Impact of Side Chains in 1-n-Alkylimidazolium Ionomers on Cu-Catalyzed Electrochemical CO 2 Reduction.

Autor: Song YI; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; School of Chemical Engineering, Sungkyunkwan University (SKKU), Suwon, 16419, Republic of Korea., Yoon B; Department of Chemistry, Chicago Center for Theoretical Chemistry, Institute for Biophysical Dynamics, and James Franck Institute, The University of Chicago, Chicago, IL 60637, USA., Lee C; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; Division of Energy & Environment Technology, KIST School, University of Science and Technology, Seoul, 02792, Republic of Korea., Kim D; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; Department of Chemical and Biological Engineering, Korea University, Seoul, 02841, Republic of Korea., Han MH; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea., Han H; School of Chemical Engineering, Sungkyunkwan University (SKKU), Suwon, 16419, Republic of Korea., Lee WH; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; Division of Energy & Environment Technology, KIST School, University of Science and Technology, Seoul, 02792, Republic of Korea., Won DH; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; Division of Energy & Environment Technology, KIST School, University of Science and Technology, Seoul, 02792, Republic of Korea.; KHU-KIST Department of Converging Science and Technology, Kyung Hee University, Seoul, 02477, Republic of Korea., Kim JK; School of Chemical Engineering, Sungkyunkwan University (SKKU), Suwon, 16419, Republic of Korea., Jeon HS; Technological Convergence Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea., Koh JH; Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul, 02792, Republic of Korea.; Division of Energy & Environment Technology, KIST School, University of Science and Technology, Seoul, 02792, Republic of Korea.
Jazyk: angličtina
Zdroj: Advanced science (Weinheim, Baden-Wurttemberg, Germany) [Adv Sci (Weinh)] 2024 Oct 31, pp. e2406281. Date of Electronic Publication: 2024 Oct 31.
DOI: 10.1002/advs.202406281
Abstrakt: This study presents the impact of the side chains in 1-n-alkylimidazolium ionomers with varying side chain lengths (C n H 2n+1 where n = 1, 4, 10, 16) on Cu-catalyzed electrochemical CO 2 reduction reaction (CO 2 RR). Longer side chains suppress the H 2 and CH 4 formation, with the n-hexadecyl ionomer (n = 16) showing the greatest reduction in kinetics by up to 56.5% and 60.0%, respectively. On the other hand, C 2 H 4 production demonstrates optimal Faradaic efficiency with the n-decyl ionomer (n = 10), a substantial increase of 59.9% compared to its methyl analog (n = 1). Through a combination of density functional theory calculations and material characterization, it is revealed that the engineering of the side chains effectively modulates the thermodynamic stability of key intermediates, thus influencing the selectivity of both CO 2 RR and hydrogen evolution reaction. Moreover, ionomer engineering enables industrially relevant partial current density of -209.5 mA cm -2 and a Faradaic efficiency of 52.4% for C 2 H 4 production at 3.95 V, even with a moderately active Cu catalyst, outperforming previous benchmarks and allowing for further improvement through catalyst engineering. This study underscores the critical role of ionomers in CO 2 RR, providing insights into their optimal design for sustainable chemical synthesis.
(© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)
Databáze: MEDLINE
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