Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes
Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes
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DOI：
10.1038/s41929-022-00751-0
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发表时间：
2022-03-03
期刊：
影响因子：
37.8
通讯作者：
Wu, Jingjie
中科院分区：
文献类型：
--
作者：
Zhang, Tianyu;Bui, Justin C.;Wu, Jingjie
电化学CO2还原为可持续生产有价值的化学品和燃料提供了一条有前途的途径。串联催化剂能够在互补活性位点上实现连续的CO2至CO和CO至多碳（C2+）产物转化，以产生高的C2+法拉第效率（FE）。不幸的是，以前的串联催化剂表现出对CO中间体的不良管理，这减少了C2+ FE。在这里，我们设计分段气体扩散电极（s-GDE），其中CO选择性催化剂层（CL）段在入口处的CO停留时间在随后的C2+选择性段，提高转化率。这种现象使得与纯铜相比，通过增加Cu CL内的 *CO覆盖率，Cu/Ag s-GDE的CO利用率和C2+电流密度都增加。最后，我们开发了一种Cu/Fe-N-Cs-GDE，其中90%的C2+ FE在C2+部分电流密度（j（c2+））超过1A cm（-2）。这些结果证明了运输的重要性，并建立了设计原则，以提高C2+ FE和J（C2+）串联CO2还原。
Electrochemical CO2 reduction provides a promising route to the sustainable generation of valuable chemicals and fuels. Tandem catalysts enable sequential CO2-to-CO and CO-to-multicarbon (C2+) product conversions on complementary active sites, to produce high C2+ Faradaic efficiency (FE). Unfortunately, previous tandem catalysts exhibit poor management of CO intermediates, which diminishes C2+ FE. Here, we design segmented gas-diffusion electrodes (s-GDEs) in which a CO-selective catalyst layer (CL) segment at the inlet prolongs CO residence time in the subsequent C2+-selective segment, enhancing conversion. This phenomenon enables increases in both the CO utilization and C2+ current density for a Cu/Ag s-GDE compared to pure Cu, by increasing the *CO coverage within the Cu CL. Lastly, we develop a Cu/Fe-N-C s-GDE with 90% C2+ FE at C2+ partial current density (j(c2+)) exceeding 1 A cm(-2). These results prove the importance of transport and establish design principles to improve C2+ FE and j(c2+) in tandem CO2 reduction.