, Y.; Li, N.; Du, S. X.; Zhang, J. T. et al. Engineering the local atomic environments of indium single-atom catalysts for efficient electrochemical production of hydrogen peroxide. Angew. Chem., Int. Ed. 2022, 61, e202117347.

Dvořák, F.; Camellone, M. F.; Tovt, A.; Tran, N. D.; Negreiros, F. R.; Vorokhta, M.; Skála, T.; Matolínová, I.; Mysliveček, J.; Matolín, V. et al. Creating single-atom Pt-ceria catalysts by surface step decoration. Nat. Commun. 2016, 7, 10801.

Xie, P. F.; Pu, T. C.; Nie, A. M.; Hwang, S.; Purdy, S. C.; Yu, W. J.; Su, D.; Miller, J. T.; Wang, C. Nanoceria-supported single-atom platinum catalysts for direct methane conversion. ACS Catal. 2018, 8, 4044–4048.

Li, H. L.; Wang, L. B.; Dai, Y. Z.; Pu, Z. T.; Lao, Z. H.; Chen, Y. W.; Wang, M. L.; Zheng, X. S.; Zhu, J. F.; Zhang, W. H. et al. Synergetic interaction between neighbouring platinum monomers in CO₂ hydrogenation. Nat. Nanotechnol. 2018, 13, 411–417.

Lee, B. H.; Park, S.; Kim, M.; Sinha, A. K.; Lee, S. C.; Jung, E.; Chang, W. J.; Lee, K. S.; Kim, J. H.; Cho, S. P. et al. Reversible and cooperative photoactivation of single-atom Cu/TiO₂ photocatalysts. Nat. Mater. 2019, 18, 620–626.

Zhang, L. Z.; Jia, Y.; Gao, G. P.; Yan, X. C.; Chen, N.; Chen, J.; Soo, M. T.; Wood, B.; Yang, D. J.; Du, A. J. et al. Graphene defects trap atomic Ni species for hydrogen and oxygen evolution reactions. Chem 2018, 4, 285–297.

Huang, F.; Deng, Y. C.; Chen, Y. L.; Cai, X. B.; Peng, M.; Jia, Z. M.; Xie, J. L.; Xiao, D. Q.; Wen, X. D.; Wang, N. et al. Anchoring Cu₁ species over nanodiamond-graphene for semi-hydrogenation of acetylene. Nat. Commun. 2019, 10, 4431.

Zhang, J.; Wu, X.; Cheong, W. C.; Chen, W. X.; Lin, R.; Li, J.; Zheng, L. R.; Yan, W. S.; Gu, L.; Chen, C. et al. Cation vacancy stabilization of single-atomic-site Pt₁/Ni(OH)_x catalyst for diboration of alkynes and alkenes. Nat. Commun. 2018, 9, 1002.

Huang, F.; Deng, Y. C.; Chen, Y. L.; Cai, X. B.; Peng, M.; Jia, Z. M.; Ren, P. J.; Xiao, D. Q.; Wen, X. D.; Wang, N. et al. Atomically dispersed Pd on nanodiamond/graphene hybrid for selective hydrogenation of acetylene. J. Am. Chem. Soc. 2018, 140, 13142–13146.

Zhang, H. B.; Yu, L.; Chen, T.; Zhou, W.; Lou, X. W. D. Surface modulation of hierarchical MoS₂ nanosheets by Ni single atoms for enhanced electrocatalytic hydrogen evolution. Adv. Funct. Mater. 2018, 28, 1807086.

Jiang, K.; Liu, B. Y.; Luo, M.; Ning, S. C.; Peng, M.; Zhao, Y.; Lu, Y. R.; Chan, T. S.; De Groot, F. M. F.; Tan, Y. W. Single platinum atoms embedded in nanoporous cobalt selenide as electrocatalyst for accelerating hydrogen evolution reaction. Nat. Commun. 2019, 10, 1743.

He, X. H.; He, Q.; Deng, Y. C.; Peng, M.; Chen, H. Y.; Zhang, Y.; Yao, S. Y.; Zhang, M. T.; Xiao, D. Q.; Ma, D. et al. A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation. Nat. Commun. 2019, 10, 3663.

Gao, C.; Chen, S. M.; Wang, Y.; Wang, J. W.; Zheng, X. S.; Zhu, J. F.; Song, L.; Zhang, W. K.; Xiong, Y. J. Heterogeneous single-atom catalyst for visible-light-driven high-turnover CO₂ reduction: The role of electron transfer. Adv. Mater. 2018, 30, 1704624.

Shao, X. Z.; Yang, X. F.; Xu, J. M.; Liu, S.; Miao, S.; Liu, X. Y.; Su, X.; Duan, H. M.; Huang, Y. Q.; Zhang, T. Iridium single-atom catalyst performing a quasi-homogeneous hydrogenation transformation of CO₂ to formate. Chem 2019, 5, 693–705.

He, T.; Chen, S. M.; Ni, B.; Gong, Y.; Wu, Z.; Song, L.; Gu, L.; Hu, W. P.; Wang, X. Zirconium-porphyrin-based metal-organic framework hollow nanotubes for immobilization of noble-metal single atoms. Angew. Chem., Int. Ed. 2018, 57, 3493–3498.

Yin, P. Q.; Yao, T.; Wu, Y. E.; Zheng, L. R.; Lin, Y.; Liu, W.; Ju, H. X.; Zhu, J. F.; Hong, X.; Deng, Z. X. et al. Single cobalt atoms with precise N-coordination as superior oxygen reduction reaction catalysts. Angew. Chem., Int. Ed. 2016, 55, 10800–10805.

Fei, H. L.; Dong, J. C.; Feng, Y. X.; Allen, C. S.; Wan, C. Z.; Volosskiy, B.; Li, M. F.; Zhao, Z. P.; Wang, Y. L.; Sun, H. T. et al. General synthesis and definitive structural identification of MN₄C₄ single-atom catalysts with tunable electrocatalytic activities. Nat. Catal. 2018, 1, 63–72.

Sa, Y. J.; Seo, D. J.; Woo, J.; Lim, J. T.; Cheon, J. Y.; Yang, S. Y.; Lee, J. M.; Kang, D.; Shin, T. J.; Shin, H. S. et al. A general approach to preferential formation of active Fe-N_x sites in Fe-N/C electrocatalysts for efficient oxygen reduction reaction. J. Am. Chem. Soc. 2016, 138, 15046–15056.

Vilé, G.; Albani, D.; Nachtegaal, M.; Chen, Z. P.; Dontsova, D.; Antonietti, M.; López, N.; Pérez-Ramírez, J. A stable single-site palladium catalyst for hydrogenations. Angew. Chem., Int. Ed. 2015, 54, 11265–11269.

Li, X. G.; Bi, W. T.; Chen, M. L.; Sun, Y. X.; Ju, H. X.; Yan, W. S.; Zhu, J. F.; Wu, X. J.; Chu, W. S.; Wu, C. Z. et al. Exclusive NiN₄ sites realize near-unity CO selectivity for electrochemical CO₂ reduction. J. Am. Chem. Soc. 2017, 139, 14889–14892.

Chen, S. H.; Li, W. H.; Jiang, W. J.; Yang, J. R.; Zhu, J. X.; Wang, L. Q.; Ou, H. H.; Zhuang, Z. C.; Chen, M. Z.; Sun, X. H. et al. MOF encapsulating N-heterocyclic carbene-ligated copper single-atom site catalyst towards efficient methane electrosynthesis. Angew. Chem., Int. Ed. 2022, 61, e202114450.

Ye, L.; Duan, X. P.; Wu, S.; Wu, T. S.; Zhao, Y. X.; Robertson, A. W.; Chou, H. L.; Zheng, J. W.; Ayvalı, T.; Day, S. et al. Self-regeneration of Au/CeO₂ based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination. Nat. Commun. 2019, 10, 914.

Zhang, X. Y.; Sun, Z. C.; Wang, B.; Tang, Y.; Nguyen, L.; Li, Y. T.; Tao, F. F. C–C coupling on single-atom-based heterogeneous catalyst. J. Am. Chem. Soc. 2018, 140, 954–962.

Xin, P. Y.; Li, J.; Xiong, Y.; Wu, X.; Dong, J. C.; Chen, W. X.; Wang, Y.; Gu, L.; Luo, J.; Rong, H. P. et al. Revealing the active species for aerobic alcohol oxidation by using uniform supported palladium catalysts. Angew. Chem., Int. Ed. 2018, 57, 4642–4646.

Matsubu, J. C.; Yang, V. N.; Christopher, P. Isolated metal active site concentration and stability control catalytic CO₂ reduction selectivity. J. Am. Chem. Soc. 2015, 137, 3076–3084.

Millet, M. M.; Algara-Siller, G.; Wrabetz, S.; Mazheika, A.; Girgsdies, F.; Teschner, D.; Seitz, F.; Tarasov, A.; Levchenko, S. V.; Schlögl, R. et al. Ni single atom catalysts for CO₂ activation. J. Am. Chem. Soc. 2019, 141, 2451–2461.

