In:
Journal of Materials Chemistry A, Royal Society of Chemistry (RSC), Vol. 11, No. 1 ( 2023), p. 241-250
Abstract:
Realizing CO 2 reduction with H 2 O oxidation on g-C 3 N 4 -based photocatalysts is quite promising yet challenging. Herein, an efficient direct Z-scheme heterostructure of ultrathin CsPbBr 3 /g-C 3 N 4 nanosheets is fabricated via a simple electrostatic self-assembly process, resulting in an effective photocatalytic reduction of CO 2 to CH 4 (184.0 μmol g −1 ) and CO (105.2 μmol g −1 ) with oxidation of H 2 O under AM 1.5G irradiation. Notably, in situ X-ray photoelectron spectroscopy (XPS) analysis demonstrated that a direct Z-scheme charge transfer mechanism at the CsPbBr 3 and g-C 3 N 4 interface is enabled, thereby achieving efficient charge separation and high redox potentials to drive photocatalytic CO 2 reduction and H 2 O oxidation synchronously. Isotopic labelling experiments revealed that the adsorbed water is activated to release H atoms and eventually assists the CO 2 reduction. Theoretical calculations further revealed that the p orbitals of Pb atoms hybridize with the 2π* orbitals of CO 2 molecules, strengthening the affinity of CO 2 and weakening the binding strength. Moreover, overlapping between Pb p orbitals and 5σ orbitals of CO molecules promote the protonation of CO* intermediates. This work provides an in-depth understanding and guidance for constructing high-efficiency catalysts for CO 2 reduction with H 2 O oxidation.
Type of Medium:
Online Resource
ISSN:
2050-7488
,
2050-7496
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2023
detail.hit.zdb_id:
2702232-8
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