Volume 137, Issue 30 e202507612
Forschungsartikel

Supramolecularly Confined Catalysis in Polyphthalocyanine-Crown-Ether Frameworks Boosts Sulfur Redox Kinetics

Xinming Zhang

Xinming Zhang

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Qing-Xuan Chen

Qing-Xuan Chen

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Wentao Zhang

Wentao Zhang

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Hongyin Hu

Hongyin Hu

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Huimin Wu

Huimin Wu

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Zhaotian Xie

Zhaotian Xie

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Xin He

Xin He

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Yilin Niu

Yilin Niu

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Xianming Deng

Xianming Deng

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Li Liu

Li Liu

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 P.R. China

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Prof. Zhenghua Zhang

Prof. Zhenghua Zhang

Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, Guangdong, 518055 P.R. China

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Prof. Dr. Lele Peng

Corresponding Author

Prof. Dr. Lele Peng

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

E-mail: [email protected]; [email protected]

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Prof. Dr. Zhen Chen

Corresponding Author

Prof. Dr. Zhen Chen

Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055 P.R. China

E-mail: [email protected]; [email protected]

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First published: 15 May 2025

Abstract

Metal phthalocyanines are considered as potent catalysts in lithium–sulfur (Li–S) chemistry. However, their adsorption capability is deficient to inhibit polysulfides from shuttling, which in turn retards the S-redox reaction in the cathode. Here we report flexible, two-dimensional (2D) polyphthalocyanine-crown-ether (PPc-CE) frameworks that provide a supramolecularly confined space created with the single-atom catalytic nickel phthalocyanine nodes and crown-ether linkers as Li host. Electrochemical and theoretical analyses reveal that a cooperative redox catalysis with the enhanced lithiophilicity of PPc-CE-coated carbon nanotubes (PPc-CE/CNTs) boosts Li–S redox kinetics and, meanwhile, suppresses the growth of Li dendrites for the long term. A Li||S cell employing PPc-CE/CNT catalysts delivers a high discharge capacity of 1,363 mAh g−1 at 0.1C and still retains a specific capacity of ∼700 mAh g−1 over 500 cycles at 1C. Our work provides insights into the molecular design of redox catalysts for Li–S batteries based on 2D polymers.

Conflict of Interests

The authors declare no conflict of interest.

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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