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 |
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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. |
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ISSN: | 1144-0546 1369-9261 |
DOI: | 10.1039/d4nj01729c |