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Promotion of Electrocatalytic Hydrogen Evolution Reaction on Nitrogen-Doped Carbon Nanosheets with Secondary Heteroatoms

Konggang QuSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaYao ZhengSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaXianxi ZhangShandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252059, ChinaKenneth DaveySchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaSheng DaiSchool of Chemical Engineering and Advanced Materials, Newcastle University, Newcastle upon Tyne NE1 7RU, United KingdomShi‐Zhang QiaoSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia
2017en
ABI

Аннотация

Dual heteroatom-doped carbon materials are efficient electrocatalysts via a synergistic effect. With nitrogen as the primary dopant, boron, sulfur, and phosphorus can be used as secondary elements for co-doped carbons. However, evaluation and analysis of the promotional effect of B, P, and S to N-doped carbons has not been widely researched. Here we report a robust platform that is constructed through polydopamine to prepare N,B-, N,P-, and N,S-co-doped carbon nanosheets, characterized by similar N species content and efficient B, P, and S doping. Systematic investigation reveals S to have the greatest promotional effect in hydrogen evolution reactions (HER) followed by P and that B decreases the activity of N-doped carbons. Experimental and theoretical analyses show the secondary heteroatom promotional effect is impacted by the intrinsic structures and extrinsic surface areas of both materials, i.e., electronic structures exclusively determine the catalytic activity of active sites, while large surface areas optimize apparent HER performance.

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