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Considering intracellular hydrogen peroxide (H2O2) plays pivotal roles in the regulation of serial biological processes, the in-situ detection of intracellular H2O2 has attracted an extensive attention. In the present work, an atomically dispersed diatomic active sites Nanozymes (FeN3/PtN4-single-atom nanozymes (SAzyme)) was prepared exhibiting enhanced peroxidase-like activity. The obvious synergistic effect between Fe–Pt heteronuclear diatomic active sites was confirmed by series of characterization and density functional theory (DFT). The peroxidase-like activity of Fe-sites could be substantially enhanced by the bonded Pt-sites via the modulation effect. As a consequence, the gap between the d-band centre (εd) of Fe 3d orbitals and the Fermi energy level was narrowed and the electronic interaction could be strengthened, leading to a lower free energy barrier and a lower activation energy as well as fortified metal–O bonding in the kinetic pathway. Therefore, the constructed FeN3/PtN4-SAzyme exhibited higher peroxidase-like activity than that of FeN4-SAzyme. The FeN3/PtN4-SAzyme-assisted oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) facilitated the colorimetric detection of dopamine (DA), an important biomolecule. The linear detection range and limit of detection (LOD) of DA and H2O2 were 1–10 μM, 0.01–1.0 mM and 0.109 μM, 7.97 μM, respectively. In addition, the constructed SAzymes were also applied for the in-situ detection of intracellular H2O2, expanding the application scope of the newborn SAzymes.
Gao, L. Z.; Zhuang, J.; Nie, L.; Zhang, J. B.; Zhang, Y.; Gu, N.; Wang, T. H.; Feng, J.; Yang, D. L.; Perrett, S. et al. Intrinsic peroxidase-like activity of ferromagnetic nanoparticles. Nat. Nanotechnol. 2007, 2, 577–583.
Liang, M. M.; Yan, X. Y. Nanozymes: From new concepts, mechanisms, and standards to applications. Acc. Chem. Res. 2019, 52, 2190–2200.
Wu, J. J. X.; Wang, X. Y.; Wang, Q.; Lou, Z. P.; Li, S. R.; Zhu, Y. Y.; Qin, L.; Wei, H. Nanomaterials with enzyme-like characteristics (nanozymes): Next-generation artificial enzymes (II). Chem. Soc. Rev. 2019, 48, 1004–1076.
Zhu, Y.; Wang, W. Y.; Cheng, J. J.; Qu Y. T.; Dai, Y.; Liu, M. M.; Yu, J. N.; Wang, C. M.; Wang, H. J.; Wang, S. C. et al. Stimuli-responsive manganese single-atom nanozyme for tumor therapy via integrated cascade reactions. Angew. Chem., Int. Ed. 2021, 60, 9480–9488.
Wang, Q. Q.; Wei, H.; Zhang, Z. Q.; Wang, E. K.; Dong, S. J. Nanozyme: An emerging alternative to natural enzyme for biosensing and immunoassay. TrAC Trends Anal. Chem. 2018, 105, 218–224.
Zhao, Y. T.; Yang, M. M.; Fu, Q. Q.; Ouyang, H.; Wen, W.; Song, Y.; Zhu, C. Z.; Lin, Y. H.; Du, D. A nanozyme- and ambient light-based smartphone platform for simultaneous detection of dual biomarkers from exposure to organophosphorus pesticides. Anal. Chem. 2018, 90, 7391–7398.
Cheng, N.; Li, J. C.; Liu, D.; Lin, Y. H.; Du, D. Single-atom nanozyme based on nanoengineered Fe–N–C catalyst with superior peroxidase-like activity for ultrasensitive bioassays. Small 2019, 15, 1901485.
Jiang, D. W.; Ni, D. L.; Rosenkrans, Z. T.; Huang, P.; Yan, X. Y.; Cai, W. B. Nanozyme: New horizons for responsive biomedical applications. Chem. Soc. Rev. 2019, 48, 3683–3704.
Huo, M. F.; Wang, L. Y.; Chen, Y.; Shi, J. L. Tumor-selective catalytic nanomedicine by nanocatalyst delivery. Nat. Commun. 2017, 8, 357.
