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Molybdenum disulfide (MoS2), a promising non-precious electrocatalyst for the hydrogen evolution reaction with two-dimensional layered structure, has received increasing attention in recent years. Its electrocatalytic performance has been limited by the low active site content and poor conductivity. Herein, we report a facile and general ultrafast laser ablation method to synthesize MoS2 quantum dots (MS-QDs) for electrocatalytic HER with fully exposed active sites and highly enhanced conductivity. The MS-QDs were prepared by ultrafast laser ablation of the corresponding bulk material in aqueous solution, during which they were partially oxidized and formed defective structures. The as-prepared MS-QDs demonstrated high activity and stability in the electrocatalytic HER, owing to their very large surface area, defective structure, abundance of active sites, and high conductivity. The present MS-QDs can also find application in optics, sensing, energy storage, and conversion technologies.
Zhang, B.; Zheng, X. L.; Voznyy, O.; Comin, R.; Bajdich, M.; Garcia-Melchor, M.; Han, L.; Xu, J.; Liu, M.; Zheng, L. et al. Homogeneously dispersed multimetal oxygen-evolving catalysts. Science 2016, 352, 333-337.
Sun, C. C.; Dong, Q. C.; Yang, J.; Dai, Z. Y.; Lin, J. J.; Chen, P.; Huang, W.; Dong, X. C. Metal-organic framework derived CoSe2 nanoparticles anchored on carbon fibers as bifunctional electrocatalysts for efficient overall water splitting. Nano Res. 2016, 9, 2234-2243.
Zou, X. X.; Zhang, Y. Noble metal-free hydrogen evolution catalysts for water splitting. Chem. Soc. Rev. 2015, 44, 5148-5180.
Gong, M.; Dai, H. J. A mini review of NiFe-based materials as highly active oxygen evolution reaction electrocatalysts. Nano Res. 2015, 8, 23-39.
Morales-Guio, C. G.; Stern, L. A.; Hu, X. L. Nanostructured hydrotreating catalysts for electrochemical hydrogen evolution. Chem. Soc. Rev. 2014, 43, 6555-6569.
Geng, X. M.; Sun, W. W.; Wu, W.; Chen, B.; Al-Hilo, A.; Benamara, M.; Zhu, H. L.; Watanabe, F.; Cui, J. B.; Chen, T. P. Pure and stable metallic phase molybdenum disulfide nanosheets for hydrogen evolution reaction. Nat. Commun. 2016, 7, 10672.
Zhang, Q. Q.; Bai, H.; Zhang, Q.; Ma, Q.; Li, Y. H.; Wan, C. Q.; Xi, G. C. MoS2 yolk-shell microspheres with a hierarchical porous structure for efficient hydrogen evolution. Nano Res. 2016, 9, 3038-3047.
Hinnemann, B.; Moses, P. G.; Bonde, J.; Jørgensen, K. P.; Nielsen, J. H.; Horch, S.; Chorkendorff, I.; Nørskov, J. K. Biomimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution. J. Am. Chem. Soc. 2005, 127, 5308-5309.
Jaramillo, T. F.; Jørgensen, K. P.; Bonde, J.; Nielsen, J. H.; Horch, S.; Chorkendorff, I. Identification of active edge sites for electrochemical H2 evolution from MoS2 nanocatalysts. Science 2007, 317, 100-102.
Hansen, L. P.; Ramasse, Q. M.; Kisielowski, C.; Brorson, M.; Johnson, E.; Topsøe, H.; Helveg, S. Atomic-scale edge structures on industrial-style MoS2 nanocatalysts. Angew. Chem., Int. Ed. 2011, 50, 10153-10156.
Acerce, M.; Voiry, D.; Chhowalla, M. Metallic 1T phase MoS2 nanosheets as supercapacitor electrode materials. Nat. Nanotechnol. 2015, 10, 313-318.
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.
Kong, D. S.; Wang, H. T.; Cha, J. J.; Pasta, M.; Koski, K. J.; Yao, J.; Cui, Y. Synthesis of MoS2 and MoSe2 films with vertically aligned layers. Nano Lett. 2013, 13, 1341-1347.
Wang, H. T.; Kong, D. S.; Johanes, P.; Cha, J. J.; Zheng, G. Y.; Yan, K.; Liu, N.; Cui, Y. MoSe2 and WSe2 nanofilms with vertically aligned molecular layers on curved and rough surfaces. Nano Lett. 2013, 13, 3426-3433.
