4.8 Article

Tuning Interfacial Active Sites over Porous Mo2N-Supported Cobalt Sulfides for Efficient Hydrogen Evolution Reactions in Acid and Alkaline Electrolytes

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 35, Pages 41573-41583

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c10060

Keywords

electrocatalyst; hydrogen evolution reaction; cobalt sulfide; molybdenum nitride; water splitting

Funding

  1. National Natural Science Foundation of China [22072183]
  2. Changsha Municipal Natural Science Foundation [kq2014119]
  3. Opening Project of Guangdong Provincial Key Laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing, South China University of Technology, China [2020kfkt02]

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A heterojunction of cobalt sulfide and Mo2N is designed for efficient hydrogen evolution reactions in both acid and alkaline electrolytes. The Mo-S bonds formed at the interface result in considerably enhanced hydrogen evolution reaction activity. This study provides a feasible strategy for designing hetero-based electrocatalysts with a tuned highly active interface.
Although various cobalt-sulfide-based materials have been reported for the hydrogen evolution reaction, only a few have achieved high activity in both acid and alkaline electrolytes due to the inherent poor conductivity and low active sites. In this work, a heterojunction of cobalt sulfide and Mo2N is designed for efficient hydrogen evolution reactions in both acid and alkaline electrolytes. X-ray photoelectron spectroscopy reveals that Mo-S bonds are formed at the interface between Mo2N and CoS2, which result in the fabricated Mo2N/CoS2 materials exhibiting a considerably enhanced hydrogen evolution reaction activity than the corresponding Mo2N, CoS2, and most reported Mo- and Co-based catalysts in electrolytes of H2SO4 and KOH solutions. Density functional theory calculations suggest that the redistribution of charges occurs at the heterointerface. In addition, the interfacial active sites possess a considerably lower hydrogen adsorption Gibbs free energy than those atoms that are far away from the interface, which is beneficial to the process of hydrogen evolution reaction. This study provides a feasible strategy for designing hetero-based electrocatalysts with a tuned highly active interface.

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