Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt-Like Electrocatalytic Activity

Hui Chen; Xuan Ai; Wang Liu; Zhoubing Xie; Weiqiang Feng; Wei Chen; Xiaoxin Zou

doi:10.1002/anie.201906394

Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt-Like Electrocatalytic Activity

Angew Chem Int Ed Engl. 2019 Aug 12;58(33):11409-11413. doi: 10.1002/anie.201906394. Epub 2019 Jul 3.

Authors

Hui Chen¹, Xuan Ai¹, Wang Liu¹, Zhoubing Xie¹, Weiqiang Feng², Wei Chen³, Xiaoxin Zou¹

Affiliations

¹ State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, China.
² College of Materials Science and Engineering, Jilin University, Changchun, 130012, China.
³ Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, Jilin University, Changchun, 130023, China.

PMID: 31187910
DOI: 10.1002/anie.201906394

Abstract

The fundamental understanding and rational manipulation of catalytic site preference at extended solid surfaces is crucial in the search for advanced catalysts. Herein we find that the Ru top sites at metallic ruthenium surface have efficient Pt-like activity for the hydrogen evolution reaction (HER), but they are subordinate to their adjacent, less active Ru₃ -hollow sites due to the stronger hydrogen-binding ability of the latter. We also present an interstitial incorporation strategy for the promotion of the Ru top sites from subordinate to dominant character, while maintaining Pt-like catalytic activity. Our combined theoretical and experimental studies further identify intermetallic RuSi as a highly active, non-Pt material for catalyzing the HER, because of its suitable electronic structure governed by a good balance of ligand and strain effects.

Keywords: electrocatalysis; electronic structure; hydrogen evolution reaction; site preference.

Abstract

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