期刊
ACS NANO
卷 17, 期 2, 页码 1287-1297出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c09423
关键词
Active edge sites; basal plane; heteroatom doping; on-chip electrochemistry; hydrogen evolution reaction
Composition modulation and edge enrichment can enhance the catalytic activity of two-dimensional materials. Phosphorus-doped MoS2 nanosheets exhibit higher hydrogen evolution reaction (HER) activity at the edges than the basal plane. This discovery provides insights for designing edge-dominant 2D catalysts.
Composition modulation and edge enrichment are established protocols to steer the electronic structures and catalytic activities of twodimensional (2D) materials. It is believed that a heteroatom enhances the catalytic performance by activating the chemically inert basal plane of 2D crystals. However, the edge and basal plane have inherently different electronic states, and how the dopants affect the edge activity remains ambiguous. Here we provide mechanistic insights into this issue by monitoring the hydrogen evolution reaction (HER) performance of phosphorus-doped MoS2 (P-MoS2) nanosheets via on-chip electrocatalytic microdevices. Upon phosphorus doping, MoS2 nanosheet gets catalytically activated and, more importantly, shows higher HER activity in the edge than the basal plane. In situ transport measurement demonstrates that the improved HER performance of P-MoS2 is derived from intrinsic catalytic activity rather than charge transfer. Density functional theory calculations manifest that the edge sites of PMoS2 are energetically more favorable for HER. The finding guides the rational design of edge-dominant P-MoS2, reaching a minuscule onset potential of similar to 30 mV and Tafel slope of 48 mV/dec that are benchmarked against other activation methods. Our results disclose the hitherto overlooked edge activity of 2D materials induced by heteroatom doping that will provide perspectives for preparing next-generation 2D catalysts.
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