Lin, L. L.; Zhou, W.; Gao, R.; Yao, S. Y.; Zhang, X.; Xu, W. Q.; Zheng, S. J.; Jiang, Z.; Yu, Q. L.; Li, Y. W. et al. Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts. Nature 2017, 544, 80–83.

Lin, L. L.; Yao, S. Y.; Gao, R.; Liang, X.; Yu, Q. L.; Deng, Y. C.; Liu, J. J.; Peng, M.; Jiang, Z.; Li, S. W. et al. A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation. Nat. Nanotechnol. 2019, 14, 354–361.

Li, S. W.; Liu, J. J.; Yin, Z.; Ren, P. J.; Lin, L. L.; Gong, Y.; Yang, C.; Zheng, X. S.; Cao, R. C.; Yao, S. Y. et al. Impact of the coordination environment on atomically dispersed Pt catalysts for oxygen reduction reaction. ACS Catal. 2020, 10, 907–913.

DeRita, L.; Dai, S.; Lopez-Zepeda, K.; Pham, N.; Graham, G. W.; Pan, X. Q.; Christopher, P. Catalyst architecture for stable single atom dispersion enables site-specific spectroscopic and reactivity measurements of CO adsorbed to Pt atoms, oxidized Pt clusters, and metallic Pt clusters on TiO₂. J. Am. Chem. Soc. 2017, 139, 14150–14165.

Jiao, L.; Regalbuto, J. R. The synthesis of highly dispersed noble and base metals on silica via strong electrostatic adsorption: I. Amorphous silica. J. Catal. 2008, 260, 329–341.

Yan, H.; Cheng, H.; Yi, H.; Lin, Y.; Yao, T.; Wang, C. L.; Li, J. J.; Wei, S. Q.; Lu, J. L. Single-atom Pd₁/graphene catalyst achieved by atomic layer deposition: Remarkable performance in selective hydrogenation of 1,3-butadiene. J. Am. Chem. Soc. 2015, 137, 10484–10487.

Cao, Y. J.; Chen, S.; Luo, Q. Q.; Yan, H.; Lin, Y.; Liu, W.; Cao, L. L.; Lu, J. L.; Yang, J. L.; Yao, T. et al. Atomic-level insight into optimizing the hydrogen evolution pathway over a Co₁-N₄ single-site photocatalyst. Angew. Chem., Int. Ed. 2017, 56, 12191–12196.

Zhang, L.; Banis, M. N.; Sun, X. L. Single-atom catalysts by the atomic layer deposition technique. Natl. Sci. Rev. 2018, 5, 628–630.

Cheng, N. C.; Stambula, S.; Wang, D.; Banis, M. N.; Liu, J.; Riese, A.; Xiao, B. W.; Li, R. Y.; Sham, T. K.; Liu, L. M. et al. Platinum single-atom and cluster catalysis of the hydrogen evolution reaction. Nat. Commun. 2016, 7, 13638.

Han, G. F.; Li, F.; Rykov, A. I.; Im, Y. K.; Yu, S. Y.; Jeon, J. P.; Kim, S. J.; Zhou, W. H.; Ge, R. L.; Ao, Z. M. et al. Abrading bulk metal into single atoms. Nat. Nanotechnol. 2022, 17, 403–407.

Qu, Y. T.; Li, Z. J.; Chen, W. X.; Lin, Y.; Yuan, T. W.; Yang, Z. K.; Zhao, C. M.; Wang, J.; Zhao, C.; Wang, X. et al. Direct transformation of bulk copper into copper single sites via emitting and trapping of atoms. Nat. Catal. 2018, 1, 781–786.

Yang, Z. K.; Chen, B. X.; Chen, W. X.; Qu, Y. T.; Zhou, F. Y.; Zhao, C. M.; Xu, Q.; Zhang, Q. H.; Duan, X. Z.; Wu, Y. E. Directly transforming copper (I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach. Nat. Commun. 2019, 10, 3734.

Sun, T. T.; Zhao, S.; Chen, W. X.; Zhai, D.; Dong, J. C.; Wang, Y.; Zhang, S. L.; Han, A. J.; Gu, L.; Yu, R. et al. Single-atomic cobalt sites embedded in hierarchically ordered porous nitrogen-doped carbon as a superior bifunctional electrocatalyst. Proc. Natl. Acad. Sci. USA 2018, 115, 12692–12697.

Han, Y. H.; Wang, Y. G.; Chen, W. X.; Xu, R. R.; Zheng, L. R.; Zhang, J.; Luo, J.; Shen, R. A.; Zhu, Y. Q.; Cheong, W. C. et al. Hollow N-doped carbon spheres with isolated cobalt single atomic sites: Superior electrocatalysts for oxygen reduction. J. Am. Chem. Soc. 2017, 139, 17269–17272.

Zhang, L. Z.; Jia, Y.; Liu, H. L.; Zhuang, L. Z.; Yan, X. C.; Lang, C. G.; Wang, X.; Yang, D. J.; Huang, K. K.; Feng, S. H. et al. Charge polarization from atomic metals on adjacent graphitic layers for enhancing the hydrogen evolution reaction. Angew. Chem., Int. Ed. 2019, 58, 9404–9408.

Fan, L. L.; Liu, P. F.; Yan, X. C.; Gu, L.; Yang, Z. Z.; Yang, H. G.; Qiu, S. L.; Yao, X. D. Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis. Nat. Commun. 2016, 7, 10667.

Ge, X. X.; Zhou, P.; Zhang, Q. H.; Xia, Z. H.; Chen, S. L.; Gao, P.; Zhang, Z.; Gu, L.; Guo, S. J. Palladium single atoms on TiO₂ as a photocatalytic sensing platform for analyzing the organophosphorus pesticide chlorpyrifos. Angew. Chem., Int. Ed. 2020, 59, 232–236.

Liu, P. X.; Zhao, Y.; Qin, R. X.; Mo, S. G.; Chen, G. X.; Gu, L.; Chevrier, D. M.; Zhang, P.; Guo, Q.; Zang, D. D. et al. Photochemical route for synthesizing atomically dispersed palladium catalysts. Science 2016, 352, 797–800.

Wei, H. H.; Huang, K.; Wang, D.; Zhang, R. Y.; Ge, B. H.; Ma, J. Y.; Wen, B.; Zhang, S.; Li, Q. Y.; Lei, M. et al. Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth. Nat. Commun. 2017, 8, 1490.

Li, Y. G.; Hao, J. C.; Song, H.; Zhang, F. Y.; Bai, X. H.; Meng, X. G.; Zhang, H. Y.; Wang, S. F.; Hu, Y.; Ye, J. H. Selective light absorber-assisted single nickel atom catalysts for ambient sunlight-driven CO₂ methanation. Nat. Commun. 2019, 10, 2359.

Yao, Y. G.; Huang, Z. N.; Xie, P. F.; Wu, L. P.; Ma, L.; Li, T. Y.; Pang, Z. Q.; Jiao, M. L.; Liang, Z.; Gao, J. L. et al. High temperature shockwave stabilized single atoms. Nat. Nanotechnol. 2019, 14, 851–857.

Deng, D. H.; Chen, X. Q.; Yu, L.; Wu, X.; Liu, Q. F.; Liu, Y.; Yang, H. X.; Tian, H. F.; Hu, Y. F.; Du, P. P. et al. A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature. Sci. Adv. 2015, 1, e1500462.

Cui, X. J.; Xiao, J. P.; Wu, Y. H.; Du, P. P.; Si, R.; Yang, H. X.; Tian, H. F.; Li, J. Q.; Zhang, W. H.; Deng, D. H. et al. A graphene composite material with single cobalt active sites: A highly efficient counter electrode for dye-sensitized solar cells. Angew. Chem., Int. Ed. 2016, 55, 6708–6712.

Ding, S. P.; Guo, Y. L.; Hülsey, M. J.; Zhang, B.; Asakura, H.; Liu, L. M.; Han, Y.; Gao, M.; Hasegawa, J. Y.; Qiao, B. T. et al. Electrostatic stabilization of single-atom catalysts by ionic liquids. Chem 2019, 5, 3207–3219.

Chen, Y. J.; Ji, S. F.; Sun, W. M.; Lei, Y. P.; Wang, Q. C.; Li, A.; Chen, W. X.; Zhou, G.; Zhang, Z. D.; Wang, Y. et al. Engineering the atomic interface with single platinum atoms for enhanced photocatalytic hydrogen production. Angew. Chem., Int. Ed. 2020, 59, 1295–1301.

Yang, J. R.; Li, W. H.; Xu, K. N.; Tan, S. D.; Wang, D. S.; Li, Y. D. Regulating the tip effect on single-atom and cluster catalysts: Forming reversible oxygen species with high efficiency in chlorine evolution reaction. Angew. Chem., Int. Ed. 2022, 61, e202200366.

Zheng, X. B.; Yang, J. R.; Li, P.; Jiang, Z. L.; Zhu, P.; Wang, Q. S.; Wu, J. B.; Zhang, E. H.; Sun, W. P.; Dou, S. X. et al. Dual-atom support boosts nickel-catalyzed urea electrooxidation. Angew. Chem., Int. Ed. 2023, 62, e202217449.

