Composition-Tuned Surface Binding on CuZn-Ni Catalysts Boosts CO2RR Selectivity toward CO Generation
journal contributionposted on 10.02.2022, 18:44 authored by Jinxi Chen, Xiaofei Wei, Rongming Cai, Jiazheng Ren, Min Ju, Xiaoqing Lu, Xia Long, Shihe Yang
The Cu/Zn ratio of the CuZn electrocatalyst is known to influence the selectivity of CO2RR, but questions remain open about how microstructure, crystal phase, and oxidation state of the metal ions change and interplay in the composition tuning process, which need to be carefully addressed for rational catalyst design. Toward this end, we designed and synthesized a series of CuZn-based aerogel materials with controlled Cu/Zn ratios and systematically investigated their effects on CO2RR catalysis. From both experimental results and theoretical calculations, we found that the introduction of Zn into Cu aerogel greatly promoted the production of CO primarily due to the unfavorable adsorption energy of *H. Surprisingly, the intake of trace Ni atoms further inhibited the H2 evolution reaction on account of the strong pinning of both *H and H2O* on the Ni sites. Therefore, the as-formed CuZn-Ni aerogel exhibited a much-improved catalytic activity and selectivity for CO generation with FE(CO) increased to 80% from 60%. This work gives insights into the surface adsorption–desorption characteristics underlying the activity and selectivity of electrocatalysts, which is of general importance for CO2RR.
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work gives insightsunfavorable adsorption energytuned surface bindingrational catalyst designquestions remain openmetal ions changebased aerogel materialstrace ni atomsni aerogel exhibitedfe ( coco primarily dueimproved catalytic activitycomposition tuning process2 </ subni sitesco generationtheoretical calculationssystematically investigatedstrong pinningoxidation stategeneral importanceexperimental resultsevolution reactioncrystal phasecarefully addressed60 %.