Wang Jiali, Tan Hui-Ying, Zhu Yanping, Chu Hang, Chen Hao Ming
Department of Chemistry, National (Taiwan) University, Taipei, 10617, Taiwan.
National Synchrotron Radiation Research Center, Hsinchu, 30076, Taiwan.
Angew Chem Int Ed Engl. 2021 Aug 2;60(32):17254-17267. doi: 10.1002/anie.202017181. Epub 2021 Apr 13.
The promoted activity and enhanced selectivity of electrocatalysts is commonly ascribed to specific structural features such as surface facets, morphology, and atomic defects. However, unraveling the factors that really govern the direct electrochemical reduction of CO (CO RR) is still very challenging since the surface state of electrocatalysts is dynamic and difficult to predict under working conditions. Moreover, theoretical predictions from the viewpoint of thermodynamics alone often fail to specify the actual configuration of a catalyst for the dynamic CO RR process. Herein, we re-survey recent studies with the emphasis on revealing the dynamic chemical state of Cu sites under CO RR conditions extracted by in situ/operando characterizations, and further validate a critical link between the chemical state of Cu and the product profile of CO RR. This point of view provides a generalizable concept of dynamic chemical-state-driven CO RR selectivity that offers an inspiration in both fundamental understanding and efficient electrocatalysts design.
电催化剂活性的提高和选择性的增强通常归因于特定的结构特征，如表面晶面、形态和原子缺陷。然而，由于电催化剂的表面状态是动态的，且在工作条件下难以预测，因此要弄清楚真正控制一氧化碳直接电化学还原（CO RR）的因素仍然极具挑战性。此外，仅从热力学角度进行的理论预测往往无法确定动态CO RR过程中催化剂的实际构型。在此，我们重新审视了近期的研究，重点是揭示通过原位/操作表征提取的CO RR条件下铜位点的动态化学状态，并进一步验证了铜的化学状态与CO RR产物分布之间的关键联系。这一观点提供了一个可推广的动态化学状态驱动CO RR选择性的概念，为基础理解和高效电催化剂设计提供了灵感。
