Nanoarchitectonics on Z-scheme and Mott-Schottky heterostructure for photocatalytic water oxidation via dual-cascade charge-transfer pathways

基于Z型和莫特-肖特基异质结构的纳米结构通过双级联电荷转移途径实现光催化水氧化

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Abstract

The bottleneck for water splitting to generate hydrogen fuel is the sluggish oxidation of water. Even though the monoclinic-BiVO(4) (m-BiVO(4))-based heterostructure has been widely applied for water oxidation, carrier recombination on dual surfaces of the m-BiVO(4) component have not been fully resolved by a single heterojunction. Inspired by natural photosynthesis, we established an m-BiVO(4)/carbon nitride (C(3)N(4)) Z-scheme heterostructure based on the m-BiVO(4)/reduced graphene oxide (rGO) Mott-Schottky heterostructure, constructing the face-contact C(3)N(4)/m-BiVO(4)/rGO (CNBG) ternary composite to remove excessive surface recombination during water oxidation. The rGO can accumulate photogenerated electrons from m-BiVO(4) through a high conductivity region over the heterointerface, with the electrons then prone to diffuse along a highly conductive carbon network. In an internal electric field at the heterointerface of m-BiVO(4)/C(3)N(4), the low-energy electrons and holes are rapidly consumed under irradiation. Therefore, spatial separation of electron-hole pairs occurs, and strong redox potentials are maintained by the Z-scheme electron transfer. These advantages endow the CNBG ternary composite with over 193% growth in O(2) yield, and a remarkable rise in ·OH and ·O(2)(-) radicals, compared to the m-BiVO(4)/rGO binary composite. This work shows a novel perspective for rationally integrating Z-scheme and Mott-Schottky heterostructures in the water oxidation reaction.

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