Li, X. N.; Huang, X.; Xi, S. B.; Miao, S.; Ding, J.; Cai, W. Z.; Liu, S.; Yang, X. L.; Yang, H. B.; Gao, J. J. et al. Single cobalt atoms anchored on porous n-doped graphene with dual reaction sites for efficient Fenton-like catalysis. J. Am. Chem. Soc. 2018, 140, 12469–12475.
Hu, P.; Han, L.; Dong, S. J. A facile one-pot method to synthesize a polypyrrole/hemin nanocomposite and its application in biosensor, dye removal, and photothermal therapy. ACS Appl. Mater. Interfaces 2014, 6, 500–506.
Hu, Z. F.; Dai, Z. C.; Hu, X. W.; Yang, B. C.; Liu, Q. Y.; Gao, C. H.; Zheng, X. W.; Yu, Y. Q. A facile preparation of FePt-loaded few-layer MoS2 nanosheets nanocomposites (F-MoS2-FePt NCs) and their application for colorimetric detection of H2O2 in living cells. J. Nanobiotechnol. 2019, 17, 38.
Hu, Z. F.; Yin, Y. H.; Liu, Q. Y.; Zheng, X. W. A functional FePt@MOFs (MIL-101(Fe)) nano-platform for high efficient colorimetric determination of H2O2. Analyst 2019, 144, 2716–2724.
Jiao, L.; Xu, W. Q.; Yan, H. Y.; Wu, Y.; Liu, C. R.; Du, D.; Lin, Y. H.; Zhu, C. Z. Fe–N–C single-atom nanozymes for the intracellular hydrogen peroxide detection. Anal. Chem. 2019, 91, 11994–11999.
Li, Z. Z.; Xin, Y. M.; Wu, W. L.; Fu, B. H.; Zhang, Z. H. Topotactic conversion of copper(I) phosphide nanowires for sensitive electrochemical detection of H2O2 release from living cells. Anal. Chem. 2016, 88, 7724–7729.
Jiang, X. Y.; Wang, H. J.; Yuan, R.; Chai, Y. Q. Functional three-dimensional porous conductive polymer hydrogels for sensitive electrochemiluminescence in situ detection of H2O2 released from live cells. Anal. Chem. 2018, 90, 8462–8469.
Shi, Q. R.; Song, Y.; Zhu, C. Z.; Yang, H. P.; Du, D.; Lin, Y. H. Mesoporous Pt nanotubes as a novel sensing platform for sensitive detection of intracellular hydrogen peroxide. ACS Appl. Mater. Interfaces 2015, 7, 24288–24295.
Xi, J. Q.; Zhang, R. F.; Wang, L. M.; Xu, W.; Liang, Q.; Li, J. Y.; Jiang, J.; Yang, Y. L.; Yan, X. Y.; Fan, K. L. et al. A nanozyme-based artificial peroxisome ameliorates hyperuricemia and ischemic stroke. Adv. Funct. Mater. 2021, 31, 2007130.
Xiang, H. J.; Feng, W.; Chen, Y. Single-atom catalysts in catalytic biomedicine. Adv. Mater. 2020, 32, 1905994.
Chen, M. M.; Yang, B. C.; Zhu, J. L.; Liu, H.; Zhang, X.; Zheng, X. W.; Liu, Q. Y. FePt nanoparticles-decorated graphene oxide nanosheets as enhanced peroxidase mimics for sensitive response to H2O2. Mater. Sci. Eng. C 2018, 90, 610–620.
Ding, Y. N.; Yang, B. C.; Liu, H.; Liu, Z. X.; Zhang, X.; Zheng, X. W.; Liu, Q. Y. FePt-Au ternary metallic nanoparticles with the enhanced peroxidase-like activity for ultrafast colorimetric detection of H2O2. Sens. Actuators B:Chem. 2018, 259, 775–783.
Zheng, Y.; Jiao, Y.; Zhu, Y. H.; Cai, Q. R.; Vasileff, A.; Li, L. H.; Han, Y.; Chen, Y.; Qiao, S. Z. Molecule-level g-C3N4 coordinated transition metals as a new class of electrocatalysts for oxygen electrode reactions. J. Am. Chem. Soc. 2017, 139, 3336–3339.