Zhao, C. X.; Liu, J. N.; Wang, J.; Wang, C. D.; Guo, X.; Li, X. Y.; Chen, X.; Song, L.; Li, B. Q.; Zhang, Q. A clicking confinement strategy to fabricate transition metal single-atom sites for bifunctional oxygen electrocatalysis. Sci. Adv. 2022, 8, eabn5091.

Chen, Z. P.; Mitchell, S.; Vorobyeva, E.; Leary, R. K.; Hauert, R.; Furnival, T.; Ramasse, Q. M.; Thomas, J. M.; Midgley, P. A.; Dontsova, D. et al. Stabilization of single metal atoms on graphitic carbon nitride. Adv. Funct. Mater. 2017, 27, 1605785.

Chen, Y. J.; Ji, S. F.; Zhao, S.; Chen, W. X.; Dong, J. C.; Cheong, W. C.; Shen, R. A.; Wen, X. D.; Zheng, L. R.; Rykov, A. I. et al. Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell. Nat. Commun. 2018, 9, 5422.

Fang, X. Z.; Shang, Q. C.; Wang, Y.; Jiao, L.; Yao, T.; Li, Y. F.; Zhang, Q.; Luo, Y.; Jiang, H. L. Single Pt atoms confined into a metal-organic framework for efficient photocatalysis. Adv. Mater. 2018, 30, 1705112.

Liu, Q. T.; Liu, X. F.; Zheng, L. R.; Shui, J. L. The solid-phase synthesis of an Fe-N-C electrocatalyst for high-power proton-exchange membrane fuel cells. Angew. Chem., Int. Ed. 2018, 57, 1204–1208.

Peng, W.; Han, J. H.; Lu, Y. R.; Luo, M.; Chan, T. S.; Peng, M.; Tan, Y. W. A general strategy for engineering single-metal sites on 3D porous N, P Co-doped Ti₃C₂T_X MXene. ACS Nano 2022, 16, 4116–4125.

George, S. M. Atomic layer deposition: An overview. Chem. Rev. 2010, 110, 111–131.

Lu, J. L.; Elam, J. W.; Stair, P. C. Synthesis and stabilization of supported metal catalysts by atomic layer deposition. Acc. Chem. Res. 2013, 46, 1806–1815.

Puurunen, R. L. A short history of atomic layer deposition: Tuomo Suntola's atomic layer epitaxy. Chem. Vap. Deposit. 2014, 20, 332–344.

Fonseca, J.; Lu, J. L. Single-atom catalysts designed and prepared by the atomic layer deposition technique. ACS Catal. 2021, 11, 7018–7059.

Cheng, N. C.; Sun, X. L. Single atom catalyst by atomic layer deposition technique. Chin. J. Catal. 2017, 38, 1508–1514.

Xia, W.; Mahmood, A.; Liang, Z. B.; Zou, R. Q.; Guo, S. J. Earth-abundant nanomaterials for oxygen reduction. Angew. Chem., Int. Ed. 2016, 55, 2650–2676.

Zheng, X. B.; Li, B. B.; Wang, Q. S.; Wang, D. S.; Li, Y. D. Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis. Nano Res. 2022, 15, 7806–7839.

Du, L.; Prabhakaran, V.; Xie, X. H.; Park, S.; Wang, Y.; Shao, Y. Y. Low-PGM and PGM-free catalysts for proton exchange membrane fuel cells: Stability challenges and material solutions. Adv. Mater. 2021, 33, 1908232.

Wang, X. X.; Swihart, M. T.; Wu, G. Achievements, challenges and perspectives on cathode catalysts in proton exchange membrane fuel cells for transportation. Nat. Catal. 2019, 2, 578–589.

Wu, D. S.; Kusada, K.; Yamamoto, T.; Toriyama, T.; Matsumura, S.; Kawaguchi, S.; Kubota, Y.; Kitagawa, H. Platinum-group-metal high-entropy-alloy nanoparticles. J. Am. Chem. Soc. 2020, 142, 13833–13838.

Yao, Y. G.; Huang, Z. N.; Xie, P. F.; Lacey, S. D.; Jacob, R. J.; Xie, H.; Chen, F. J.; Nie, A. M.; Pu, T. C.; Rehwoldt, M. et al. Carbothermal shock synthesis of high-entropy-alloy nanoparticles. Science 2018, 359, 1489–1494.

Yao, Y. G.; Dong, Q.; Brozena, A.; Luo, J.; Miao, J. W.; Chi, M. F.; Wang, C.; Kevrekidis, I. G.; Ren, Z. J.; Greeley, J. et al. High-entropy nanoparticles: Synthesis-structure-property relationships and data-driven discovery. Science 2022, 376, eabn3103.

Li, T. Y.; Yao, Y. G.; Huang, Z. N.; Xie, P. F.; Liu, Z. Y.; Yang, M. H.; Gao, J. L.; Zeng, K. Z.; Brozena, A. H.; Pastel, G. et al. Denary oxide nanoparticles as highly stable catalysts for methane combustion. Nat. Catal. 2021, 4, 62–70.

Stranks, S. D.; Eperon, G. E.; Grancini, G.; Menelaou, C.; Alcocer, M. J. P.; Leijtens, T.; Herz, L. M.; Petrozza, A.; Snaith, H. J. Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber. Science 2013, 342, 341–344.

Chen, X. B.; Mao, S. S. Titanium dioxide nanomaterials: Synthesis, properties, modifications, and applications. Chem. Rev. 2007, 107, 2891–2959.

Poizot, P.; Laruelle, S.; Grugeon, S.; Dupont, L.; Tarascon, J. M. Nano-sized transition-metal oxides as negative-electrode materials for lithium-ion batteries. Nature 2000, 407, 496–499.

Kudo, A.; Miseki, Y. Heterogeneous photocatalyst materials for water splitting. Chem. Soc. Rev. 2009, 38, 253–278.

Zou, X. X.; Zhang, Y. Noble metal-free hydrogen evolution catalysts for water splitting. Chem. Soc. Rev. 2015, 44, 5148–5180.

Wang, L. G.; Duan, X. X.; Liu, X. J.; Gu, J.; Si, R.; Qiu, Y.; Qiu, Y. M.; Shi, D. E.; Chen, F. H.; Sun, X. M. et al. Atomically dispersed Mo supported on metallic Co₉S₈ nanoflakes as an advanced noble-metal-free bifunctional water splitting catalyst working in universal pH conditions. Adv. Energy Mater. 2020, 10, 1903137.

Choi, W.; Choudhary, N.; Han, G. H.; Park, J.; Akinwande, D.; Lee, Y. H. Recent development of two-dimensional transition metal dichalcogenides and their applications. Mater. Today 2017, 20, 116–130.

Hwang, J. Y.; Myung, S. T.; Sun, Y. K. Sodium-ion batteries: Present and future. Chem. Soc. Rev. 2017, 46, 3529–3614.

Wang, L. G.; Xia, L.; Wu, Y. J.; Tian, Y. Zr-doped β-In₂S₃ ultrathin nanoflakes as photoanodes: Enhanced visible-light-driven photoelectrochemical water splitting. ACS Sustainable Chem. Eng. 2016, 4, 2606–2614.

Martinez, U.; Babu, S. K.; Holby, E. F.; Chung, H. T.; Yin, X.; Zelenay, P. Progress in the development of Fe-based PGM-free electrocatalysts for the oxygen reduction reaction. Adv. Mater. 2019, 31, 1806545.

Thompson, S. T.; Papageorgopoulos, D. Platinum group metal-free catalysts boost cost competitiveness of fuel cell vehicles. Nat. Catal. 2019, 2, 558–561.

Ni, W. Y.; Wang, T.; Héroguel, F.; Krammer, A.; Lee, S.; Yao, L.; Schüler, A.; Luterbacher, J. S.; Yan, Y. S.; Hu, X. L. An efficient nickel hydrogen oxidation catalyst for hydroxide exchange membrane fuel cells. Nat. Mater. 2022, 21, 804–810.

Ye, K.; Cao, A.; Shao, J. Q.; Wang, G.; Si, R.; Ta, N.; Xiao, J. P.; Wang, G. X. Synergy effects on Sn-Cu alloy catalyst for efficient CO₂ electroreduction to formate with high mass activity. Sci. Bull. 2020, 65, 711–719.

He, J. Y.; Liu, W. H.; Wang, H.; Wu, Y.; Liu, X. J.; Nieh, T. G.; Lu, Z. P. Effects of Al addition on structural evolution and tensile properties of the FeCoNiCrMn high-entropy alloy system. Acta Mater. 2014, 62, 105–113.

Jiao, J. Q.; Lin, R.; Liu, S. J.; Cheong, W. C.; Zhang, C.; Chen, Z.; Pan, Y.; Tang, J. G.; Wu, K. L.; Hung, S. F. et al. Copper atom-pair catalyst anchored on alloy nanowires for selective and efficient electrochemical reduction of CO₂. Nat. Chem. 2019, 11, 222–228.

Chen, Y. J.; Pei, J. J.; Chen, Z.; Li, A.; Ji, S. F.; Rong, H. P.; Xu, Q.; Wang, T.; Zhang, A. J.; Tang, H. L. et al. Pt atomic layers with tensile strain and rich defects boost ethanol electrooxidation. Nano Lett. 2022, 22, 7563–7571.

