Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 9, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202110657
Keywords
CO2 conversion; Electrochemistry; Ionic liquids; Polymer modification; Tandem catalyst
Categories
Funding
- Key Research Program of Frontier Sciences, CAS [ZDBS-LY-JSC022]
- Excellent Young Scientists Fund [22022815]
- National Natural Science Foundation of China [U1704251, 21776291]
- Zhengzhou High Level Talent Certificate [20180200052]
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A poly(ionic liquid) (PIL)-based Cu-0-Cu-I tandem catalyst was designed for the electroreduction of CO2 to C2+ products. The catalyst showed high reaction rate and selectivity, with a high Faradaic efficiency and partial current density. Mechanistic studies revealed the importance of Cu-0-PIL and PIL-Cu-I interfaces in achieving the desired reactivity.
Electroreduction of CO2 on a polymer-modified Cu-based catalyst has shown high multi-electron reduction (>2 e(-)) selectivity, however, most of the corresponding current densities are still too small to support industrial applications. In this work, we designed a poly(ionic liquid) (PIL)-based Cu-0-Cu-I tandem catalyst for the production of C2+ products with both high reaction rate and high selectivity. Remarkably, a high C2+ faradaic efficiency (FEC2+) of 76.1 % with a high partial current density of 304.2 mA cm(-2) is obtained. Mechanistic studies reveal the numbers and highly dispersed Cu-0-PIL-Cu-I interfaces are vital for such reactivity. Specifically, Cu nanoparticles derived Cu-0-PIL interfaces account for high current density and a moderate C(2+ )selectivity, whereas Cu-I species derived PIL-Cu-I interfaces exhibit high activity for C-C coupling with the local enriched *CO intermediate. Furthermore, the presence of the PIL layer promotes the C2+ selectivity by lowering the barrier of C-C coupling.
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