期刊
ACS NANO
卷 13, 期 6, 页码 6824-6834出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b01583
关键词
hydrogen evolution reaction; MoS2; sulfur vacancies; undercoordinated Mo; H-2-annealing
类别
资金
- US Army RDECOM [W911NF-17-2-0033]
- CNRS Cellule Energie exploratory Project: R2D-CO2
- European Research Council (ERC) under the European Union [804320]
- National Natural Science Foundation of China [21503092]
- Zhejiang Provincial Natural Science Foundation of China [LY19B030005]
- Graduate School Ecole doctorale des Sciences Chimiques [ED 459]
- European Research Council (ERC) [804320] Funding Source: European Research Council (ERC)
Low-dimensional materials have been examined as electrocatalysts for the hydrogen evolution reaction (HER). Among them, two-dimensional transition metal dichalcogenides (2D-TMDs) such as MoS2 have been identified as potential candidates. However, the performance of TMDs toward HER in both acidic and basic media remains inferior to that of noble metals such as Pt and its alloys. This calls for investigating the influence of controlled defect engineering of 2D TMDs on their performance toward hydrogen production. Here, we explored the HER activity from defective multilayered MoS2 over a large range of surface S vacancy concentrations up to 90%. Amorphous MoS2 and 2H MoS2 with ultrarich S vacancies demonstrated the highest HER performance in acid and basic electrolytes, respectively. We also report that the HER performance from multilayered MoS2 can be divided into two domains corresponding to point defects at low concentrations of surface S vacancies (Stage 1) and large regions of undercoordinated Mo atoms for high concentrations of surface S vacancies (Stage 2). The highest performance is obtained for Stage 2 in the presence of undercoordinated Mo atoms with a TOF of similar to 2 s(-1) at an overpotential of 160 mV in 0.1 M KOH which compares favorably to the best results in the literature. Overall, our work provides deeper insight on the HER mechanism from defected MoS2 and provides guidance for the development of defect-engineered TMD-based electrocatalysts.
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