Authors
Zongzhao Liu, Bo Cheng, Hengchao Wang, Qiang Zhang, Yucheng Liu, Ke Wang, Zhaohang Ben, Di Wang, Yan Lu
Published in
Small (Weinheim an der Bergstrasse, Germany). Pages e75833. Sep 18, 2026. Epub Sep 18, 2026.
Abstract
Structural defects in conjugated polymers are traditionally perceived as detrimental charge traps that impair optoelectronic performance. Here, we demonstrate a counterintuitive "defect-enabled" strategy for benchmark photocatalytic hydrogen evolution. Two donor (D)-acceptor (A) linear conjugated polymers (P-s and P-d) are synthesized via Suzuki-Miyaura polycondensation (P-s) and direct arylation polymerization (P-d), using dibenzothiophene-S, S-dioxide (DBTO) and 10-methylphenothiazine as A and D units, respectively. A comprehensive solid-state 13C NMR, XPS, Raman, and elemental analysis methodology is established to quantify structural defects, specifically A-A homo‑coupling (DBTO-DBTO) junctions that deviate from the ideal alternating D-A structure in these insoluble polymers. Remarkably, P-d exhibits approximately five-fold higher defect density (32.4% vs. 6.5%). This defect-induced DBTO enrichment simultaneously narrows the bandgap (1.81 vs. 2.10 eV), accelerates charge separation (evidenced by TRPL, TAS, and EIS), and provides abundant active sites (DFT-identified oxygen sites with ΔGH ≈ 1.38 eV). As a result, P-d achieves an outstanding hydrogen evolution rate of 476.38 mmol h- 1 g- 1 (with 2 wt.% Pt and 0.5% NP-40), surpassing most reported linear conjugated polymer photocatalysts. This work establishes a clear structure-property correlation for structural defects in polymeric photocatalysts and introduces a rational defect-engineering strategy for designing high-performance energy conversion materials.
PMID:
42758880
Bibliographic data and abstract were imported from PubMed on 19 Sep 2026.
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