表面氯原子对光催化CO2还原中电荷分布和反应势垒的影响

IF 9.9 2区 材料科学 Q1 Engineering
Wendong Zhang , Wenjun Ma , Yuerui Ma , Peng Chen , Qingqing Ye , Yi Wang , Zhongwei Jiang , Yingqing Ou , Fan Dong
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引用次数: 0

摘要

光催化还原二氧化碳以生产高附加值的碳基燃料已被认为是缓解全球变暖问题的一种可行方法。然而,由于质子辅助多电子反应中涉及的传递过程动态缓慢,其转化效率和产物选择性仍然较低。降低中间产物的形成能垒是提高最终产物选择性和生产率的有效方法。在本研究中,我们旨在通过掺杂表面氯原子来调节 Bi2WO6 的表面电子结构,从而实现有效的光催化二氧化碳还原。表面氯原子可增强光的吸收能力,影响其能带结构,促进电荷分离。结合 DFT 计算发现,表面 Cl 原子不仅能改变表面电荷分布,从而影响 H2O 和 CO2 的竞争吸附,还能降低中间产物的形成能垒,生成更多的 ∗COOH 中间产物,从而促进 CO 的生成。总之,本研究展示了一种很有前景的表面卤化策略,可提高层状结构 Bi 基催化剂的光催化 CO2 还原活性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Effects of surface chlorine atoms on charge distribution and reaction barriers for photocatalytic CO2 reduction

Photocatalytic CO2 reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues. However, the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions. Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products. In this study, we aim to regulate the surface electronic structure of Bi2WO6 by doping surface chlorine atoms to achieve effective photocatalytic CO2 reduction. Surface Cl atoms can enhance the absorption ability of light, affect its energy band structure and promote charge separation. Combined with DFT calculations, it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H2O and CO2, but also lower the formation energy barrier of intermediate products to generate more intermediate ∗COOH, thus facilitating CO production. Overall, this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO2 reduction activity of a layered structure Bi-based catalyst.

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来源期刊
Nano Materials Science
Nano Materials Science Engineering-Mechanics of Materials
CiteScore
20.90
自引率
3.00%
发文量
294
审稿时长
9 weeks
期刊介绍: Nano Materials Science (NMS) is an international and interdisciplinary, open access, scholarly journal. NMS publishes peer-reviewed original articles and reviews on nanoscale material science and nanometer devices, with topics encompassing preparation and processing; high-throughput characterization; material performance evaluation and application of material characteristics such as the microstructure and properties of one-dimensional, two-dimensional, and three-dimensional nanostructured and nanofunctional materials; design, preparation, and processing techniques; and performance evaluation technology and nanometer device applications.
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