电荷迁移方向操纵的 BiVO4 量子点/过四羧酸 Z 型异质结与纳米金修饰在人工 H2O2 光合作用中的协同作用

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI:10.1016/S1872-2067(24)60058-6
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引用次数: 0

摘要

在此,我们通过简便的水解-重组过程合成了具有由形成的内部电场驱动的各向异性电荷迁移的过烯四羧酸(PTA)纳米片。通过原位引入 BiVO4 量子点(BQD)和纳米金,在 PTA 纳米片上不同的光生电子和空穴聚集区的基础上,战略性地构建了具有自由流动的界面电荷转移和空间分离的氧化还原中心的 Z 型异质结。与原始 PTA 相比,优化的 BQD/PTA-Au 在 405 纳米波长下的 H2O2 生成率和表观量子产率分别提高了约 6.4 倍和 4.8 倍。电子顺磁共振、原位辐照 X 射线光电子能谱和原位漫反射红外傅立叶变换能谱揭示了这种优异的活性归因于匹配电荷迁移方向的级联 Z 型电荷转移,以及金活性位点对超氧自由基诱导的 2e 氧还原途径的加速作用。这项工作为设计太阳能驱动的 H2O2 生产的高效 Z 方案系统提供了一种策略。
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Synergy of charge migration direction-manipulated Z-scheme heterojunction of BiVO4 quantum dots/perylenetetracarboxylic acid and nanosized Au modification for artificial H2O2 photosynthesis

Herein, perylenetetracarboxylic acid (PTA) nanosheets with anisotropic charge migration driven by the formed internal electric fields are synthesized through a facile hydrolysis-reassembly process. Strategically, a Z-scheme heterojunction with free-flowing interfacial charge transfer and spatially separated redox centers is constructed based on the distinct photogenerated electrons and holes accumulation regions of PTA nanosheets by in-situ introducing BiVO4 quantum dots (BQD) and nanosized Au. The optimized BQD/PTA-Au exhibits a ca. 6.4-fold and 4.8-fold enhancement in H2O2 production rate and apparent quantum yield at 405 nm compared with pristine PTA, respectively. The exceptional activities are attributed to the cascade Z-scheme charge transfer followed the matched charge migration orientation, as well as the Au active sites for accelerating 2e oxygen reduction pathway induced by superoxide radicals, as unraveled by electron paramagnetic resonance, in-situ irradiated X-ray photoelectron spectroscopy and in-situ diffuse reflectance infrared Fourier transformation spectroscopy. This work provides a strategy to design an efficient Z-scheme system towards solar-driven H2O2 production.

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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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