期刊
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
卷 343, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.123534
关键词
Heterostructure; Interlayer spacing expansion; Molybdenum disulfide; Molybdenum dioxide; Hydrogen evolution reaction
This study reports a heterostructured material MoO2 @E-MoS2 containing expanded layer spacing and 1 T phase MoS2, which exhibits superior HER catalytic performance by modulating the electronic structure and improving the electrical conductivity and active site exposure of the catalyst.
The inferior hydrogen evolution reaction (HER) catalytic performance of MoS2 can be attributed to its small edge ratio, large inert substrate surface, and poor electrical conductivity, while the multiple strategies are expected to be employed simultaneously to modulate the electronic structure of MoS2 and yield catalysts with superior HER catalytic performance. Here, we report a MoS2 containing a 1 T phase with expanded layer spacing and construct it as a heterostructured material with MoO2 (MoO2 @E-MoS2). Specifically, the presence of the 1 T phase and expanded layer structure of MoS2 can enhance electrode conductivity, increase active site exposure, promote H2O adsorption, and optimize the Gibbs-free energy of hydrogen. The constructed heterostructure can modulate the electronic structure of the catalyst, enhance electron transfer at the interface, elevate water adsorption energy, and reduce the hydrogen reaction energy barrier. Moreover, density functional theory calculations indicate that the S site of MoS2 in this catalyst exhibits a higher affinity for H2O adsorption, while the Mo site demonstrates a greater capacity for H* adsorption/desorption. Ultimately, MoO2 @E-MoS2 shows low overpotentials of 93 and 99 mV at a current density of 10 mA cm-2, as well as exceptional long-term stabilities exceeding 70 and 130 h at current densities ranging from 10 to 30 mA cm-2 in acidic and alkaline media, respectively.
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