Bu, L. Z.; Zhang, N.; Guo, S. J.; Zhang, X.; Li, J.; Yao, J. L.; Wu, T.; Lu, G.; Ma, J. Y.; Su, D. et al. Biaxially strained PtPb/Pt core/shell nanoplate boosts oxygen reduction catalysis. Science 2016, 354, 1410–1414.

Huang, X. Q.; Zhao, Z. P.; Cao, L.; Chen, Y.; Zhu, E. B.; Lin, Z. Y.; Li, M. F.; Yan, A. M.; Zettl, A.; Wang, Y. M. et al. High-performance transition metal-doped Pt₃Ni octahedra for oxygen reduction reaction. Science 2015, 348, 1230–1234.

Luo, M. C.; Zhao, Z. L.; Zhang, Y. L.; Sun, Y. J.; Xing, Y.; Lv, F.; Yang, Y.; Zhang, X.; Hwang, S.; Qin, Y. N. et al. PdMo bimetallene for oxygen reduction catalysis. Nature 2019, 574, 81–85.

Tian, X. L.; Zhao, X.; Su, Y. Q.; Wang, L. J.; Wang, H. M.; Dang, D.; Chi, B.; Liu, H. F.; Hensen, E. J. M.; Lou, X. W. et al. Engineering bunched Pt-Ni alloy nanocages for efficient oxygen reduction in practical fuel cells. Science 2019, 366, 850–856.

Jansonius, R. P.; Reid, L. M.; Virca, C. N.; Berlinguette, C. P. Strain engineering electrocatalysts for selective CO₂ Reduction. ACS Energy Lett. 2019, 4, 980–986.

Liu, D. Y.; Zeng, Q.; Liu, H.; Hu, C. Q.; Chen, D.; Xu, L.; Yang, J. Combining the core-shell construction with an alloying effect for high efficiency ethanol electrooxidation. Cell Rep. Phys. Sci. 2021, 2, 100357.

Zhou, Y.; Gu, Q. F.; Yin, K.; Li, Y. J.; Tao, L.; Tan, H.; Yang, Y.; Guo, S. J. Engineering e_g orbital occupancy of Pt with Au alloying enables reversible Li-O₂ batteries. Angew. Chem., Int. Ed. 2022, 61, e202201416.

Zheng, X. B.; Li, P.; Dou, S. X.; Sun, W. P.; Pan, H. G.; Wang, D. S.; Li, Y. D. Non-carbon-supported single-atom site catalysts for electrocatalysis. Energy Environ. Sci. 2021, 14, 2809–2858.

Tang, H. L.; Su, Y.; Zhang, B. S.; Lee, A. F.; Isaacs, M. A.; Wilson, K.; Li, L.; Ren, Y. G.; Huang, J. H.; Haruta, M. et al. Classical strong metal-support interactions between gold nanoparticles and titanium dioxide. Sci. Adv. 2017, 3, e1700231.

Dong, J. H.; Fu, Q.; Li, H. B.; Xiao, J. P.; Yang, B.; Zhang, B. S.; Bai, Y. X.; Song, T. Y.; Zhang, R. K.; Gao, L. J. et al. Reaction-induced strong metal-support interactions between metals and inert boron nitride nanosheets. J. Am. Chem. Soc. 2020, 142, 17167–17174.

Yu, J. S.; Kang, S.; Yoon, S. B.; Chai, G. Fabrication of ordered uniform porous carbon networks and their application to a catalyst supporter. J. Am. Chem. Soc. 2002, 124, 9382–9383.

Chai, G. S.; Shin, I. S.; Yu, J. S. Synthesis of ordered, uniform, macroporous carbons with mesoporous walls templated by aggregates of polystyrene spheres and silica particles for use as catalyst supports in direct methanol fuel cells. Adv. Mater. 2004, 16, 2057–2061.

Choi, W. C.; Woo, S. I.; Jeon, M. K.; Sohn, J. M.; Kim, M. R.; Jeon, H. J. Platinum nanoclusters studded in the microporous nanowalls of ordered mesoporous carbon. Adv. Mater. 2005, 17, 446–451.

Han, S.; Yun, Y.; Park, K. W.; Sung, Y. E.; Hyeon, T. Simple solid-phase synthesis of hollow graphitic nanoparticles and their application to direct methanol fuel cell electrodes. Adv. Mater. 2003, 15, 1922–1925.

Luo, Z. X.; Zhao, G. Q.; Pan, H. G.; Sun, W. P. Strong metal-support interaction in heterogeneous catalysts. Adv. Energy Mater. 2022, 12, 2201395.

Yao, S. Y.; Zhang, X.; Zhou, W.; Gao, R.; Xu, W. Q.; Ye, Y. F.; Lin, L. L.; Wen, X. D.; Liu, P.; Chen, B. B. et al. Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction. Science 2017, 357, 389–393.

Van Deelen, T. W.; Mejía, C. H.; De Jong, K. P. Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity. Nat. Catal. 2019, 2, 955–970.

Yang, J. R.; Li, W. H.; Wang, D. S.; Li, Y. D. Electronic metal-support interaction of single-atom catalysts and applications in electrocatalysis. Adv. Mater. 2020, 32, 2003300.

Li, W. H.; Yang, J. R.; Wang, D. S. Long-range interactions in diatomic catalysts boosting electrocatalysis. Angew. Chem., Int. Ed. 2022, 61, e202213318.

Wan, J. W.; Chen, W. X.; Jia, C. Y.; Zheng, L. R.; Dong, J. C.; Zheng, X. S.; Wang, Y.; Yan, W. S.; Chen, C.; Peng, Q. et al. Defect effects on TiO₂ nanosheets: Stabilizing single atomic site Au and promoting catalytic properties. Adv. Mater. 2018, 30, 1705369.

Zhang, J. Q.; Zhao, Y. F.; Guo, X.; Chen, C.; Dong, C. L.; Liu, R. S.; Han, C. P.; Li, Y. D.; Gogotsi, Y.; Wang, G. X. Single platinum atoms immobilized on an MXene as an efficient catalyst for the hydrogen evolution reaction. Nat. Catal. 2018, 1, 985–992.

Zheng, X. B.; Cui, P. X.; Qian, Y. M.; Zhao, G. Q.; Zheng, X. S.; Xu, X.; Cheng, Z. X.; Liu, Y. Y.; Dou, S. X.; Sun, W. P. Multifunctional active-center-transferable platinum/lithium cobalt oxide heterostructured electrocatalysts towards superior water splitting. Angew. Chem., Int. Ed. 2020, 59, 14533–14540.

Zhang, Z. D.; Zhou, M.; Chen, Y. J.; Liu, S. J.; Wang, H. F.; Zhang, J.; Ji, S. F.; Wang, D. S.; Li, Y. D. Pd single-atom monolithic catalyst: Functional 3D structure and unique chemical selectivity in hydrogenation reaction. Sci. China Mater. 2021, 64, 1919–1929.

Wang, L. G.; Liu, H.; Zhuang, J. H.; Wang, D. S. Small-scale big science: From nano- to atomically dispersed catalytic materials. Small Sci. 2022, 2, 2200036.

Yang, X. F.; Wang, A. Q.; Qiao, B. T.; Li, J.; Liu, J. Y.; Zhang, T. Single-atom catalysts: A new frontier in heterogeneous catalysis. Acc. Chem. Res. 2013, 46, 1740–1748.

Wang, H. W.; Gu, X. K.; Zheng, X. S.; Pan, H. B.; Zhu, J. F.; Chen, S.; Cao, L. N.; Li, W. X.; Lu, J. L. Disentangling the size-dependent geometric and electronic effects of palladium nanocatalysts beyond selectivity. Sci. Adv. 2019, 5, eaat6413.

Wei, S. J.; Li, A.; Liu, J. C.; Li, Z.; Chen, W. X.; Gong, Y.; Zhang, Q. H.; Cheong, W. C.; Wang, Y.; Zheng, L. R. et al. Direct observation of noble metal nanoparticles transforming to thermally stable single atoms. Nat. Nanotechnol. 2018, 13, 856–861.

Li, W.; Wang, D. D.; Zhang, Y. Q.; Tao, L.; Wang, T. H.; Zou, Y. Q.; Wang, Y. Y.; Chen, R.; Wang, S. Y. Defect engineering for fuel-cell electrocatalysts. Adv. Mater. 2020, 32, 1907879.

Zhang, Y. Q.; Tao, L.; Xie, C.; Wang, D. D.; Zou, Y. Q.; Chen, R.; Wang, Y. Y.; Jia, C. K.; Wang, S. Y. Defect engineering on electrode materials for rechargeable batteries. Adv. Mater. 2020, 32, 1905923.

Zhang, B.; Hou, J. G.; Wu, Y. Z.; Cao, S. Y.; Li, Z. W.; Nie, X. W.; Gao, Z. M.; Sun, L. C. Tailoring active sites in mesoporous defect-rich NC/V_o-WON heterostructure array for superior electrocatalytic hydrogen evolution. Adv. Energy Mater. 2019, 9, 1803693.

