Lei Gong, Weining Zhang, Yan Zhuang, Kaiyue Zhang, Qiuyu Zhao, Dongdong Xiao, Shuo Liu, Zhiwei Liu, Yongzheng Zhang
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High-Entropy Metal Sulfide Promises High-Performance Carbon Dioxide Reduction.
The efficient conversion of carbon dioxide (CO2) requires the development of stable catalysts with high selectivity and reactivity within a wide potential range. Here, the high-entropy metal sulfide CuAgZnSnS4 is designed for CO2 reduction with excellent performance (FEcarbon products ≥ 90%) in whole test potential windows (600 mV) based on the synergistic effect of the high-entropy metal sulfide. In particular, CuAgZnSnS4 exhibits better single-product selectivity with the highest FEHCOOH/FECO value (29.03) at -1.28 versus reversible hydrogen electrode (RHE). In combination with in situ measurements and theoretical calculations, it is further revealed that the synergistic effect of CuAgZnSnS4 realizes the controllable regulation of the surface electronic structure at Sn active sites, strengthening orbital interactions between *OCHO and Sn active sites. As a result, the effective adsorption and activation of *OCHO instead of *H are obtained, improving the single-product selectivity of electrocatalytic CO2 reduction and inhibiting the competitive hydrogen evolution reaction significantly. Our findings may complete the understanding of the synergistic effect for high-entropy materials in catalysis and offer new insight into the design of efficient electrocatalysts with high catalytic activity.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.