Jiao, L.; Yan, H. Y.; Wu, Y.; Gu, W. L.; Zhu, C. Z.; Du, D.; Lin, Y. H. When nanozymes meet single-atom catalysis. Angew. Chem., Int. Ed. 2020, 59, 2565–2576.
Peng, Y.; Lu, B. Z.; Chen, S. W. Carbon-supported single atom catalysts for electrochemical energy conversion and storage. Adv. Mater. 2018, 30, 1801995.
Zhang, H. B.; Lu, X. F.; Wu, Z. P.; Lou, X. W. D. Emerging multifunctional single-atom catalysts/nanozymes. ACS Cent. Sci. 2020, 6, 1288–1301.
Jiao, L.; Wu, J. B.; Zhong, H.; Zhang, Y.; Xu, W. Q.; Wu, Y.; Chen, Y. F.; Yan, H. Y.; Zhang, Q. H.; Gu, W. L. et al. Densely isolated FeN4 sites for peroxidase mimicking. ACS Catal. 2020, 10, 6422–6429.
Sun, X. H.; Tuo, Y. X.; Ye, C. L.; Chen, C.; Lu, Q.; Li, G. N.; Jiang, P.; Chen, S. H.; Zhu, P.; Ma, M. et al. Phosphorus induced electron localization of single iron sites for boosted CO2 electroreduction reaction. Angew. Chem., Int. Ed. 2021, 60, 23614–23618.
Cui, T. T.; Ma, L. N.; Wang, S. B.; Ye, C. L.; Liang, X.; Zhang, Z. D.; Meng, G.; Zheng, L. R.; Hu, H. S.; Zhang, J. W. et al. Atomically dispersed Pt–N3C1 sites enabling efficient and selective electrocatalytic C–C bond cleavage in lignin models under ambient conditions. J. Am. Chem. Soc. 2021, 143, 9429–9439.
Xu, B. L.; Wang, H.; Wang, W. W.; Gao, L. Z.; Li, S. S.; Pan, X. T.; Wang, H. Y.; Yang, H. L.; Meng, X. Q.; Wu, Q. W. et al. A single-atom nanozyme for wound disinfection applications. Angew. Chem. 2019, 131, 4965–4970.
Lin, S. C.; Wei, H. Design of high performance nanozymes: A single-atom strategy. Sci. China Life Sci. 2019, 62, 710–712.
Huang, L.; Chen, J. X.; Gan, L. F.; Wang, J.; Dong, S. J. Single-atom nanozymes. Sci. Adv. 2019, 5, eaav5490.
Jiao, L.; Yan, H. Y.; Wu, Y.; Gu, W. L.; Zhu, C. Z.; Du, D.; Lin, Y. H. When nanozymes meet single-atom catalysis. Angew. Chem. 2020, 132, 2585–2596.
Wu, Y.; Wu, J. B.; Jiao, L.; Xu, W. Q.; Wang, H. J.; Wei, X. Q.; Gu, W. L.; Ren, G. X.; Zhang, N.; Zhang, Q. H. et al. Cascade reaction system integrating single-atom nanozymes with abundant Cu sites for enhanced biosensing. Anal. Chem. 2020, 92, 3373–3379.
Ji, S. F.; Jiang, B.; Hao, H. G.; Chen, Y. J.; Dong, J. C.; Mao, Y.; Zhang, Z. D.; Gao, R.; Chen, W. X.; Zhang, R. F. et al. Matching the kinetics of natural enzymes with a single-atom iron nanozyme. Nat. Catal. 2021, 4, 407–417.
Gao, G. P.; Jiao, Y.; Waclawik, E. R.; Du, A. J. Single atom (Pd/Pt) supported on graphitic carbon nitride as an efficient photocatalyst for visible-light reduction of carbon dioxide. J. Am. Chem. Soc. 2016, 138, 6292–6297.
Wang, S. F.; Li, F. Y.; Qiao, R. R.; Hu, X.; Liao, H. W.; Chen, L. M.; Wu, J. H.; Wu, H. H.; Zhao, M.; Liu, J. N. et al. Arginine-rich manganese silicate nanobubbles as a ferroptosis-inducing agent for tumor-targeted theranostics. ACS Nano 2018, 12, 12380–12392.
