期刊
ACS CATALYSIS
卷 7, 期 10, 页码 7312-7318出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b02885
关键词
vertical MoS2 nanosheets; carburization; Mo2C nanodomains; hybrid nanostructure; hydrogen evolution reaction; Mo-S-C motifs
资金
- Robert A. Welch Foundation [E-1728]
- National Science Foundation [2015M582538, ACI-1053575]
- 111 project [B13042]
- NSF-CBET [1605331]
- NSF CAREER award [1454384]
- NSF-MRI award [1531814]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- Direct For Computer & Info Scie & Enginr
- Office of Advanced Cyberinfrastructure (OAC) [1531814] Funding Source: National Science Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1454384, 1605331] Funding Source: National Science Foundation
Maximizing and creating active sites has been a general strategy to increase the performance of a catalyst. Because of the high electrocatalytic hydrogen evolution reactivity (HER) of ultrafine Mo2C nanocrystals and edges of two-dimensional MoS2, an electrode with a synergistic integration of these two nanomaterials is expected to show a better HER performance. Here we report this hybrid nanostructure of vertically aligned MoS2/Mo2C nanosheets on conductive carbon paper. It was revealed that the original structure of MoS2 nanosheets remains intact after the carburization, but the surfaces are incorporated with either Mo2C nanodomains or a heteroatomic mixture of S and C. The hybrid catalyst exhibits a much lower HER overpotential in comparison to those of the corresponding Mo2C and MoS2 alone. Its high activity is congruent with DFT calculations, which show that multiple S and C coordinated Mo sites with near zero Gibbs free energy of hydrogen adsorption exist. Thus, the low overpotential of this binder-free hybrid catalyst is a result of active sites of Mo-S-C and highly dispersed Mo2C nanodomains on the original edges and basal planes of MoS2. Our prediction and realization of active HER sites nanostructure opens up a route toward the development of more active HER catalysts. with this hybrid two-dimensional
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