期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 12, 页码 14315-14324出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c01091
关键词
WTe2; electrocatalytic microdevice; hydrogen evolution reaction; charge effect; steric hindrance
资金
- National Natural Science Foundation of China [22071069, 21805102, 21825103]
- Hubei Provincial Natural Science Foundation of China [2019CFA002]
- Foundation of Basic and Applied Basic Research of Guangdong Province [2019B1515120087]
- Fundamental Research Funds for the Central University [2019kfyXMBZ018]
- Analytical and Testing Center in Huazhong University of Science and Technology
The high electrical conductivity of 1T'-WTe2 shows potential for hydrogen evolution reaction (HER) catalysis, but actual activity does not align with expectations. By doping electronegative F atoms onto WTe2 sheets, researchers were able to enhance HER activity and improve hydrogen adsorption behavior, providing a new pathway for constructing electrocatalysts efficiently.
The high electrical conductivity of 1T'-WTe2 deserves particular attention and may show a high potential for hydrogen evolution reaction (HER) catalysis. However, the actual activity certainly does not match expectations, and the inferior HER activity is actually still ambiguous at the atomic level. Unraveling the underlying HER behaviors of 1T'-WTe2 will give rise to a new family of HER catalysts. Our structural analysis reveals that the inferior activity could result from insufficient charge density around the Te site and blocked adsorption channel at the W site, which cause too weak hydrogen adsorption. Herein, we fabricated a single WTe2 sheet-based electrocatalytic microdevice for directly extracting enhanced HER activity of doped electronegative F atoms. The overpotential at -10 mA cm(-2) reduced to 0.27 V after F doping compared to 0.45 V for the original state. In situ electrochemical measurement and electrical tests on a single sheet indicate that doped F can regulate surface charge and hydrogen adsorption behavior. Furthermore, the theory simulation uncovers that the smaller atomic radius of F contributes to an empty coordination environment; meanwhile, strong electronegativity induces hydrogen adsorption. Thus, the Delta G(H)* at W sites around the doped F is as low as 0.18 eV. Synergistically modulating the charge properties and opening steric hindrance provides a new pathway to rationally construct electrocatalysts and beyond.
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