Enhanced piezo-photocatalytic water splitting activity via engineering robust dipole moments in covalent organic frameworks.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41387708.
- Also identified by DOI 10.1038/s41467-025-67467-0 and PMC identifier 12819517.
- Licence recorded as CC BY-NC-ND.
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Abstract
Covalent organic frameworks with tunable optical bandgaps and notable piezoelectricity enable sustainable piezo-photocatalytic production of H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> via pure water splitting. Strong dipole moments can significantly boost piezoelectric properties, necessitating a systematic exploration of their structure-property relationships. Here, we synthesize a series of β-ketoenamine/imine-linked covalent organic frameworks, such as TP-BT-0F/1F/2F-COF, BTA-BT-0F-COF, and TP-SB-COF, through molecular design engineering. The combination of symmetry-breaking benzothiadiazole units and in-plane polarized β-ketoenamine linkages creates a robust dipole moment in TP-BT-0F-COF. This material demonstrates a high piezoelectric coefficient and bandgap narrowing, achieving H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> production rates of 1501.4 and 1435.8 μmol g<sup>-1</sup> h<sup>-1</sup> under co-exposure to ultrasound (60 W, 40 kHz) and visible light. Density functional theory identifies N<sup>8</sup> and C<sup>6</sup> sites on benzothiadiazole units as potential catalytic sites for H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> evolution, respectively. Molecular design of covalent organic frameworks with prominent dipole moments advances mechano-optical energy conversion technologies.