Boosting photocatalytic water oxidation on lead chromate through crystal facet engineering

IF 11.5 Q1 CHEMISTRY, PHYSICAL

Chem Catalysis Pub Date : 2024-10-25 DOI:10.1016/j.checat.2024.101153

Wenchao Jiang, Chenwei Ni, Yejun Xiao, Yue Zhao, Chu Han, Xuan Wu, Chengbo Zhang, Haibo Chi, Rengui Li, Can Li

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Abstract

Although crystal facet engineering of semiconductor crystals has been demonstrated to be effective in particulate photocatalysts for solar energy conversion, it is imperative to rationally regulate the exposed crystal facets and their configurations to improve charge separation efficiency. In this study, focusing on visible-light-driven water oxidation photocatalyst lead chromate (PbCrO₄), we find that a flux-assisted treatment enables the precise tuning of the hole-accumulating facets of anisotropic PbCrO₄ crystal, transitioning the top surface from {−101} to {001} facets while preserving its spatial charge separation characteristics. Owing to the superior hole-accumulating property and water oxidation kinetics of the {001} facets, the resulting Flux-PbCrO₄ crystals achieve a charge separation efficiency exceeding 75%, leading to a remarkable improvement in photocatalytic water oxidation activity. Further incorporation of cocatalysts onto the Flux-PbCrO₄ crystals results in an apparent quantum efficiency of 18.5% at 500 nm for photocatalytic water oxidation.

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通过晶面工程提高铬酸铅的光催化水氧化能力

虽然在用于太阳能转换的微粒光催化剂中，半导体晶体的晶面工程已被证明是有效的，但要提高电荷分离效率，必须合理调节暴露的晶面及其构型。在本研究中，我们以可见光驱动的水氧化光催化剂铬酸铅（PbCrO4）为研究对象，发现通过助焊剂辅助处理，可以精确调节各向异性 PbCrO4 晶体的空穴堆积面，在保留其空间电荷分离特性的同时，将顶面从 {-101} 过渡到 {001} 面。由于{001}面具有优异的空穴聚集特性和水氧化动力学特性，所得到的 Flux-PbCrO4 晶体的电荷分离效率超过 75%，从而显著提高了光催化水氧化活性。在 Flux-PbCrO4 晶体上进一步加入茧催化剂后，500 纳米波长下光催化水氧化的表观量子效率达到了 18.5%。

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来源期刊

Chem Catalysis

CiteScore

10.50

自引率

6.40%

发文量

期刊介绍： Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.