等离子体效应和肖特基结的协同作用有效促进 Bi4O5I2@Cu 光催化 CO2 还原,ACS Sustainable Chemistry & Engineering

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等离子体效应和肖特基结的协同作用有效促进 Bi4O5I2@Cu 光催化 CO2 还原
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-11-21 , DOI: 10.1021/acssuschemeng.3c06046
Qingling Huang ₁ , Jie Lin ₁ , Deshuai Yang ₂ , Yingfei Hu ₃ , Guobing Zhou ₁ , Wei Li ₂ , Jianqiang Hu _{1,

4} , Zhen Yang _{1,

4}

Affiliation

为了实现高效光催化CO ₂还原，在宽光谱范围内实现高效光吸收以及光生电子和空穴的快速分离至关重要。在此，我们通过将Cu纳米颗粒（NP）原位光沉积到由众多纳米片组装而成的Bi 4 O 5 I 2 微米花（MF）上来_合成Bi ₄ O ₅ I ₂ @Cu_光催化剂_。_{Bi 4} O ₅ I ₂ @Cu的分层杂化结合了两个独特的优点：Cu NPs诱导的表面等离子共振（SPR）效应和Bi ₄ O ₅ I ₂ /Cu肖特基结。具体来说，Cu NPs的SPR效应可以将光吸收范围拓宽至近红外，从而产生热电子。然后，其中一些热电子迁移穿过 Bi ₄ O ₅ I ₂ /Cu 的肖特基势垒，注入 Bi ₄ O ₅ I ₂ MF 的导带 (CB)。_{该过程增加了Bi 4} O ₅ I ₂ CB中的电子密度，有利于CO ₂光还原。另一方面，Bi ₄ O ₅ I ₂ /Cu肖特基异质结有效防止电子从Bi ₄ O ₅ I _{2回流到Cu，并促进光生空穴在Bi}₄ O ₅ I价带（VB）中的传输在密度泛函理论（DFT）计算的支持下，将₂转化为Cu NPs用于H _{2 O氧化，证实了电荷载流子的有效空间分离和迁移的实现。}在没有任何牺牲试剂的可见光照射下，具有最佳 Cu NP 负载的Bi ₄ O ₅ I _{2 @Cu-0.5 表现出显着提高的 CO 产率，达到 7.34 μmol g}^–1 h ^–1，大约是 13.1 倍其性能优于裸 Bi ₄ O ₅ I ₂ MF，并且也超过了最报道的基于卤氧化铋和基于等离子体激元的光催化剂。因此，这项工作为协同利用等离子体效应和肖特基结来开发优异的光催化剂提供了新的策略。

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Synergism of the Plasmonic Effect and Schottky Junction to Effectively Facilitate Photocatalytic CO2 Reduction of Bi4O5I2@Cu

To achieve highly efficient photocatalytic CO₂ reduction, it is crucial to attain efficient light absorption across a wide spectral range and rapid separation of photogenerated electrons and holes. Herein, we synthesize a Bi₄O₅I₂@Cu photocatalyst by the in situ photodeposition of Cu nanoparticles (NPs) onto Bi₄O₅I₂ micron flowers (MFs) assembled from numerous nanosheets. The hierarchical hybrid of Bi₄O₅I₂@Cu combines two distinct merits: the surface plasmon resonance (SPR) effect induced by Cu NPs and the Bi₄O₅I₂/Cu Schottky junction. Specifically, the SPR effect of Cu NPs can broaden the range of light absorption to the near-infrared, resulting in the generation of hot electrons. Some of these hot electrons then migrate across the Schottky barrier of Bi₄O₅I₂/Cu, injecting into the conduction band (CB) of Bi₄O₅I₂ MFs. This process increases the electron density in the CB of Bi₄O₅I₂, which is beneficial for the CO₂ photoreduction. On the other hand, the Bi₄O₅I₂/Cu Schottky heterojunction effectively prevents the electron backflow from Bi₄O₅I₂ to Cu and facilitates the transfer of photogenerated holes in the valence band (VB) of Bi₄O₅I₂ into Cu NPs for H₂O oxidation, as supported by density functional theory (DFT) calculations, confirming the achievement of efficient spatial separation and migration of charge carriers. Under visible light irradiation without any sacrificial reagent, Bi₄O₅I₂@Cu-0.5 with an optimal loading of Cu NPs demonstrates a significantly enhanced CO production rate of 7.34 μmol g^–1 h^–1, which is approximately 13.1 times higher than that of the bare Bi₄O₅I₂ MFs and also surpasses those of the most reported bismuth oxyhalide-based and plasmon-based photocatalysts. Therefore, this work offers a new strategy for the development of excellent photocatalysts by the synergistic utilization of the plasmonic effect and Schottky junction.

更新日期：2023-11-21

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