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首页> 外文期刊>ACS applied materials & interfaces >Tuning the Product Selectivity of the Cu Hollow Fiber Gas Diffusion Electrode for Efficient CO2 Reduction to Formate by Controlled Surface Sn Electrodeposition
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Tuning the Product Selectivity of the Cu Hollow Fiber Gas Diffusion Electrode for Efficient CO2 Reduction to Formate by Controlled Surface Sn Electrodeposition

机译：调整Cu中空纤维气体扩散电极的产品选择性，以通过受控表面Sn电沉积进行高效的CO2减少培养

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摘要

The efficient CO2 electrochemical reduction reaction (CO2RR) relies not only on the development of selective/active catalysts but also on the advanced electrode configuration to solve the critical issue of poor CO2 mass transport and derived sluggish cathodic reaction kinetics. In this work, to achieve a favorable reaction rate and product selectivity, we designed and synthesized an asymmetric porous Cu hollow fiber gas diffusion electrode (HFGDE) with controlled Sn surface electrodeposition. The HFGDE derived from the optimal Sn electrodeposition condition exhibited a formate Faradaic efficiency (FE) of 78% and a current density of 88 mA cm(-2) at -1.2 V versus reversible hydrogen electrode, which are more than 2 times higher than those from the pristine Cu HFGDE. The achieved performance outperformed most of the other Sn-based GDEs, indicating the creation of sufficient contact among CO2, electrolyte, and electrode catalyst through the design of the hollow fiber pore structure and catalytic active sites. The enhancement of formate production selectivity and the suppression of the hydrogen by-product were attributed to the optimized ratio of SnOx species on the electrode surface. The best performance was seen in the HFGDE with the highest Sn2+/Sn4+ (120 s deposition), likely due to the modulating effect of the Cu substrate via electron donation with Sn species. The selectivity control strategy developed in the asymmetric HFGDE provides an efficient and facile method to stimulate selective electrochemical reactions in which the gas-phase reactant with low solubility is involved.
机译：高效的CO 2电化学还原反应（CO2RR）不仅依赖于选择性/活性催化剂的开发，而且还依赖于先进的电极配置，以解决差的CO2质量运输和衍生缓慢的阴极反应动力学的临界问题。在这项工作中，为了实现有利的反应速率和产品选择性，我们设计并合成了具有受控Sn表面电沉积的不对称多孔Cu中空纤维气体扩散电极（HFGDE）。来自最佳Sn电沉积病症的HFGDE表现出78％的甲酸含量（Fe），电流密度为-1.2V与可逆氢电极，比那些高出2倍以上来自原始Cu HFGDE。实现的性能优于大多数其他基于SN的GDES，表明通过设计中空纤维孔结构和催化活性位点，在CO 2，电解质和电极催化剂中产生足够的接触。甲酸盐产生选择性的增强和氢副产物的抑制归因于电极表面上的SNOX种类的优化比。在HFGDE中可以看到最佳性能，具有最高的SN2 + / SN4 +（120s沉积），可能是由于Cu基质通过用Sn种类的电子捐赠调节效果。在不对称HFGDE中开发的选择性控制策略提供了一种有效且容易的方法，以刺激选择性电化学反应，其中涉及低溶解度的气相反应物。

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