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. 2025 May 16;30(10):2190.
doi: 10.3390/molecules30102190.

D1-A-D2 Conjugated Porous Polymers Provide Additional Electron Transfer Pathways for Efficient Photocatalytic Hydrogen Production

Zheng-Hui Xie  1 , Yu-Jie Zhang  1 , Jinhua Li  1 , Shi-Yong Liu  1   2
Affiliations

D1-A-D2 Conjugated Porous Polymers Provide Additional Electron Transfer Pathways for Efficient Photocatalytic Hydrogen Production

Zheng-Hui Xie et al. Molecules. .

Abstract

The strategic design of donor-acceptor (D-A) conjugated porous polymers has emerged as a pivotal methodology for advancing efficient photocatalytic hydrogen evolution. However, conventional D-A polymeric architectures face inherent limitations: excessively strong acceptor units may lower the LUMO energy level, compromising proton (H+) reduction capability, while weak D-A interactions result in inadequate light-harvesting capacity and insufficient photogenerated electrons, ultimately diminishing photocatalytic activity. To address these challenges, we developed a new D1-A-D2 conjugated porous polymer (CPP) system. The strategic incorporation of a secondary donor benzothiophene (DBBTh) unit enabled precise bandgap engineering in D1-A-D2 CPPs. Experimental results demonstrate that DBBTh integration significantly enhances both light absorption efficiency and proton reduction ability. Under visible-light irradiation (λ > 420 nm), the Py-BKh1 photocatalyst achieved a hydrogen evolution rate (HER) of 10.2 mmol h-1 g-1 with an apparent quantum yield (AQY) of 9.5% at 500 nm. This work provides a groundbreaking paradigm for designing high-performance organic photocatalysts.

Keywords: D1-A-D2 conjugated polymer; direct C–H arylation polymerization; photocatalysis; visible-light-driven hydrogen evolution; π-conjugated porous polymers.

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Conflict of interest statement

The authors declare that they have no conflicts of interest.

Figures

Figure 1
Figure 1
(a) Synthetic routes of Py-BKh0, Py-BKh1, Py-BKh2, and Py-BKh3; (b) FTIR spectra and (c) solid-state 13C NMR spectra of all polymers; SEM images of Py-BKh0 (d), Py-BKh1 (e), Py-BKh2 (f), and Py-BKh3 (g); and TEM images of Py-BKh0 (h), Py-BKh1 (i), Py-BKh2 (j), and (k) Py-BKh3.
Figure 2
Figure 2
(a) UV–vis DRS. (b) Tauc-plot maps. (c) Energy band alignments. (d) Steady-state PL spectra. (e) TPR under visible light irradiation. (f) EIS of all CPPs.
Figure 3
Figure 3
(a) Hydrogen production rate over time, (b) normalized HER for all CPPs, (c) AQY of Py-BKh1 at different wavelengths, (d) cyclic hydrogen production test for Py-BKh1.
Figure 4
Figure 4
(a) UV−vis DRS and (b) FT-IR spectra of Py-BKh1 before and after recycling tests.
See this image and copyright information in PMC

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