Robust Electrocatalytic CO2 Reduction in Acid Enabled by 'Molecularly Charged' Cobalt Phthalocyanine: A Profound Understanding from Electric Double Layer - Details

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Electrocatalytic　CO2　reduction　(eCO2R)　in　acid　holds　promise　in　renewable　electricity-powered　CO2　utilization　with　high　efficiency,　but　the　hydrogen　evolution　reaction　(HER)　often　prevails　and　results　in　a　low　eCO2R　selectivity.　Here,　using　cobalt　phthalocyanine/Ketjen　black　(CoPc/KB)　as　the　model　catalysts,　we　systematically　study　the　effect　of　active　site　density,　operational　current　density,　and　hydrated　cations　on　the　acidic　eCO2R　selectivity　and　decipher　it　through　the　componential　dynamics　of　electric　double　layer　(EDL).　The　optimal　CoPc-4/KB　demonstrates　a　near-unity　CO　Faradaic　efficiency　from　50　to　400　mA　cm-2　and　superb　operational　stability　(＞120　h)　at　100　mA　cm-2.　Aided　by　in　situ　Raman　and　infrared　spectroscopies,　we　reveal　that　the　proper　cations　establish　an　electrostatic　shield　for　mitigating　bulk　H+　penetration　and　mediate　the　interfacial　water　structure　for　suppressing　HER.　This　study　should　elicit　further　profound　thinking　on　robust　eCO2R　system　design　from　the　perspective　of　multiphasic　and　dynamic　EDL.　©　2024　American　Chemical　Society.

Keyword：

Catalyst selectivity Cobalt Electrochemistry Carbon dioxide Catalyst activity Efficiency Positive ions

Author Community：

[ 1 ] [Jiao, Zhenyang]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 2 ] [Song, Daqi]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 3 ] [Wei, Le]Beijing Key Laboratory of Microstructure and Properties of Solids, College of Materials Science and Engineering, Beijing University of Technology, Beijing; 100124, China
[ 4 ] [Ma, Mutian]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 5 ] [Hua, Wei]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 6 ] [Zheng, Zhangyi]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 7 ] [Wang, Min]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 8 ] [Su, Yanhui]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 9 ] [Ke, Xiaoxing]Beijing Key Laboratory of Microstructure and Properties of Solids, College of Materials Science and Engineering, Beijing University of Technology, Beijing; 100124, China
[ 10 ] [Lyu, Fenglei]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 11 ] [Lyu, Fenglei]Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou; 215006, China
[ 12 ] [Deng, Zhao]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 13 ] [Deng, Zhao]Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou; 215006, China
[ 14 ] [Zhong, Jun]Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou; 215123, China
[ 15 ] [Peng, Yang]Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou; 215006, China
[ 16 ] [Peng, Yang]Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou; 215006, China

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Source ：

Journal of Physical Chemistry Letters

Year： 2024

Issue： 28

Volume： 15

Page： 7342-7350

5 . 7 0 0

JCR@2022

Cited Count：

WoS CC Cited Count：

SCOPUS Cited Count： 2

ESI Highly Cited Papers on the List： 0 Unfold All

WanFang Cited Count：

Chinese Cited Count：

30 Days PV： 7

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