Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte

Qin，Hai Gang; Du，Yun Fan; Bai，Yi Yang; Li，Fu Zhi; Yue，Xian; Wang，Hao; Peng，Jian Zhao; Gu，Jun

2023-12-01

10.1038/s41467-023-41396-2

Nature Communications   Impact Factor & Quartile

2041-1723

Electrochemical CO reduction in acidic electrolytes is a promising strategy to achieve high utilization efficiency of CO. Although alkali cations in acidic electrolytes play a vital role in suppressing hydrogen evolution and promoting CO reduction, they also cause precipitation of bicarbonate on the gas diffusion electrode (GDE), flooding of electrolyte through the GDE, and drift of the electrolyte pH. In this work, we realize the electroreduction of CO in a metal cation-free acidic electrolyte by covering the catalyst with cross-linked poly-diallyldimethylammonium chloride. This polyelectrolyte provides a high density of cationic sites immobilized on the surface of the catalyst, which suppresses the mass transport of H and modulates the interfacial field strength. By adopting this strategy, the Faradaic efficiency (FE) of CO reaches 95 ± 3% with the Ag catalyst and the FE of formic acid reaches 76 ± 3% with the In catalyst in a 1.0 pH electrolyte in a flow cell. More importantly, with the metal cation-free acidic electrolyte the amount of electrolyte flooding through the GDE is decreased to 2.5 ± 0.6% of that with alkali cation-containing acidic electrolyte, and the FE of CO maintains above 80% over 36 h of operation at −200 mA·cm.

SCI

English

NI Journal Papers

First ; Corresponding

National Natural Science Foundation of China-Yunnan Joint Fund[22272073];Science, Technology and Innovation Commission of Shenzhen Municipality[JCYJ20210324104414039];Science, Technology and Innovation Commission of Shenzhen Municipality[JCYJ20220818100410023];Science, Technology and Innovation Commission of Shenzhen Municipality[KCXST20221021111207017];

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:001087583700025

NATURE PORTFOLIO

2-s2.0-85171161533

Scopus

Department of Chemistry,Southern University of Science and Technology,Shenzhen,Guangdong,China

Qin，Hai Gang,Du，Yun Fan,Bai，Yi Yang,et al. Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte[J]. Nature Communications,2023,14(1).

Qin，Hai Gang.,Du，Yun Fan.,Bai，Yi Yang.,Li，Fu Zhi.,Yue，Xian.,...&Gu，Jun.(2023).Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte.Nature Communications,14(1).

Qin，Hai Gang,et al."Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte".Nature Communications 14.1(2023).