具有OH -斥力的电极调节CO吸附，增强C-C耦合

IF 9.1 Q1 ENGINEERING, CHEMICAL Green Chemical Engineering Pub Date : 2023-09-01 DOI:10.1016/j.gce.2022.07.007

Qixing Zhang , Dan Ren , Jing Gao , Zhongke Wang , Juan Wang , Sanjiang Pan , Manjing Wang , Jingshan Luo , Ying Zhao , Michael Grätzel , Xiaodan Zhang

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摘要

由可再生电力驱动的电化学CO2减排是将可持续能源作为燃料储存的有前景的策略之一。然而，对于该工艺的进一步应用，增值多碳产品的选择性仍然很差。在这里，我们通过在铜（Cu）电极上形成对OH−具有排斥性的Nafion层来调节CO吸附，有助于增强CO2还原为C2+产物的选择性，同时抑制C1产物。操作拉曼光谱表明，局部OH−会吸附在部分活性位点上，降低对CO的吸附。因此，对OH−具有排斥性的电极可以调节OH−的浓度，从而增加对CO的吸收，增强C–C耦合。这项工作表明，电极设计可能是提高CO2还原为多碳产物的选择性的有效策略。

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Regulated CO adsorption by the electrode with OH− repulsive property for enhancing C–C coupling

Electrochemical CO₂ reduction driven by renewable electricity is one of the promising strategies to store sustainable energy as fuels. However, the selectivity of value-added multi-carbon products remains poor for further application of this process. Here, we regulate CO adsorption by forming a Nafion layer on the copper (Cu) electrode that is repulsive to OH⁻, contributing to enhanced selectivity of CO₂ reduction to C₂₊ products with the suppression of C₁ products. The operando Raman spectroscopy indicates that the local OH⁻ would adsorb on part of active sites and decrease the adsorption of CO. Therefore, the electrode with repulsive to OH⁻ can adjust the concentration of OH⁻, leading to the increased adsorption of CO and enhanced C–C coupling. This work shows that electrode design could be an effective strategy for improving the selectivity of CO₂ reduction to multi-carbon products.