Chengbo Ma, Jun Wang, Xiaomei Liu, Ning Li, Wen Liu, Yang Li, Xiaobin Fan and Wenchao Peng*,
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引用次数: 0
Abstract
In this study, zinc single-atom catalysts (SACs) (Zn SACs) with Zn–N2O2 as the coordination shell and the epoxy group (C–O–C) as the second coordination structure are synthesized. The obtained Zn SACs exhibit a high 2e– ORR selectivity of >85% in a wide potential window of 0–0.65 V vs RHE and achieve a high generation rate of 828.9 mmol gcat–1 h–1 for H2O2. Experimental and theoretical calculations have confirmed that the second coordination structure of adjacent C–O–C can effectively optimize the adsorption energy of Zn–N2O2 for *OOH and tune the 2e– ORR selectivity. In addition, a small onset potential of 0.38 V vs RHE is achieved for sulfides oxidation reaction (SOR) by the obtained Zn SACs. Moreover, a coupled system of anodic SOR and cathodic 2e– ORR is fabricated, which can save 45% energy consumption compared to the OER-2e– ORR system due to a decreased cell voltage of 2.03 V at 20 mA cm–2. This study provides new bifunctional Zn SACs modified by adjacent C–O–C, which are effective as bifunctional catalysts for electrosynthesis of H2O2 and electro-oxidation of sulfides. These two reactions can be performed together in a coupled system with decreased energy cost and thus should have better application potential.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.