Cheng, L.; Huang, W. J.; Gong, Q. F.; Liu, C. H.; Liu, Z.; Li, Y. G.; Dai, H. J. Ultrathin WS2 nanoflakes as a high-performance electrocatalyst for the hydrogen evolution reaction. Angew. Chem., Int. Ed. 2014, 53, 7860-7863.
Gong, Q. F.; Cheng, L.; Liu, C. H.; Zhang, M.; Feng, Q. L.; Ye, H. L.; Zeng, M.; Xie, L. M.; Liu, Z.; Li, Y. G. Ultrathin MoS2(1-x)Se2x alloy nanoflakes for electrocatalytic hydrogen evolution reaction. ACS Catal. 2015, 5, 2213-2219.
Li, H.; Tsai, C.; Koh, A. L.; Cai, L. L.; Contryman, A. W.; Fragapane, A. H.; Zhao, J. H.; Han, H. S.; Manoharan, H. C.; Abild-Pedersen, F. et al. Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies. Nat. Mater. 2016, 15, 48-53.
Yin, Y.; Han, J. C.; Zhang, Y. M.; Zhang, X. H.; Xu, P.; Yuan, Q.; Samad, L.; Wang, X. J.; Wang, Y.; Zhang, Z. H. et al. Contributions of phase, sulfur vacancies, and edges to the hydrogen evolution reaction catalytic activity of porous molybdenum disulfide nanosheets. J. Am. Chem. Soc. 2016, 138, 7965-7972.
Liu, D. B.; Xu, W. Y.; Liu, Q.; He, Q.; Haleem, Y. A.; Wang, C. D.; Xiang, T.; Zou, C. W.; Chu, W. S.; Zhong, J. et al. Unsaturated-sulfur-rich MoS2 nanosheets decorated on free-standing SWNT film: Synthesis, characterization and electrocatalytic application. Nano Res. 2016, 9, 2079-2087.
Kiriya, D.; Lobaccaro, P.; Nyein, H. Y. Y.; Taheri, P.; Hettick, M.; Shiraki, H.; Sutter-Fella, C. M.; Zhao, P. D.; Gao, W.; Maboudian, R. et al. General thermal texturization process of MoS2 for efficient electrocatalytic hydrogen evolution reaction. Nano Lett. 2016, 16, 4047-4053.
Voiry, D.; Fullon, R.; Yang, J.; de Carvalho Castro E Silva, C.; Kappera, R.; Bozkurt, I.; Kaplan, D.; Lagos, M. J.; Batson, P. E.; Gupta, G. et al. The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen. Nat. Mater. 2016, 15, 1003-1009.
Yang, L. J.; Zhou, W. J.; Lu, J.; Hou, D. M.; Ke, Y. T.; Li, G. Q.; Tang, Z. H.; Kang, X. W.; Chen, S. W. Hierarchical spheres constructed by defect-rich MoS2/carbon nanosheets for efficient electrocatalytic hydrogen evolution. Nano Energy 2016, 22, 490-498.
Xie, J. F.; Zhang, H.; Li, S.; Wang, R. X.; Sun, X.; Zhou, M.; Zhou, J. F.; Lou, X. W.; Xie, Y. Defect-rich MoS2 ultrathin nanosheets with additional active edge sites for enhanced electrocatalytic hydrogen evolution. Adv. Mater. 2013, 25, 5807-5813.
Vrubel, H.; Merki, D.; Hu, X. L. Hydrogen evolution catalyzed by MoS3 and MoS2 particles. Energy Environ. Sci. 2012, 5, 6136-6144.
Benck, J. D.; Chen, Z. B.; Kuritzky, L. Y.; Forman, A. J.; Jaramillo, T. F. Amorphous molybdenum sulfide catalysts for electrochemical hydrogen production: Insights into the origin of their catalytic activity. ACS Catal. 2012, 2, 1916-1923.
Morales-Guio, C. G.; Hu, X. L. Amorphous molybdenum sulfides as hydrogen evolution catalysts. Accounts Chem. Res. 2014, 47, 2671-2681.
Ting, L. R. L.; Deng, Y. L.; Ma, L.; Zhang, Y. J.; Peterson, A. A.; Yeo, B. S. Catalytic activities of sulfur atoms in amorphous molybdenum sulfide for the electrochemical hydrogen evolution reaction. ACS Catal. 2016, 6, 861-867.
