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In Situ Engineering of the Cu+/Cu0 Interface to Boost C2+ Selectivity in CO2 Electroreduction
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-08-04 , DOI: 10.1021/acsami.2c05992 Ruian Du 1 , Tan Li 1 , Qiqi Wu 1 , Peng Wang 1 , Xianfeng Yang 2 , Yan Fan 2 , Yongcai Qiu 1 , Keyou Yan 1 , Pei Wang 3 , Yun Zhao 1 , Wei-Wei Zhao 4 , Guangxu Chen 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-08-04 , DOI: 10.1021/acsami.2c05992 Ruian Du 1 , Tan Li 1 , Qiqi Wu 1 , Peng Wang 1 , Xianfeng Yang 2 , Yan Fan 2 , Yongcai Qiu 1 , Keyou Yan 1 , Pei Wang 3 , Yun Zhao 1 , Wei-Wei Zhao 4 , Guangxu Chen 1
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The Cu+/Cu0 interface in the Cu-based electrocatalyst is essential to promote the electrochemical reduction of carbon dioxide (ERCO2) to produce multi-carbon hydrocarbons and alcohols with high selectivity. However, due to the high activity of the Cu+/Cu0 interface, it is easy to be oxidized in the air. How to control and prepare a Cu-based electrocatalyst with an abundant and stable Cu+/Cu0 interface in situ is a huge challenge. Here, combined with density functional theory (DFT) calculations and experimental studies, we found that the trace halide ions adsorbed on Cu2O can slow the reduction kinetics of Cu+ → Cu0, which allowed us to in-situ well control the synthesis of the CuO-derived electrocatalyst with rich Cu+/Cu0 interfaces. Our Cu catalyst with a rich Cu+/Cu0 interface exhibits excellent ERCO2 performance. Under the operation potential of −0.98 V versus RHE, the Faraday efficiency of C2H4 and C2+ products are 55.8 and 75.7%, respectively, which is about 16% higher than that of CuO-derived electrocatalysts that do not use halide ions. The high 
comes from the improvement of the coupling efficiency of reaction intermediates such as CO–CO, which is proved by DFT calculations, and the suppression of hydrogen evolution reaction. Therefore, we provide an in-situ engineering strategy, which is simple and effective for the design and preparation of high-performance ERCO2 catalysts.
中文翻译：
Cu+/Cu0 界面的原位工程以提高 CO2 电还原中 C2+ 的选择性
Cu基电催化剂中的Cu + /Cu 0界面对于促进二氧化碳（ERCO 2）的电化学还原以产生高选择性的多碳烃和醇至关重要。但由于Cu + /Cu 0界面活性高，在空气中易被氧化。如何原位控制和制备具有丰富且稳定的Cu + /Cu 0界面的Cu基电催化剂是一个巨大的挑战。在这里，结合密度泛函理论（DFT）计算和实验研究，我们发现吸附在Cu 2 O上的痕量卤离子可以减缓Cu +的还原动力学。→ Cu 0，这使我们能够原位很好地控制具有丰富Cu + /Cu 0界面的CuO衍生的电催化剂的合成。我们的 Cu 催化剂具有丰富的 Cu + /Cu 0界面，表现出优异的 ERCO 2性能。在-0.98 V相对RHE的工作电位下，C 2 H 4和C 2+产物的法拉第效率分别为55.8%和75.7%，比不使用卤化物的CuO衍生电催化剂的法拉第效率高约16%离子。高来自于 CO-CO 等反应中间体的耦合效率的提高，通过 DFT 计算证明，以及对析氢反应的抑制。因此，我们提供了一种原位工程策略，该策略对于高性能ERCO 2催化剂的设计和制备简单有效。
更新日期：2022-08-04
comes from the improvement of the coupling efficiency of reaction intermediates such as CO–CO, which is proved by DFT calculations, and the suppression of hydrogen evolution reaction. Therefore, we provide an in-situ engineering strategy, which is simple and effective for the design and preparation of high-performance ERCO2 catalysts.
中文翻译：
Cu+/Cu0 界面的原位工程以提高 CO2 电还原中 C2+ 的选择性
Cu基电催化剂中的Cu + /Cu 0界面对于促进二氧化碳（ERCO 2）的电化学还原以产生高选择性的多碳烃和醇至关重要。但由于Cu + /Cu 0界面活性高，在空气中易被氧化。如何原位控制和制备具有丰富且稳定的Cu + /Cu 0界面的Cu基电催化剂是一个巨大的挑战。在这里，结合密度泛函理论（DFT）计算和实验研究，我们发现吸附在Cu 2 O上的痕量卤离子可以减缓Cu +的还原动力学。→ Cu 0，这使我们能够原位很好地控制具有丰富Cu + /Cu 0界面的CuO衍生的电催化剂的合成。我们的 Cu 催化剂具有丰富的 Cu + /Cu 0界面，表现出优异的 ERCO 2性能。在-0.98 V相对RHE的工作电位下，C 2 H 4和C 2+产物的法拉第效率分别为55.8%和75.7%，比不使用卤化物的CuO衍生电催化剂的法拉第效率高约16%离子。高
来自于 CO-CO 等反应中间体的耦合效率的提高，通过 DFT 计算证明，以及对析氢反应的抑制。因此，我们提供了一种原位工程策略，该策略对于高性能ERCO 2催化剂的设计和制备简单有效。
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