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

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.

An electron-hole rich dual-site nickel catalyst for efficient photocatalytic overall water splitting

“…5 c, h and Supplementary Figs. 32 – 33 ) 51 . In addition, it is obvious that Ni atom of NiS owns more negative charge because a lot of electron transfer occurs from the Ni 2 P and PCOS region to the NiS (Fig.…”

Non-precious metal-based heterostructure catalysts for hydrogen evolution reaction: mechanisms, design principles, and future prospects

“…90 For composite catalysts, the electron transfer between components increases the electron density near the Fermi energy level, generating high conductivity, which further changes the ratio of antibonding states to bring ΔG (H*) closer to the ideal value, resulting in an appropriate adsorption energy and contributing to the HER activity. 91 These can be fully demonstrated in the study of Ni 2 P optimization. Zhang et al 92 3 Composite catalysts…”

“…90 For composite catalysts, the electron transfer between components increases the electron density near the Fermi energy level, generating high conductivity, which further changes the ratio of antibonding states to bring Δ G (H*) closer to the ideal value, resulting in an appropriate adsorption energy and contributing to the HER activity. 91 These can be fully demonstrated in the study of Ni 2 P optimization. Zhang et al 92 prepared MoO 2 /Ni 2 P catalysts by constructing heterostructures for Ni 2 P. MoO 2 affected the d-band electron arrangement of Ni 2 P, resulting in a decrease of the d-band center of Ni from −1.82 eV to −1.92 eV of Ni 2 P, which enhanced the desorption process of H*, resulting in better reaction kinetics and catalytic HER proceeding.…”