Sun, W.; Du, L.; Tan, Q.; Zhou, J. G.; Hu, Y. F.; Du, C. Y.; Gao, Y. Z.; Yin, G. P. Engineering of nitrogen coordinated single cobalt atom moieties for oxygen electroreduction. ACS Appl. Mater. Interfaces 2019, 11, 41258–41266.
Chen, Y. J.; Wang, P. X.; Hao, H. G.; Hong, J. J.; Li, H. J.; Ji, S. F.; Li, A.; Gao, R.; Dong, J. C.; Han, X. D. et al. Thermal atomization of platinum nanoparticles into single atoms: An effective strategy for engineering high-performance nanozymes. J. Am. Chem. Soc. 2021, 143, 18643–18651.
Ding, H.; Hu, B.; Zhang, B.; Zhang, H.; Yan, X. Y.; Nie, G. H.; Liang, M. M. Carbon-based nanozymes for biomedical applications. Nano Res. 2021, 14, 570–583.
Ding, H.; Wang, D. J.; Huang, H. B.; Chen, X. Z.; Wang, J.; Sun, J. J.; Zhang, J. L.; Lu, L.; Miao, B. P.; Cai, Y. J. et al. Black phosphorus quantum dots as multifunctional nanozymes for tumor photothermal/catalytic synergistic therapy. Nano Res. 2022, 15, 1554–1563.
Yin, S. H.; Yang, J.; Han, Y.; Li, G.; Wan, L. Y.; Chen, Y. H.; Chen, C.; Qu, X. M.; Jiang, Y. X.; Sun, S. G. Construction of highly active metal-containing nanoparticles and FeCo–N4 composite sites for the acidic oxygen reduction reaction. Angew. Chem., Int. Ed. 2020, 59, 21976–21979.
Li, X. Z.; Fang, Y. Y.; Wang, J.; Fang, H. Y.; Xi, S. B.; Zhao, X. X.; Xu, D. Y.; Xu, H. M.; Yu, W.; Hai, X. et al. Ordered clustering of single atomic Te vacancies in atomically thin PtTe2 promotes hydrogen evolution catalysis. Nat. Commun. 2021, 12, 2351.
Shi, Y.; Ma, Z. R.; Xiao, Y. Y.; Yin, Y. C.; Huang, W. M.; Huang, Z. C.; Zheng, Y. Z.; Mu, F. Y.; Huang, R.; Shi, G. Y. et al. Electronic metal-support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction. Nat. Commun. 2021, 12, 3021.
Jiao, L.; Zhu, J. T.; Zhang, Y.; Yang, W. J.; Zhou, S. Y.; Li, A. W.; Xie, C. F.; Zheng, X. S.; Zhou, W.; Yu, S. H. et al. Non-bonding interaction of neighboring Fe and Ni single-atom pairs on MOF-derived n-doped carbon for enhanced CO2 electroreduction. J. Am. Chem. Soc. 2021, 143, 19417–19424.
Chen, Y. W.; Ding, R.; Li, J.; Liu, J. G. Highly active atomically dispersed platinum-based electrocatalyst for hydrogen evolution reaction achieved by defect anchoring strategy. Appl. Catal. B:Environ. 2022, 301, 120830.
Kumar, A.; Bui, V. Q.; Lee, J.; Wang, L. L.; Jadhav, A. R.; Liu, X. H.; Shao, X. D.; Liu, Y.; Yu, J. M.; Hwang, Y. et al. Moving beyond bimetallic-alloy to single-atom dimer atomic-interface for all-pH hydrogen evolution. Nat. Commun. 2021, 12, 6766.
Xiao, M. L.; Zhu, J. B.; Li, S.; Li, G. R.; Liu, W. W.; Deng, Y. P.; Bai, Z. Y.; Ma, L.; Feng, M.; Wu, T. P. et al. 3d-Orbital occupancy regulated Ir–Co atomic pair toward superior bifunctional oxygen electrocatalysis. ACS Catal. 2021, 11, 8837–8846.
