Tandem effect of Ag@C@Cu catalysts enhances ethanol selectivity for electrochemical CO2 reduction in flow reactors

作者：Jie Zhang, Thi Ha My Pham, Youngdon Ko, Mo Li, Shuliang Yang, Cedric David Koolen, Liping Zhong, Wen Luo, Andreas Züttel · 发表于：Cell Reports Physical Science · 年份：2022 · DOI：10.1016/j.xcrp.2022.100949 · 被引用次数：74 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Electrocatalysts for Energy Conversion

CO-selective metals (e.g., Ag) on Cu catalysts improve the selectivity of multi-carbon (C2+) products in electrochemical CO2 reduction. However, the origin of the improvement remains unclear due to the convolution of tandem and interface effects. Here, Ag@C@Cu core-shell catalysts were synthesized, in which the thin carbon interlayer inhibited the direct interaction between Ag and Cu while still allowing the reduction of CO2 on Ag, thus isolating the tandem effect from other effects. This catalyst produced higher ratios of ethanol to ethylene relative to the monometallic Cu catalyst, demonstrating that the locally increased CO concentration promoted the ethanol pathway over the ethylene pathway. Further, the selectivity of ethanol was optimized by tuning the thickness of the Cu shell. This work provides a rational approach to design core-shell catalysts for understanding structure-performance relationships and demonstrates the key role of the tandem effect in tuning the selectivity of C2+ products.