Zhang, B. W.; Qi, Z. Y.; Wu, Z. S.; Lui, Y. H.; Kim, T. H.; Tang, X. H.; Zhou, L.; Huang, W. Y.; Hu, S. Defect-rich 2D material networks for advanced oxygen evolution catalysts. ACS Energy Lett. 2019, 4, 328–336.

Zhu, J. W.; Huang, Y. P.; Mei, W. C.; Zhao, C. Y.; Zhang, C. T.; Zhang, J.; Amiinu, I. S.; Mu, S. C. Effects of intrinsic pentagon defects on electrochemical reactivity of carbon nanomaterials. Angew. Chem., Int. Ed. 2019, 58, 3859–3864.

Yang, H. G.; Sun, C. H.; Qiao, S. Z.; Zou, J.; Liu, G.; Smith, S. C.; Cheng, H. M.; Lu, G. Q. Anatase TiO₂ single crystals with a large percentage of reactive facets. Nature 2008, 453, 638–641.

Li, R. G.; Zhang, F. X.; Wang, D.; Yang, J. X.; Li, M. R.; Zhu, J.; Zhou, X.; Han, H. X.; Li, C. Spatial separation of photogenerated electrons and holes among {010} and {110} crystal facets of BiVO₄. Nat. Commun. 2013, 4, 1432.

Chen, R. T.; Pang, S.; An, H. Y.; Zhu, J.; Ye, S.; Gao, Y. Y.; Fan, F. T.; Li, C. Charge separation via asymmetric illumination in photocatalytic Cu₂O particles. Nat. Energy 2018, 3, 655–663.

Takata, T.; Jiang, J. Z.; Sakata, Y.; Nakabayashi, M.; Shibata, N.; Nandal, V.; Seki, K.; Hisatomi, T.; Domen, K. Photocatalytic water splitting with a quantum efficiency of almost unity. Nature 2020, 581, 411–414.

Li, M. F.; Zhao, Z. P.; Cheng, T.; Fortunelli, A.; Chen, C. Y.; Yu, R.; Zhang, Q. H.; Gu, L.; Merinov, B. V.; Lin, Z. Y. et al. Ultrafine jagged platinum nanowires enable ultrahigh mass activity for the oxygen reduction reaction. Science 2016, 354, 1414–1419.

Liu, J. W.; You, F. T.; He, B. W.; Wu, Y. L.; Wang, D. D.; Zhou, W. Q.; Qian, C.; Yang, G. B.; Liu, G. F.; Wang, H. et al. Directing the architecture of surface-clean Cu₂O for CO electroreduction. J. Am. Chem. Soc. 2022, 144, 12410–12420.

Zou, Z. H.; Wang, T. T.; Zhao, X. H.; Jiang, W. J.; Pan, H. R.; Gao, D. Q.; Xu, C. L. Expediting in-situ electrochemical activation of two-dimensional metal-organic frameworks for enhanced OER intrinsic activity by iron incorporation. ACS Catal. 2019, 9, 7356–7364.

Zhao, Y. F.; Kumar, P. V.; Tan, X.; Lu, X. X.; Zhu, X. F.; Jiang, J. J.; Pan, J.; Xi, S. B.; Yang, H. Y.; Ma, Z. P. et al. Modulating Pt-O-Pt atomic clusters with isolated cobalt atoms for enhanced hydrogen evolution catalysis. Nat. Commun. 2022, 13, 2430.

Pei, Z. H.; Lu, X. F.; Zhang, H. B.; Li, Y. X.; Luan, D. Y.; Lou, X. W. Highly efficient electrocatalytic oxygen evolution over atomically dispersed synergistic Ni/Co dual sites. Angew. Chem., Int. Ed. 2022, 61, e202207537.

Yan, Y.; Yin, Y. X.; Guo, Y. G.; Wan, L. J. A sandwich-like hierarchically porous carbon/graphene composite as a high-performance anode material for sodium-ion batteries. Adv. Energy Mater. 2014, 4, 1301584.

Wang, J.; Liu, J. L.; Chao, D. L.; Yan, J. X.; Lin, J. Y.; Shen, Z. X. Self-assembly of honeycomb-like MoS₂ nanoarchitectures anchored into graphene foam for enhanced lithium-ion storage. Adv. Mater. 2014, 26, 7162–7169.

Zhang, Z. B.; Wang, C. C.; Zakaria, R.; Ying, J. Y. Role of particle size in nanocrystalline TiO₂-based photocatalysts. J. Phys. Chem. B 1998, 102, 10871–10878.

Chen, C.; Kang, Y. J.; Huo, Z. Y.; Zhu, Z. W.; Huang, W. Y.; Xin, H. L.; Snyder, J. D.; Li, D. G.; Herron, J. A.; Mavrikakis, M. et al. Highly crystalline multimetallic nanoframes with three-dimensional electrocatalytic surfaces. Science 2014, 343, 1339–1343.

Vogt, C.; Weckhuysen, B. M. The concept of active site in heterogeneous catalysis. Nat. Rev. Chem. 2022, 6, 89–111.

Babucci, M.; Guntida, A.; Gates, B. C. Atomically dispersed metals on well-defined supports including zeolites and metal-organic frameworks: Structure, bonding, reactivity, and catalysis. Chem. Rev. 2020, 120, 11956–11985.

Montini, T.; Melchionna, M.; Monai, M.; Fornasiero, P. Fundamentals and catalytic applications of CeO₂-based materials. Chem. Rev. 2016, 116, 5987–6041.

Natinsky, B. S.; Liu, C. Two are better than one. Nat. Chem. 2019, 11, 200–201.

Zhu, P.; Xiong, X.; Wang, D. S. Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction. Nano Res. 2022, 15, 5792–5815.

Li, R. Z.; Wang, D. S. Understanding the structure-performance relationship of active sites at atomic scale. Nano Res. 2022, 15, 6888–6923.

Zhao, J. J.; Fu, C. H.; Ye, K.; Liang, Z.; Jiang, F. L.; Shen, S. Y.; Zhao, X. R.; Ma, L.; Shadike, Z.; Wang, X. M. et al. Manipulating the oxygen reduction reaction pathway on Pt-coordinated motifs. Nat. Commun. 2022, 13, 685.

Pan, Y.; Chen, Y. J.; Wu, K. L.; Chen, Z.; Liu, S. J.; Cao, X.; Cheong, W. C.; Meng, T.; Luo, J.; Zheng, L. R. et al. Regulating the coordination structure of single-atom Fe-N_xC_y catalytic sites for benzene oxidation. Nat. Commun. 2019, 10, 4290.

Yang, J. R.; Li, W. H.; Tan, S. D.; Xu, K. N.; Wang, Y.; Wang, D. S.; Li, Y. D. The electronic metal-support interaction directing the design of single atomic site catalysts: Achieving high efficiency towards hydrogen evolution. Angew. Chem., Int. Ed. 2021, 60, 19085–19091.

Li, W. H.; Yang, J. R.; Jing, H. Y.; Zhang, J.; Wang, Y.; Li, J.; Zhao, J.; Wang, D. S.; Li, Y. D. Creating high regioselectivity by electronic metal-support interaction of a single-atomic-site catalyst. J. Am. Chem. Soc. 2021, 143, 15453–15461.

Wu, J. B.; Su, J. W.; Wu, T.; Huang, L.; Li, Q.; Luo, Y. X.; Jin, H. R.; Zhou, J.; Zhai, T. Y.; Wang, D. S. et al. Scalable synthesis of 2D Mo₂C and thickness-dependent hydrogen evolution on its basal plane and edges. Adv. Mater. 2023, 35, 2209954.

Li, Q.; Wu, J. B.; Wu, T.; Jin, H. R.; Zhang, N.; Li, J.; Liang, W. X.; Liu, M. L.; Huang, L.; Zhou, J. Phase engineering of atomically thin perovskite oxide for highly active oxygen evolution. Adv. Funct. Mater. 2021, 31, 2102002.

Ye, C. L.; Peng, M.; Li, Y.; Wang, D. S.; Chen, C.; Li, Y. D. Atomically dispersed Pt in ordered PtSnZn intermetallic with Pt-Sn and Pt-Zn pairs for selective propane dehydrogenation. Sci. China Mater. 2023, 66, 1071–1078.

Yan, J. H.; Dong, K. Q.; Zhang, Y. Y.; Wang, X.; Aboalhassan, A. A.; Yu, J. Y.; Ding, B. Multifunctional flexible membranes from sponge-like porous carbon nanofibers with high conductivity. Nat. Commun. 2019, 10, 5584.

Zhuang, Z. C.; Li, Y.; Li, Y. H.; Huang, J. Z.; Wei, B.; Sun, R.; Ren, Y. J.; Ding, J.; Zhu, J. X.; Lang, Z. Q. et al. Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides. Energy Environ. Sci. 2021, 14, 1016–1028.

Wang, Y.; Wang, D. S.; Li, Y. D. Rational design of single-atom site electrocatalysts: From theoretical understandings to practical applications. Adv. Mater. 2021, 33, 2008151.

Chen, Y. J.; Gao, R.; Ji, S. F.; Li, H. J.; Tang, K.; Jiang, P.; Hu, H. B.; Zhang, Z. D.; Hao, H. G.; Qu, Q. Y. et al. Atomic-level modulation of electronic density at cobalt single-atom sites derived from metal-organic frameworks: Enhanced oxygen reduction performance. Angew. Chem., Int. Ed. 2021, 60, 3212–3221.