Lee, S. C.; Benck, J. D.; Tsai, C.; Park, J.; Koh, A. L.; Abild-Pedersen, F.; Jaramillo, T. F.; Sinclair, R. Chemical and phase evolution of amorphous molybdenum sulfide catalysts for electrochemical hydrogen production. ACS Nano 2016, 10, 624-632.
Kibsgaard, J.; Jaramillo, T. F.; Besenbacher, F. Building an appropriate active-site motif into a hydrogen-evolution catalyst with thiomolybdate[Mo3S13]2- clusters. Nat. Chem. 2014, 6, 248-253.
Ren, X. P.; Pang, L. Q.; Zhang, Y. X.; Ren, X. D.; Fan, H. B.; Liu, S. Z. One-step hydrothermal synthesis of monolayer MoS2 quantum dots for highly efficient electrocatalytic hydrogen evolution. J. Mater. Chem. A 2015, 3, 10693-10697.
Gopalakrishnan, D.; Damien, D.; Shaijumon, M. M. MoS2 quantum dot-interspersed exfoliated MoS2 nanosheets. ACS Nano 2014, 8, 5297-5303.
Qiao, W.; Yan, S. M.; Song, X. Y.; Zhang, X.; Sun, Y.; Chen, X.; Zhong, W.; Du, Y. W. Monolayer MoS2 quantum dots as catalysts for efficient hydrogen evolution. RSC Adv. 2015, 5, 97696-97701.
Xu, S. J.; Li, D.; Wu, P. Y. One-pot, facile, and versatile synthesis of monolayer MoS2/WS2 quantum dots as bioimaging probes and efficient electrocatalysts for hydrogen evolution reaction. Adv. Funct. Mater. 2015, 25, 1127-1136.
Li, Y. G.; Wang, H. L.; Xie, L. M.; Liang, Y. Y.; Hong, G. S.; Dai, H. J. MoS2 nanoparticles grown on graphene: An advanced catalyst for the hydrogen evolution reaction. J. Am. Chem. Soc. 2011, 133, 7296-7299.
Tang, Y. J.; Wang, Y.; Wang, X. L.; Li, S. L.; Huang, W.; Dong, L. Z.; Liu, C. H.; Li, Y. F.; Lan, Y. Q. Molybdenum disulfide/nitrogen-doped reduced graphene oxide nanocomposite with enlarged interlayer spacing for electrocatalytic hydrogen evolution. Adv. Energy Mater. 2016, 6, 1600116.
Chen, Z. B.; Cummins, D.; Reinecke, B. N.; Clark, E.; Sunkara, M. K.; Jaramillo, T. F. Core-shell MoO3-MoS2 nanowires for hydrogen evolution: A functional design for electrocatalytic materials. Nano Lett. 2011, 11, 4168-4175.
Li, D. J.; Maiti, U. N.; Lim, J.; Choi, D. S.; Lee, W. J.; Oh, Y.; Lee, G. Y.; Kim, S. O. Molybdenum sulfide/n-doped CNT forest hybrid catalysts for high-performance hydrogen evolution reaction. Nano Lett. 2014, 14, 1228-1233.
Lukowski, M. A.; Daniel, A. S.; Meng, F.; Forticaux, A.; Li, L. S.; Jin, S. Enhanced hydrogen evolution catalysis from chemically exfoliated metallic MoS2 nanosheets. J. Am. Chem. Soc. 2013, 135, 10274-10277.
Voiry, D.; Yamaguchi, H.; Li, J. W.; Silva, R.; Alves, D. C. B.; Fujita, T.; Chen, M. W.; Asefa, T.; Shenoy, V. B.; Eda, G. et al. Enhanced catalytic activity in strained chemically exfoliated WS2 nanosheets for hydrogen evolution. Nat. Mater. 2013, 12, 850-855.
Wang, H. T.; Lu, Z. Y.; Xu, S. C.; Kong, D. S.; Cha, J. J.; Zheng, G. Y.; Hsu, P. C.; Yan, K.; Bradshaw, D.; Prinz, F. B. et al. Electrochemical tuning of vertically aligned MoS2 nanofilms and its application in improving hydrogen evolution reaction. Proc. Natl. Acad. Sci. U.S.A. 2013, 110, 19701-19706.
