Promoting the Volmer Step of Alkaline Hydrogen Oxidation Reaction by Incorporating Zn Single Atoms into Ru Lattice and Carbon Frameworks

Abstract The Volmer step is considered to play a critical role in the alkaline hydrogen oxidation reaction (HOR) process. However, current research mainly focuses on optimizing the adsorption strength of H ads and OH ads , while the importance of maximizing the adsorption interfaces with different adsorbates is rarely addressed. Herein, a multi‐strategy approach is explored by simultaneously incorporating Zn single atoms into Ru lattice and carbon support (denoted as (Zn 1 Ru) SAA /Zn 1 ‐N‐C) to construct a high activity and stable alkaline HOR catalyst. This novel catalyst achieves an impressive mass activity of up to 4.98 mA µg Ru −1 at 50 mV, which surpasses that of Ru/N‐C by 1.9 times and even surpasses that of Pt/C by 7.5 times. In addition, the novel catalyst has superior long‐term stability and CO resistance. Experimental results and theoretical calculations reveal that the unique structure of Zn 1 Ru) SAA /Zn 1 ‐N‐C not only enhances the catalyst (Ru nanoparticles)‐support interaction, it facilitates the electron transfer between catalyst and support, and further optimizes the adsorption behavior of various intermediates, but also forms distinct micro‐regions of adsorbed H (*H) and adsorbed OH (*OH) on the Ru nanoparticle surface, thereby promoting the Volmer process. The research provides a new understanding of the complex design of advanced alkaline HOR catalysts.