journal article·2026-04Open access

Atomic‐Level Ionic Displacement Polarization Enhanced Piezocatalytic Hydrogen Evolution in Covalent Organic Frameworks

Ge Yan, Xiaodong Sun, Kailai Zhang, Shuai Zhang, Haijun Hu, Hui Li, Zhenglong Li, Hongwei Huang, Liqun Ye, Jiyang Li, Yunling Liu, Hongge Pan, Tianyi Ma

Advanced Functional Materials· Volume 36· Issue 34

Abstract

ABSTRACT Adjusting the structural units of the covalent organic frameworks (COFs) to enhance polarization intensity can resolve the severe carrier recombination issue in piezocatalysis. Herein, two isomorphic COFs are synthesized and compared, including zwitterionic COF (SQ‐TAPT) with uneven charge distribution and neutral COF (PDA‐TAPT) with charge‐stabilization. Due to the increased Born effective charges arising from ionic bonding, SQ‐TAPT exhibits stronger ionic displacement polarization, resulting in a higher polarizability and enhanced piezoelectric response. Specifically, the d 33 value of SQ‐TAPT can reach 1.1 nm/V. Besides, all the Gibbs free energies in the active sites of SQ‐TAPT are lower than that of PDA‐TAPT, with the most optimal free energy of 0.56 eV. Moreover, the zwitterionic charge characteristic of SQ‐TAPT also gives it a superior hydrophilicity, conducive to hydrogen production in the process of water splitting. Attributable to the advantages of SQ‐TAPT, its piezoelectric hydrogen production rate can achieve 745.9 µmol·g −1 ·h −1 in the absence of co‐catalysts, which is 2.9 times higher than that of PDA‐TAPT, and exhibited a high piezocatalytic activity that is competitive with the state‐of‐the‐art catalysts reported. SQ‐TAPT demonstrates the feasibility of utilizing zwitterionic COFs in piezocatalysis. This research provides a novel perspective for modulating charge distribution, which in turn aids in designing piezoelectric catalysts based on molecular structure.
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Research context

OpenAlex topics: Covalent Organic Framework Applications · Advanced Photocatalysis Techniques · Ammonia Synthesis and Nitrogen Reduction

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Adv. Mater. College of Chemistry Liaoning University Shenyang P. R. China

Centre for Atomaterials and Nanomanufacturing (CAN) School of Science RMIT University Melbourne Victoria Australia

School of Chemistry and Chemical Engineering South China University of Technology Guangzhou Guangdong P. R. China

ARC Industrial Transformation Research Hub for Intelligent Energy Efficiency in Future Protected Cropping (E2Crop) Melbourne Victoria Australia

Institute of Science and Technology for New Energy Xi'an Technological University Xi'an P. R. China

Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral Materials School of Materials Science and Technology China University of Geosciences Beijing P. R. China

College of Materials and Chemical Engineering Key Laboratory of inorganic nonmetallic crystalline and energy conversion materials China Three Gorges University Yichang P. R. China

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun P. R. China

Funding

National Natural Science Foundation of China · Australian Research Council · Higher Education Discipline Innovation Project

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