Volume 134, Issue 5 e202115503
Zuschrift

Proton/Electron Donors Enhancing Electrocatalytic Activity of Supported Conjugated Microporous Polymers for CO2 Reduction

Dr. Rong Wang

Dr. Rong Wang

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200438 China

These authors contributed equally to this work.

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Xinyue Wang

Xinyue Wang

Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China

These authors contributed equally to this work.

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Weijun Weng

Weijun Weng

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200438 China

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Ying Yao

Ying Yao

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200438 China

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Dr. Pinit Kidkhunthod

Dr. Pinit Kidkhunthod

Synchrotron Light Research Institute (Public Organization), 111 University Avenue, Muang District, Nakhon Ratchasima, 30000 Thailand

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Prof. Dr. Changchun Wang

Prof. Dr. Changchun Wang

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200438 China

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Prof. Dr. Yang Hou

Corresponding Author

Prof. Dr. Yang Hou

Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China

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Prof. Dr. Jia Guo

Corresponding Author

Prof. Dr. Jia Guo

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200438 China

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First published: 01 December 2021

Abstract

Metal phthalocyanines (MePc) hold great promise in electrochemical reduction of CO2 to value-added chemicals, whereas the catalytic activity of MePc-containing polymers often suffers from a limited molecular modulation strategy. Herein, we synthesize an ultrathin conjugated microporous polymer sheath around carbon nanotubes by an ionothermal copolymerization of CoPc and H2Pc via the Scholl reaction. Given the H2Pc-mediated regulation in the synthesis, CoII metal is well preserved in the form of single atoms on the polymer sheath of the carbon nanotubes. With the synergistic effect of H2Pc moieties as proton/electron donors, the composites can selectively reduce CO2 to CO with a high Faradaic efficiency (max. 97 % at −0.9 V) in broad potential windows, exceptional turnover frequency (97 592 h−1 at −0.65 V) and large current density (>200 mA cm−2). It is thus desirable to develop a family of heterogeneous polymerized MePc with molecularly regulating electrocatalytic activity.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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