Volume 137, Issue 9 e202419865
Zuschrift

Selenium-Substitution Strategy for Enhanced Mobility, Tunable Bandgap, and Improved Electrochemical Energy Storage in Semiconducting Conjugated Coordination Polymers

Sha Wu

Sha Wu

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of Chinese Academy of Sciences, Beijing, 100049 China

These authors contributed equally to this work

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Dr. Xing Huang

Corresponding Author

Dr. Xing Huang

Center for Advancing Electronics Dresden (cfaed), Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062 Germany

These authors contributed equally to this work

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Dr. Shuai Fu

Dr. Shuai Fu

Center for Advancing Electronics Dresden (cfaed), Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062 Germany

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Ze Li

Ze Li

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of Chinese Academy of Sciences, Beijing, 100049 China

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Siping Yin

Siping Yin

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of Chinese Academy of Sciences, Beijing, 100049 China

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Wenkai Liao

Wenkai Liao

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of Chinese Academy of Sciences, Beijing, 100049 China

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Dr. Mingchao Wang

Dr. Mingchao Wang

Center for Advancing Electronics Dresden (cfaed), Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062 Germany

School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen, 518055 China

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Dr. Yang Lu

Dr. Yang Lu

Center for Advancing Electronics Dresden (cfaed), Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062 Germany

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Prof. Mischa Bonn

Prof. Mischa Bonn

Max Planck Institute for Polymer Research, Mainz, 55128 Germany

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Dr. Yimeng Sun

Dr. Yimeng Sun

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Xinliang Feng

Corresponding Author

Prof. Xinliang Feng

Center for Advancing Electronics Dresden (cfaed), Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, 01062 Germany

Max Planck Institute of Microstructure Physics, Halle Saale, 06120 Germany

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Prof. Wei Xu

Corresponding Author

Prof. Wei Xu

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of Chinese Academy of Sciences, Beijing, 100049 China

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First published: 21 January 2025

Abstract

Conjugated coordination polymers (c-CPs), a novel class of organic–inorganic hybrid materials, are distinguished by their unique structural characteristics and exceptional charge transport properties. The electronic properties of these materials are critically determined by the constituting coordination atoms, with electron-rich selenol ligands emerging as promising candidates for constructing high-mobility semiconducting c-CPs. Despite their potential, c-CPs incorporating selenium-substituted ligands remain scarce due to the synthetic challenges associated with both the ligands and the coordination polymers. In this study, we successfully synthesized a new tetraselenol-hydroxyquinone (TSHQ) ligand using a “4+2” design strategy and developed a semiconducting three-dimensional Ag−Se coordination polymer, Ag4TSHQ. Ag4TSHQ exhibits room-temperature electrical conductivity of up to 1.6 S/m and shares the same structural topology as Ag4TTHQ (TTHQ=tetrathiol-hydroxyquinone), enabling precise band gap modulation from 0.6 eV to 1.5 eV via a mixed-ligand approach. Time-resolved terahertz spectroscopy reveals that the charge mobility of Ag4TSHQ in the dc limit is ~350 cm2/V ⋅ s, which is twice that of its sulfur counterpart, Ag4TTHQ. Furthermore, our evaluations of their electrochemical energy storage capabilities demonstrate that Ag4TSHQ effectively utilizes its redox potential, achieving a remarkable specific capacitance of up to 340 F/g-significantly outperforming Ag4TTHQ, which has a capacitance of 294 F/g. These findings underscore the potential of selenium-ligand-based c-CPs for optoelectronic applications and energy storage technologies.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available on request from the corresponding author. The data are not publicly available due to privacy or ethical restrictions.

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