Enhanced photocatalytic hydrogen production through modification of B←N coordination units

Low efficiency of photogenerated electron-hole separation has been a challenge for organic conjugated polymer photocatalysts. Our preceding studies have revealed that polymers containing B←N coordination bonds can form a localized built-in electric field that effectively promotes photogenerated char...

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Veröffentlicht in:New journal of chemistry 2024-08, Vol.48 (33), p.14655-14662
Hauptverfasser: Gu, Junyi, Qiang, Yanan, Mu, Xuemei, Liu, Zhihai, Zhang, Chao, Lai, Min, Pan, Xiaobo, Zhao, Hao
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Sprache:eng
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Zusammenfassung:Low efficiency of photogenerated electron-hole separation has been a challenge for organic conjugated polymer photocatalysts. Our preceding studies have revealed that polymers containing B←N coordination bonds can form a localized built-in electric field that effectively promotes photogenerated charge separation. However, B←N coordination units are still scarce and require more examples to find regularities in their structural design. The systematic development and testing of B←N coordination units is necessary for the efficient development of subsequent polymers containing B←N coordination bonds. In this work, three conjugated polymers containing B←N coordination bonds, PBN-Ni , PBP-Ni , and PBS-Ni , were synthesized by changing the substituents of the boron atoms and introducing narrow-band thiophene units to form conjugate and energy band gradients. The energy band modulation and localized built-in electric field construction were both achieved as planned, while the bandgap and photogenerated charge transport capabilities caused performance discrepancies. The experimental results showed that PBN-Ni had a better photocatalytic hydrogen evolution (HER) performance, reaching 104.6 μmol h −1 ( λ > 420 nm). The optimal optical absorption edge of PBS-Ni was up to 643 nm, but the HER was lower, at 33.2 μmol h −1 ( λ > 420 nm, 1% Pt). PBP-Ni optimized some of the optical absorption efficiencies (511 nm) while ensuring the HER activity (96.6 μmol h −1 , λ > 420 nm). This work tentatively explores the characterization of the B←N coordination bond-containing base units serving as photocatalysts and provides the basic model experience and data reference for the subsequent expansion of B←N coordination bond-containing units and the development of B←N coordination bond-containing copolymer systems. Built-in electric field construction and energy band modulation of B←N containing polymer units to expand B←N photocatalyst systems.
ISSN:1144-0546
1369-9261
DOI:10.1039/d4nj01729c