Han, Y. H.; Dai, J.; Xu, R. R.; Ai, W. Y.; Zheng, L. R.; Wang, Y.; Yan, W. S.; Chen, W. X.; Luo, J.; Liu, Q. et al. Notched-polyoxometalate strategy to fabricate atomically dispersed Ru catalysts for biomass conversion. ACS Catal. 2021, 11, 2669–2675.

Jia, Y. L.; Xue, Z. Q.; Yang, J.; Liu, Q. L.; Xian, J. H.; Zhong, Y. C.; Sun, Y. M.; Zhang, X. X.; Liu, Q. H.; Yao, D. X. et al. Tailoring the electronic structure of an atomically dispersed zinc electrocatalyst: Coordination environment regulation for high selectivity oxygen reduction. Angew. Chem., Int. Ed. 2022, 61, e202110838.

Tian, S. B.; Wang, B. X.; Gong, W. B.; He, Z. Z.; Xu, Q.; Chen, W. X.; Zhang, Q. H.; Zhu, Y. Q.; Yang, J. R.; Fu, Q. et al. Dual-atom Pt heterogeneous catalyst with excellent catalytic performances for the selective hydrogenation and epoxidation. Nat. Commun. 2021, 12, 3181.

Segler, M. H. S.; Preuss, M.; Waller, M. P. Planning chemical syntheses with deep neural networks and symbolic AI. Nature 2018, 555, 604–610.

Collins, K. D.; Glorius, F. A robustness screen for the rapid assessment of chemical reactions. Nat. Chem. 2013, 5, 597–601.

Robinson, R. LXIII.-A synthesis of tropinone. J. Chem. Soc. Trans. 1917, 111, 762–768.

Chong, L. N.; Gao, G. P.; Wen, J. G.; Li, H. X.; Xu, H. P.; Green, Z.; Sugar, J. D.; Kropf, A. J.; Xu, W. Q.; Lin, X. M. et al. La-and Mn-doped cobalt spinel oxygen evolution catalyst for proton exchange membrane electrolysis. Science 2023, 380, 609–616.

Smith, R. D. L.; Prévot, M. S.; Fagan, R. D.; Zhang, Z. P.; Sedach, P. A.; Siu, M. K. J.; Trudel, S.; Berlinguette, C. P. Photochemical route for accessing amorphous metal oxide materials for water oxidation catalysis. Science 2013, 340, 60–63.

Huang, J. Z.; Sheng, H. Y.; Ross, R. D.; Han, J. C.; Wang, X. J.; Song, B.; Jin, S. Modifying redox properties and local bonding of Co₃O₄ by CeO₂ enhances oxygen evolution catalysis in acid. Nat. Commun. 2021, 12, 3036.

Jing, H. Y.; Zhu, P.; Zheng, X. B.; Zhang, Z. D.; Wang, D. S.; Li, Y. D. Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis. Adv. Powder Mater. 2022, 1, 100013.

Wang, L. G.; Ma, N.; Wu, N.; Wang, X. G.; Xin, J. J.; Wang, D. S.; Lin, J. H.; Li, X. G.; Sun, J. L. Stable, efficient, copper coordination polymer-derived heterostructured catalyst for oxygen evolution under pH-universal conditions. ACS Appl. Mater. Interfaces 2021, 13, 25461–25471.

Liu, Z. H.; Du, Y.; Yu, R. H.; Zheng, M. B.; Hu, R.; Wu, J. S.; Xia, Y. Y.; Zhuang, Z. C.; Wang, D. S. Tuning mass transport in electrocatalysis down to sub-5 nm through nanoscale grade separation. Angew. Chem., Int. Ed. 2023, 62, e202212653.

Rong, C. L.; Shen, X. J.; Wang, Y.; Thomsen, L.; Zhao, T. W.; Li, Y. B.; Lu, X. Y.; Amal, R.; Zhao, C. Electronic structure engineering of single-atom Ru sites via Co-N₄ sites for bifunctional pH-universal water splitting. Adv. Mater. 2022, 34, 2110103.

Wan, L.; Xu, Z. A.; Xu, Q.; Wang, P. C.; Wang, B. G. Overall design of novel 3D-ordered MEA with drastically enhanced mass transport for alkaline electrolyzers. Energy Environ. Sci. 2022, 15, 1882–1892.

Browne, M. P.; Redondo, E.; Pumera, M. 3D printing for electrochemical energy applications. Chem. Rev. 2020, 120, 2783–2810.

Zheng, X. B.; Yang, J. R.; Xu, Z. F.; Wang, Q. S.; Wu, J. B.; Zhang, E. H.; Dou, S. X.; Sun, W. P.; Wang, D. S.; Li, Y. D. Ru-Co pair sites catalyst boosts the energetics for the oxygen evolution reaction. Angew. Chem., Int. Ed. 2022, 61, e202205946.

Lin, C.; Li, J. L.; Li, X. P.; Yang, S.; Luo, W.; Zhang, Y. J.; Kim, S. H.; Kim, D. H.; Shinde, S. S.; Li, Y. F. et al. In-situ reconstructed Ru atom array on α-MnO₂ with enhanced performance for acidic water oxidation. Nat. Catal. 2021, 4, 1012–1023.

Hao, S. Y.; Sheng, H. Y.; Liu, M.; Huang, J. Z.; Zheng, G. K.; Zhang, F.; Liu, X. N.; Su, Z. W.; Hu, J. J.; Qian, Y. et al. Torsion strained iridium oxide for efficient acidic water oxidation in proton exchange membrane electrolyzers. Nat. Nanotechnol. 2021, 16, 1371–1377.

Wen, Y. Z.; Chen, P. N.; Wang, L.; Li, S. Y.; Wang, Z. Y.; Abed, J.; Mao, X. N.; Min, Y. M.; Dinh, C. T.; Luna, P. D. et al. Stabilizing highly active Ru sites by suppressing lattice oxygen participation in acidic water oxidation. J. Am. Chem. Soc. 2021, 143, 6482–6490.

Shi, Z. P.; Li, J.; Wang, Y. B.; Liu, S. W.; Zhu, J. B.; Yang, J. H.; Wang, X.; Ni, J.; Jiang, Z.; Zhang, L. J. et al. Customized reaction route for ruthenium oxide towards stabilized water oxidation in high-performance PEM electrolyzers. Nat. Commun. 2023, 14, 843.

Sun, K. A.; Wu, X. Y.; Zhuang, Z. W.; Liu, L. Y.; Fang, J. J.; Zeng, L. Y.; Ma, J. G.; Liu, S. J.; Li, J. Z.; Dai, R. Y. et al. Interfacial water engineering boosts neutral water reduction. Nat. Commun. 2022, 13, 6260.

Fu, X. B.; Zhang, J. H.; Zhan, S. Q.; Xia, F. J.; Wang, C. J.; Ma, D. S.; Yue, Q.; Wu, J. S.; Kang, Y. J. High-entropy alloy nanosheets for fine-tuning hydrogen evolution. ACS Catal. 2022, 12, 11955–11959.

Cipriano, L. A.; Di Liberto, G.; Pacchioni, G. Superoxo and peroxo complexes on single-atom catalysts: Impact on the oxygen evolution reaction. ACS Catal. 2022, 12, 11682–11691.

He, Q.; Zhou, Y. Z.; Shou, H. W.; Wang, X. Y.; Zhang, P. J.; Xu, W. J.; Qiao, S. C.; Wu, C. Q.; Liu, H. J.; Liu, D. B. et al. Synergic reaction kinetics over adjacent ruthenium sites for superb hydrogen generation in alkaline media. Adv. Mater. 2022, 34, 2110604.

Dinh, C. T.; Jain, A.; De Arquer, F. P. G.; De Luna, P.; Li, J.; Wang, N.; Zheng, X. L.; Cai, J.; Gregory, B. Z.; Voznyy, O. et al. Multi-site electrocatalysts for hydrogen evolution in neutral media by destabilization of water molecules. Nat. Energy 2019, 4, 107–114.

Chen, J. D.; Chen, C. H.; Qin, M. K.; Li, B.; Lin, B. B.; Mao, Q.; Yang, H. B.; Liu, B.; Wang, Y. Reversible hydrogen spillover in Ru-WO_3−x enhances hydrogen evolution activity in neutral pH water splitting. Nat. Commun. 2022, 13, 5382.

Yang, Q.; Liu, H. X.; Yuan, P.; Jia, Y.; Zhuang, L. Z.; Zhang, H. W.; Yan, X. C.; Liu, G. H.; Zhao, Y. F.; Liu, J. Z. et al. Single carbon vacancy traps atomic platinum for hydrogen evolution catalysis. J. Am. Chem. Soc. 2022, 144, 2171–2178.

Zheng, Y.; Jiao, Y.; Vasileff, A.; Qiao, S. Z. The hydrogen evolution reaction in alkaline solution: From theory, single crystal models, to practical electrocatalysts. Angew. Chem., Int. Ed. 2018, 57, 7568–7579.

