In Situ Halogen‐Ion Leaching Regulates Multiple Sites on Tandem Catalysts for Efficient CO2 Electroreduction to C2+ Products. Issue 21 (24th March 2022)

• Record Type: Journal Article
• Authors: Yang, Ruoou; Duan, Junyuan; Dong, Panpan; Wen, Qunlei; Wu, Mao; Liu, Youwen; Liu, Yan; Li, Huiqiao; Zhai, Tianyou
• Is Part Of: Angewandte Chemie international edition. Volume 61:Issue 21(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-03-24
• Subjects: AgI−CuO -- CO2 Electroreduction -- Cu0/Cu+ Sites -- Iodine Ions Leaching -- Tandem Catalysts; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202116706
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Tandem catalysts can divide the reaction into distinct steps by local multiple sites and thus are attractive to trigger CO2 RR to C2+ products. However, the evolution of catalysts generally exists during CO2 RR, thus a closer investigation of the reconstitution, interplay, and active origin of dual components in tandem catalysts is warranted. Here, taking AgI−CuO as a conceptual tandem catalyst, we uncovered the interaction of two phases during the electrochemical reconstruction. Multiple operando techniques unraveled that in situ iodine ions leaching from AgI restrained the entire reduction of CuO to acquire stable active Cu 0 /Cu + species during the CO2 RR. This way, the residual iodine species of the Ag matrix accelerated CO generation and iodine‐induced Cu 0 /Cu + promotes C−C coupling. This self‐adaptive dual‐optimization endowed our catalysts with an excellent C2+ Faradaic efficiency of 68.9 %. Material operando changes in this work offer a new approach for manipulating active species towards enhancing C2+ products. Abstract : The interplay of dual components in tandem catalysts is uncovered and utilized during the electrochemical reconstruction for promoting CO2 electroreduction to C2+ products. Taking AgI−CuO as a conceptual tandem catalyst, in situ iodine ions leaching from AgI restrain the entire reduction of CuO to acquire stable active Cu 0 /Cu + species, thus achieving a high C2+ Faradaic efficiency of 68.9 %.