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.
Wang, H. T.; Lu, Z. Y.; Kong, D. S.; Sun, J.; Hymel, T. M.; Cui, Y. Electrochemical tuning of MoS2 nanoparticles on three-dimensional substrate for efficient hydrogen evolution. ACS Nano 2014, 8, 4940-4947.
Ding, J. B.; Zhou, Y.; Li, Y. G.; Guo, S. J.; Huang, X. Q. MoS2 nanosheet assembling superstructure with a three-dimensional ion accessible site: A new class of bifunctional materials for batteries and electrocatalysis. Chem. Mater. 2016, 28, 2074-2080.
Merki, D.; Vrubel, H.; Rovelli, L.; Fierro, S.; Hu, X. L. Fe, Co, and Ni ions promote the catalytic activity of amorphous molybdenum sulfide films for hydrogen evolution. Chem. Sci. 2012, 3, 2515-2525.
Sun, X.; Dai, J.; Guo, Y. Q.; Wu, C. Z.; Hu, F. T.; Zhao, J. Y.; Zeng, X. C.; Xie, Y. Semimetallic molybdenum disulfide ultrathin nanosheets as an efficient electrocatalyst for hydrogen evolution. Nanoscale 2014, 6, 8359-8367.
Kagan, C. R.; Lifshitz, E.; Sargent, E. H.; Talapin, D. V. Building devices from colloidal quantum dots. Science 2016, 353, 885.
Mak, K. F.; Lee, C.; Hone, J.; Shan, J.; Heinz, T. F. Atomically thin MoS2: A new direct-gap semiconductor. Phys. Rev. Lett. 2010, 105, 136805.
Zeng, H. B.; Du, X. W.; Singh, S. C.; Kulinich, S. A.; Yang, S. K.; He, J. P.; Cai, W. P. Nanomaterials via laser ablation/ irradiation in liquid: A review. Adv. Funct. Mater. 2012, 22, 1333-1353.
Liu, P.; Liang, Y.; Lin, X. Z.; Wang, C. X.; Yang, G. W. A general strategy to fabricate simple polyoxometalate nanostructures: Electrochemistry-assisted laser ablation in liquid. ACS Nano 2011, 5, 4748-4755.
Wang, H. Q.; Koshizaki, N.; Li, L.; Jia, L. C.; Kawaguchi, K.; Li, X. Y.; Pyatenko, A.; Swiatkowska-Warkocka, Z.; Bando, Y.; Golberg, D. Size-tailored ZnO submicrometer spheres: Bottom-up construction, size-related optical extinction, and selective aniline trapping. Adv. Mater. 2011, 23, 1865-1870.
Petersen, S.; Barcikowski, S. In situ bioconjugation: Single step approach to tailored nanoparticle-bioconjugates by ultrashort pulsed laser ablation. Adv. Funct. Mater. 2009, 19, 1167-1172.
Zeng, H. B.; Yang, S. K.; Cai, W. P. Reshaping formation and luminescence evolution of ZnO quantum dots by laser-induced fragmentation in liquid. J. Phys. Chem. C 2011, 115, 5038-5043.
Gopalakrishnan, D.; Damien, D.; Li, B.; Gullappalli, H.; Pillai, V. K.; Ajayan, P. M.; Shaijumon, M. M. Electrochemical synthesis of luminescent MoS2 quantum dots. Chem. Commun. 2015, 51, 6293-6296.
Lv, X. J.; She, G. W.; Zhou, S. X.; Li, Y. M. Highly efficient electrocatalytic hydrogen production by nickel promoted molybdenum sulfide microspheres catalysts. RSC Adv. 2013, 3, 21231.
Xie, J. F.; Zhang, J. J.; Li, S.; Grote, F.; Zhang, X. D.; Zhang, H.; Wang, R. X.; Lei, Y.; Pan, B. C.; Xie, Y. Controllable disorder engineering in oxygen-incorporated MoS2 ultrathin nanosheets for efficient hydrogen evolution. J. Am. Chem. Soc. 2013, 135, 17881-17888.
Cummins, D. R.; Martinez, U.; Sherehiy, A.; Kappera, R.; Martinez-Garcia, A.; Schulze, R. K.; Jasinski, J.; Zhang, J.; Gupta, R. K.; Lou, J. et al. Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction. Nat. Commun. 2016, 7, 11857.