Li, X.; He, Y. H.; Cheng, S. B.; Li, B. Y.; Zeng, Y. C.; Xie, Z. H.; Meng, Q. P.; Ma, L.; Kisslinger, K.; Tong, X. et al. Atomic structure evolution of Pt-Co binary catalysts: Single metal sites versus intermetallic nanocrystals. Adv. Mater. 2021, 33, 2106371.
Li, Y. Z.; Wei, B.; Zhu, M. H.; Chen, J. C.; Jiang, Q. K.; Yang, B.; Hou, Y.; Lei, L. C.; Li, Z. J.; Zhang, R. F. et al. Synergistic effect of atomically dispersed Ni–Zn pair sites for enhanced CO2 electroreduction. Adv. Mater. 2021, 33, 2102212.
Wang, Z.; Jin, X. Y.; Zhu, C.; Liu, Y. P.; Tan, H.; Ku, R. Q.; Zhang, Y. Q.; Zhou, L. J.; Liu, Z.; Hwang, S. J. et al. Atomically dispersed Co2–N6 and Fe–N4 costructures boost oxygen reduction reaction in both alkaline and acidic media. Adv. Mater. 2021, 33, 2104718.
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.
Cao, S. W.; Li, H.; Tong, T.; Chen, H. C.; Yu, A. C.; Yu, J. G.; Chen, H. M. Single-atom engineering of directional charge transfer channels and active sites for photocatalytic hydrogen evolution. Adv. Funct. Mater. 2018, 28, 1802169.
Li, X. G.; Bi, W. T.; Zhang, L.; Tao, S.; Chu, W. S.; Zhang, Q.; Luo, Y.; Wu, C. Z.; Xie, Y. Single-atom Pt as Co-catalyst for enhanced photocatalytic H2 evolution. Adv. Mater. 2016, 28, 2427–2431.
Garlyyev, B.; Kratzl, K.; Rück, M.; Michalička, J.; Fichtner, J.; Macak, J. M.; Kratky, T.; Gunther, S.; Cokoja, M.; Bandarenka, A. S. et al. Optimizing the size of platinum nanoparticles for enhanced mass activity in the electrochemical oxygen reduction reaction. Angew. Chem., Int. Ed. 2019, 58, 9596–9600.
Han, A.; 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.
Du, F. X.; Liu, L. C.; Wu, Z. H.; Zhao, Z. Y.; Geng, W.; Zhu, B. H.; Ma, T.; Xiang, X.; Ma, L.; Cheng, C. et al. Pd-single-atom coordinated biocatalysts for chem-/sono-/photo-trimodal tumor therapies. Adv. Mater. 2021, 33, 2101095.
Lu, X. Y.; Gao, S. S.; Lin, H.; Yu, L. D.; Han, Y. H.; Zhu, P.; Bao, W. C.; Yao, H. L.; Chen, Y.; Shi, J. L. Bioinspired copper single-atom catalysts for tumor parallel catalytic therapy. Adv. Mater. 2020, 32, 2002246.
Ishibashi, K. I.; Fujishima, A.; Watanabe, T.; Hashimoto, K. Quantum yields of active oxidative species formed on TiO2 photocatalyst. J. Photochem. Photobiol. A:Chem. 2000, 134, 139–142.
Kaur, B.; Pandiyan, T.; Satpati, B.; Srivastava, R. Simultaneous and sensitive determination of ascorbic acid, dopamine, uric acid, and tryptophan with silver nanoparticles-decorated reduced graphene oxide modified electrode. Colloids Surf. B:Biointerf. 2013, 111, 97–106.
Li, W. H.; Ma, L.; Wu, B. X.; Zhang, Y.; Li, Z. A chemically reduced graphene oxide-Au nanocage composite for the electrochemical detection of dopamine and uric acid. Anal. Methods 2017, 9, 3819–3824.
Ivanova, M. N.; Grayfer, E. D.; Plotnikova, E. E.; Kibis, L. S.; Darabdhara, G.; Boruah, P. K.; Das, M. R.; Fedorov, V. E. Pt-decorated boron nitride nanosheets as artificial nanozyme for detection of dopamine. ACS Appl. Mater. Interfaces 2019, 11, 22102–22112.