Zhang, J. Y.; Zhang, H. C.; Cheng, M. J.; Lu, Q. Tailoring the electrochemical production of H₂O₂: Strategies for the rational design of high-performance electrocatalysts. Small 2020, 16, 1902845.

Tian, Y. H.; Li, M.; Wu, Z. Z.; Sun, Q.; Yuan, D.; Johannessen, B.; Xu, L.; Wang, Y.; Dou, Y. H.; Zhao, H. J. et al. Edge-hosted atomic Co-N₄ sites on hierarchical porous carbon for highly selective two-electron oxygen reduction reaction. Angew. Chem., Int. Ed. 2022, 61, e202213296.

Mao, J. J.; He, C. T.; Pei, J. J.; Liu, Y.; Li, J.; Chen, W. X.; He, D. S.; Wang, D. S.; Li, Y. D. Isolated Ni atoms dispersed on Ru nanosheets: High-performance electrocatalysts toward hydrogen oxidation reaction. Nano Lett. 2020, 20, 3442–3448.

Han, A. L.; Wang, X. J.; Tang, K.; Zhang, Z. D.; Ye, C. L.; Kong, K. J.; Hu, H. B.; Zheng, L. R.; Jiang, P.; Zhao, C. X. et al. An adjacent atomic platinum site enables single-atom iron with high oxygen reduction reaction performance. Angew. Chem., Int. Ed. 2021, 60, 19262–19271.

Han, A.; Sun, W. M.; Wan, X.; Cai, D. D.; Wang, X. J.; Li, F.; Shui, J. L.; Wang, D. S. Construction of Co₄ atomic clusters to enable Fe-N₄ motifs with highly active and durable oxygen reduction performance. Angew. Chem., Int. Ed. 2023, 62, e202303185.

Wang, Y.; Wu, J.; Tang, S. H.; Yang, J. R.; Ye, C. L.; Chen, J.; Lei, Y. P.; Wang, D. S. Synergistic Fe-Se atom Pairs as bifunctional oxygen electrocatalysts boost low-temperature rechargeable Zn-Air battery. Angew. Chem., Int. Ed. 2023, 62, e202219191.

Kim, H. W.; Bukas, V. J.; Park, H.; Park, S.; Diederichsen, K. M.; Lim, J.; Cho, Y. H.; Kim, J.; Kim, W.; Han, T. H. et al. Mechanisms of two-electron and four-electron electrochemical oxygen reduction reactions at nitrogen-doped reduced graphene oxide. ACS Catal. 2020, 10, 852–863.

Deng, Y. J.; Luo, J. M.; Chi, B.; Tang, H. B.; Li, J.; Qiao, X. C.; Shen, Y. J.; Yang, Y. J.; Jia, C. M.; Rao, P. et al. Advanced atomically dispersed metal-nitrogen-carbon catalysts toward cathodic oxygen reduction in PEM fuel cells. Adv. Energy Mater. 2021, 11, 2101222.

Zhuang, Z. C.; Xia, L. X.; Huang, J. Z.; Zhu, P.; Li, Y.; Ye, C. L.; Xia, M. G.; Yu, R. H.; Lang, Z. Q.; Zhu, J. X. et al. Continuous modulation of electrocatalytic oxygen reduction activities of single-atom catalysts through p-n junction rectification. Angew. Chem., Int. Ed. 2023, 62, e202212335.

Cui, T. T.; Wang, Y. P.; Ye, T.; Wu, J.; Chen, Z. Q.; Li, J.; Lei, Y. P.; Wang, D. S.; Li, Y. D. Engineering dual single-atom sites on 2D ultrathin N-doped carbon nanosheets attaining ultra-low-temperature zinc-air battery. Angew. Chem., Int. Ed. 2022, 61, e202115219.

Kim, S.; Lee, Y. M. Two-dimensional nanosheets and membranes for their emerging technologies. Curr. Opin. Chem. Eng. 2023, 39, 100893.

Hu, C.; Xu, J. J.; Tan, Y. Z.; Huang, X. Q. Recent advances of ruthenium-based electrocatalysts for hydrogen energy. Trends Chem. 2023, 5, 225–239.

Liu, S. S.; Wang, M. F.; Qian, T.; Ji, H. Q.; Liu, J.; Yan, C. L. Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation. Nat. Commun. 2019, 10, 3898.

Sim, H. Y. F.; Chen, J. R. T.; Koh, C. S. L.; Lee, H. K.; Han, X. M.; Phan-Quang, G. C.; Pang, J. Y.; Lay, C. L.; Pedireddy, S.; Phang, I. Y. et al. ZIF-induced d-band modification in a bimetallic nanocatalyst:Achieving over 44% efficiency in the ambient nitrogen reduction reaction. Angew. Chem., Int. Ed. 2020, 59, 16997–17003.

Sahoo, S.; Dekel, D. R.; Maric, R.; Alpay, S. P. Atomistic insights into the hydrogen oxidation reaction of palladium-ceria bifunctional catalysts for anion-exchange membrane fuel cells. ACS Catal. 2021, 11, 2561–2571.

Gruber, N.; Galloway, J. N. An earth-system perspective of the global nitrogen cycle. Nature 2008, 451, 293–296.

Chen, G. F.; Cao, X. R.; Wu, S. Q.; Zeng, X. Y.; Ding, L. X.; Zhu, M.; Wang, H. H. Ammonia electrosynthesis with high selectivity under ambient conditions via a Li⁺ incorporation strategy. J. Am. Chem. Soc. 2017, 139, 9771–9774.

Guo, C. X.; Ran, J. R.; Vasileff, A.; Qiao, S. Z. Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH₃) under ambient conditions. Energy Environ. Sci. 2018, 11, 45–56.

Van Der Ham, C. J. M.; Koper, M. T. M.; Hetterscheid, D. G. H. Challenges in reduction of dinitrogen by proton and electron transfer. Chem. Soc. Rev. 2014, 43, 5183–5191.

Li, S. J.; Bao, D.; Shi, M. M.; Wulan, B. R.; Yan, J. M.; Jiang, Q. Amorphizing of Au nanoparticles by CeO_x-RGO hybrid support towards highly efficient electrocatalyst for N₂ reduction under ambient conditions. Adv. Mater. 2017, 29, 1700001.

Wang, J.; Yu, L.; Hu, L.; Chen, G.; Xin, H. L.; Feng, X. F. Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential. Nat. Commun. 2018, 9, 1795.

Wang, M. F.; Liu, S. S.; Qian, T.; Liu, J.; Zhou, J. Q.; Ji, H. Q.; Xiong, J.; Zhong, J.; Yan, C. L. Over 56.55% faradaic efficiency of ambient ammonia synthesis enabled by positively shifting the reaction potential. Nat. Commun. 2019, 10, 341.

Fu, X. B.; Pedersen, J. B.; Zhou, Y. Y.; Saccoccio, M.; Li, S. F.; Sažinas, R.; Li, K.; Andersen, S. Z.; Xu, A. N.; Deissler, N. H. et al. Continuous-flow electrosynthesis of ammonia by nitrogen reduction and hydrogen oxidation. Science 2023, 379, 707–712.

Shen, H. D.; Choi, C.; Masa, J.; Li, X.; Qiu, J. S.; Jung, Y.; Sun, Z. Y. Electrochemical ammonia synthesis: Mechanistic understanding and catalyst design. Chem 2021, 7, 1708–1754.

Yu, X. M.; Han, P.; Wei, Z. X.; Huang, L. S.; Gu, Z. X.; Peng, S. J.; Ma, J. M.; Zheng, G. F. Boron-doped graphene for electrocatalytic N₂ reduction. Joule 2018, 2, 1610–1622.

Chen, S. H.; Wang, B. Q.; Zhu, J. X.; Wang, L. Q.; Ou, H. H.; Zhang, Z. D.; Liang, X.; Zheng, L. R.; Zhou, L.; Su, Y. Q. et al. Lewis acid site-promoted single-atomic Cu catalyzes electrochemical CO₂ methanation. Nano Lett. 2021, 21, 7325–7331.

Zhu, J. B.; Xiao, M. L.; Ren, D. Z.; Gao, R.; Liu, X. Z.; Zhang, Z.; Luo, D.; Xing, W.; Su, D.; Yu, A. P. et al. Quasi-covalently coupled Ni-Cu atomic pair for synergistic electroreduction of CO₂. J. Am. Chem. Soc. 2022, 144, 9661–9671.

Qian, Y.; Liu, Y.; Zhao, Y.; Zhang, X.; Yu, G. Single vs double atom catalyst for N₂ activation in nitrogen reduction reaction: A DFT perspective. EcoMat 2020, 2, e12014.

Nitopi, S.; Bertheussen, E.; Scott, S. B.; Liu, X. Y.; Engstfeld, A. K.; Horch, S.; Seger, B.; Stephens, I. E. L.; Chan, K.; Hahn, C. et al. Progress and perspectives of electrochemical CO₂ reduction on copper in aqueous electrolyte. Chem. Rev. 2019, 119, 7610–7672.

De Luna, P.; Hahn, C.; Higgins, D.; Jaffer, S. A.; Jaramillo, T. F.; Sargent, E. H. What would it take for renewably powered electrosynthesis to displace petrochemical processes. Science 2019, 364, eaav3506.

