First Author:Hu, Ze-Nan

Correspondence Author:Sun, Hong-bin Hu, Jianshe Liang, Qionglin Yang, Yang

Co author:Ai, Yongjian Xu, Wenjuan Zhang, Xinyue Sun, Zejun Guo, Liutao Guo, Rongxiu Wang, Yao Ding, Kelong

Journal:Small

Volume:18

DOI number:10.1002/smll.202200439

Affiliation of Author(s):Department of Chemistry, Northeastern University

Teaching and Research Group:物理化学

Place of Publication:GERMANY

Abstract:The intercrystalline interfaces have been proven vital in heterostructure cata-lysts. However, it is still challenging to generate specified heterointerfacesand to make clear the mechanism of a reaction on the interface. Herein, thiswork proposes a strategy of Fe-catalyzed cascade formation of heterointer-faces for comprehending the hydrogen evolution reaction (HER). In the puresolid-phase reaction system, Fe catalyzes the in situ conversion of MoO2 toMoC and then Mo2C, and the consecutive formation leaves lavish intercrys-talline interfaces of MoO2 -MoC (in Fe-MoO2/MoC@NC) or MoC-Mo2 C (inFe-MoC/β-Mo 2 C@NC), which contribute to HER activity. The improved HERactivity on the interface leads to further checking of the mechanism withdensity functional theory calculation. The computation results reveal that theelectroreduction (Volmer step) produced H* prefers to be adsorbed on Mo2C;then two pathways are proposed for the HER on the interface of MoC-Mo2C,including the single-molecular adsorption pathway (Rideal mechanism) andthe bimolecular adsorption pathway (Langmuir–Hinshelwood mechanism).The calculation results further show that the former is favorable, and thereaction on the MoC-Mo 2 C heterointerface significantly lowers the energybarriers of the rate-determining steps

Document Code:WOS:000776841100001

Discipline:Natural Science

First-Level Discipline:Chemistry

Page Number:2200439

ISSN No.:1613-6810

Translation or Not:no