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https://hdl.handle.net/2440/139677
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Type: | Journal article |
Title: | Proton Shuttling by Polyaniline of High Brønsted Basicity for Improved Electrocatalytic Ethylene Production from CO₂ |
Other Titles: | Proton Shuttling by Polyaniline of High Bronsted Basicity for Improved Electrocatalytic Ethylene Production from CO2 |
Author: | Cheng, J. Chen, L. Xie, X. Feng, K. Sun, H. Qin, Y. Hua, W. Zheng, Z. He, Y. Pan, W. Yang, W. Lyu, F. Zhong, J. Deng, Z. Jiao, Y. Peng, Y. |
Citation: | Angewandte Chemie International Edition, 2023; 62(44):e202312113-1-e202312113-11 |
Publisher: | Wiley |
Issue Date: | 2023 |
ISSN: | 1433-7851 1521-3773 |
Statement of Responsibility: | Jian Cheng, Ling Chen, Xulan Xie, Kun Feng, Hao Sun, Yongze Qin, Wei Hua, Zhangyi Zheng, Ying He, Weiyi Pan, Wenjun Yang, Fenglei Lyu, Jun Zhong, Zhao Deng, Yan Jiao, and Yang Peng |
Abstract: | Hybrid organic/inorganic composites with the organic phase tailored to modulatelocal chemical environment at the Cu surface arise as an enchanting category of catalysts for electrocatalytic CO2 reduction reaction (CO2RR). A fundamental understanding on how the organics of different functionality, polarity, and hydrophobicity affect the reaction path is, however, still lacking to guide rational catalyst design. Herein, polypyrrole (PPy) and polyaniline (PANI) manifesting different Brønsted basicity are compared for their regulatory roles on the CO2RR pathways regarding *CO coverage, proton source and interfacial polarity. Concerted efforts from in situ IR, Raman and operando modelling unveil that at the PPy/Cu interface with limited *CO coverage, hydridic *H produced by the Volmer step favors the carbon hydrogenation of *CO to form *CHO through a Tafel process; Whereas at the PANI/Cu interface with concentrated CO2 and high *CO coverage, protonic H+ shuttled through the benzenoid -NH- protonates the oxygen of *CO, yielding *COH for asymmetric coupling with nearby *CO to form *OCCOH under favored energetics. As a result of the tailored chemical environment, the restructured PANI/Cu composite demonstrates a high partial current density of 0.41 A cm-2 at a maximal Faraday efficiency of 67.5% for ethylene production, ranking among states of the art. |
Keywords: | Brønsted basicity electrocatalytic CO2 reduction reaction Ethylene polyaniline polypyrrole |
Description: | Version of record online: September 6, 2023 |
Rights: | © 2023 Wiley-VCH Gm. |
DOI: | 10.1002/anie.202312113 |
Grant ID: | http://purl.org/au-research/grants/arc/FT190100636 |
Published version: | http://dx.doi.org/10.1002/anie.202312113 |
Appears in Collections: | Chemical Engineering publications |
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