Gu, J.; Hsu, C. S.; Bai, L. C.; Chen, H. M.; Hu, X. L. Atomically dispersed Fe³⁺ sites catalyze efficient CO₂ electroreduction to CO. Science 2019, 364, 1091–1094.

Wang, X. L.; De Araújo, J. F.; Ju, W.; Bagger, A.; Schmies, H.; Kühl, S.; Rossmeisl, J.; Strasser, P. Mechanistic reaction pathways of enhanced ethylene yields during electroreduction of CO₂-CO co-feeds on Cu and Cu-tandem electrocatalysts. Nat. Nanotechnol. 2019, 14, 1063–1070.

Birdja, Y. Y.; Pérez-Gallent, E.; Figueiredo, M. C.; Göttle, A. J.; Calle-Vallejo, F.; Koper, M. T. M. Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels. Nat. Energy 2019, 4, 732–745.

Zhang, Z. D.; Zhu, J. X.; Chen, S. H.; Sun, W. M.; Wang, D. S. Liquid fluxional Ga single atom catalysts for efficient electrochemical CO₂ reduction. Angew. Chem., Int. Ed. 2023, 62, e202215136.

Shen, Y.; Ren, C. J.; Zheng, L. R.; Xu, X. Y.; Long, R.; Zhang, W. Q.; Yang, Y.; Zhang, Y. C.; Yao, Y. F.; Chi, H. Q. et al. Room-temperature photosynthesis of propane from CO₂ with Cu single atoms on vacancy-rich TiO₂. Nat. Commun. 2023, 14, 1117.

Huang, J. E.; Li, F. W.; Ozden, A.; Rasouli, A. S.; De Arquer, F. P. G.; Liu, S. J.; Zhang, S. Z.; Luo, M. C.; Wang, X.; Lum, Y. et al. CO₂ electrolysis to multicarbon products in strong acid. Science 2021, 372, 1074–1078.

Jiao, L.; Yang, W. J.; Wan, G.; Zhang, R.; Zheng, X. S.; Zhou, H.; Yu, S. H.; Jiang, H. L. Single-atom electrocatalysts from multivariate metal-organic frameworks for highly selective reduction of CO₂ at low pressures. Angew. Chem., Int. Ed. 2020, 59, 20589–20595.

Bao, H. H.; Qiu, Y.; Peng, X. Y.; Wang, J. A.; Mi, Y. Y.; Zhao, S. Z.; Liu, X. J.; Liu, Y. F.; Cao, R.; Zhuo, L. C. et al. Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products. Nat. Commun. 2021, 12, 238.

Shang, H. S.; Wang, T.; Pei, J. J.; Jiang, Z. L.; Zhou, D. N.; Wang, Y.; Li, H. J.; Dong, J. C.; Zhuang, Z. B.; Chen, W. X. et al. Design of a single-atom indium^δ+-N₄ interface for efficient electroreduction of CO₂ to formate. Angew. Chem., Int. Ed. 2020, 59, 22465–22469.

Yang, J. R.; Li, W. H.; Wang, D. S.; Li, Y. D. Single-atom materials: Small structures determine macroproperties. Small Struct. 2021, 2, 2000051.

Cai, Y. M.; Fu, J. J.; Zhou, Y.; Chang, Y. C.; Min, Q. H.; Zhu, J. J.; Lin, Y. H.; Zhu, W. L. Insights on forming N, O-coordinated Cu single-atom catalysts for electrochemical reduction CO₂ to methane. Nat. Commun. 2021, 12, 586.

Das, S.; Pérez-Ramírez, J.; Gong, J. L.; Dewangan, N.; Hidajat, K.; Gates, B. C.; Kawi, S. Core–shell structured catalysts for thermocatalytic, photocatalytic, and electrocatalytic conversion of CO₂. Chem. Soc. Rev. 2020, 49, 2937–3004.

Yang, Y.; Li, Y. K.; Zhao, Y. X.; Wei, G. P.; Ren, Y.; Asmis, K. R.; He, S. G. Catalytic Co-conversion of CH₄ and CO₂ mediated by rhodium-titanium oxide anions RhTiO₂⁻. Angew. Chem., Int. Ed. 2021, 60, 13788–13792.

Shi, L.; Yang, G. H.; Tao, K.; Yoneyama, Y.; Tan, Y. S.; Tsubaki, N. An introduction of CO₂ conversion by dry reforming with methane and new route of low-temperature methanol synthesis. Acc. Chem. Res. 2013, 46, 1838–1847.

Galvis, H. M. T.; De Jong, K. P. Catalysts for production of lower olefins from synthesis gas: A review. ACS Catal. 2013, 3, 2130–2149.

Pakhare, D.; Spivey, J. A review of dry (CO₂) reforming of methane over noble metal catalysts. Chem. Soc. Rev. 2014, 43, 7813–7837.

Posada-Borbón, A.; Grönbeck, H. A first-principles-based microkinetic study of CO₂ reduction to CH₃OH over In₂O₃(110). ACS Catal. 2021, 11, 9996–10006.

Liu, B.; Liu, J.; Xin, L.; Zhang, T.; Xu, Y. B.; Jiang, F.; Liu, X. H. Unraveling reactivity descriptors and structure sensitivity in low-temperature NH₃-SCR reaction over CeTiO_x catalysts: A combined computational and experimental study. ACS Catal. 2021, 11, 7613–7636.

Luo, Z. X.; Castleman, A. W. Jr; Khanna, S. N. Reactivity of metal clusters. Chem. Rev. 2016, 116, 14456–14492.

Zhao, Y. X.; Li, Z. Y.; Yang, Y.; He, S. G. Methane activation by gas phase atomic clusters. Acc. Chem. Res. 2018, 51, 2603–2610.

Geng, C. Y.; Weiske, T.; Li, J. L.; Shaik, S.; Schwarz, H. Intrinsic reactivity of diatomic 3d transition-metal carbides in the thermal activation of methane: Striking electronic structure effects. J. Am. Chem. Soc. 2019, 141, 599–610.

Miller, G. B. S.; Esser, T. K.; Knorke, H.; Gewinner, S.; Schöllkopf, W.; Heine, N.; Asmis, K. R.; Uggerud, E. Spectroscopic identification of a bidentate binding motif in the anionic magnesium-CO₂ complex ([ClMgCO₂]⁻). Angew. Chem., Int. Ed. 2014, 53, 14407–14410.

Zhao, D.; Tian, X. X.; Doronkin, D. E.; Han, S. L.; Kondratenko, V. A.; Grunwaldt, J. D.; Perechodjuk, A.; Vuong, T. H.; Rabeah, J.; Eckelt, R. et al. In situ formation of ZnO_x species for efficient propane dehydrogenation. Nature 2021, 599, 234–238.

Motagamwala, A. H.; Almallahi, R.; Wortman, J.; Igenegbai, V. O.; Linic, S. Stable and selective catalysts for propane dehydrogenation operating at thermodynamic limit. Science 2021, 373, 217–222.

Hannagan, R. T.; Giannakakis, G.; Réocreux, R.; Schumann, J.; Finzel, J.; Wang, Y. C.; Michaelides, A.; Deshlahra, P.; Christopher, P.; Flytzani-Stephanopoulos, M. et al. First-principles design of a single-atom-alloy propane dehydrogenation catalyst. Science 2021, 372, 1444–1447.

Chang, X.; Zhao, Z. J.; Lu, Z. P.; Chen, S.; Luo, R.; Zha, S.; Li, L. L.; Sun, G. D.; Pei, C. L.; Gong, J. L. Designing single-site alloy catalysts using a degree-of-isolation descriptor. Nat. Nanotechnol. 2023, 18, 611–616.

Correa-Baena, J. P.; Hippalgaonkar, K.; Van Duren, J.; Jaffer, S.; Chandrasekhar, V. R.; Stevanovic, V.; Wadia, C.; Guha, S.; Buonassisi, T. Accelerating materials development via automation, machine learning, and high-performance computing. Joule 2018, 2, 1410–1420.

Krivanek, O. L.; Chisholm, M. F.; Nicolosi, V.; Pennycook, T. J.; Corbin, G. J.; Dellby, N.; Murfitt, M. F.; Own, C. S.; Szilagyi, Z. S.; Oxley, M. P. et al. Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy. Nature 2010, 464, 571–574.

Sun, Z. H.; Liu, Q. H.; Yao, T.; Yan, W. S.; Wei, S. Q. X-ray absorption fine structure spectroscopy in nanomaterials. Sci. China Mater. 2015, 58, 313–341.

Funke, H.; Scheinost, A. C.; Chukalina, M. Wavelet analysis of extended X-ray absorption fine structure data. Phys. Rev. B 2005, 71, 094110.

Liu, J. C.; Wang, Y. G.; Li, J. Toward rational design of oxide-supported single-atom catalysts: Atomic dispersion of gold on ceria. J. Am. Chem. Soc. 2017, 139, 6190–6199.

Xie, Y. C.; Zhang, C.; Hu, X. Q.; Zhang, C.; Kelley, S. P.; Atwood, J. L.; Lin, J. Machine learning assisted synthesis of metal-organic nanocapsules. J. Am. Chem. Soc. 2020, 142, 1475–1481.