Solar-CO2 -to-Syngas Conversion Enabled by Precise Charge Transport Modulation.
Small
; 19(35): e2300804, 2023 Aug.
Article
em En
| MEDLINE
| ID: mdl-37183292
ABSTRACT
The rational design of the directional charge transfer channel represents an important strategy to finely tune the charge migration and separation in photocatalytic CO2 -to-fuel conversion. Despite the progress made in crafting high-performance photocatalysts, developing elegant photosystems with precisely modulated interfacial charge transfer feature remains a grand challenge. Here, a facile one-pot method is developed to achieve in situ self-assembly of Pd nanocrystals (NYs) on the transition metal chalcogenide (TMC) substrate with the aid of a non-conjugated insulating polymer, i.e., branched polyethylenimine (bPEI), for photoreduction of CO2 to syngas (CO/H2 ). The generic reducing capability of the abundant amine groups grafted on the molecular backbone of bPEI fosters the homogeneous growth of Pd NYs on the TMC framework. Intriguingly, the self-assembled TMCs@bPEI@Pd heterostructure with bi-directional spatial charge transport pathways exhibit significantly boosted photoactivity toward CO2 -to-syngas conversion under visible light irradiation, wherein bPEI serves as an efficient hole transfer mediator, and simultaneously Pd NYs act as an electron-withdrawing modulator for accelerating spatially vectorial charge separation. Furthermore, in-depth understanding of the in situ formed intermediates during the CO2 photoreduction process are exquisitely probed. This work provides a quintessential paradigm for in situ construction of multi-component heterojunction photosystem for solar-to-fuel energy conversion.
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MEDLINE
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En
Ano de publicação:
2023
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Article