利用内嵌电场调节Co3O4/ZnO异质结气凝胶,增强二氧化碳光还原到太阳能燃料。

IF 5.8 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Nanoscale Pub Date : 2025-06-26 DOI:10.1039/d5nr01315a
Wei Zhao,Sijia Ren,Yanfang Zheng,Yunlong Sun,Xiaodong Wu,Caiyue Liu,Jinpeng Shi,Kun Yang,Xiaobin Ma,Sheng Cui,Xiaodong Shen
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引用次数: 0

摘要

p - n型异质结具有良好的载流子分离效率、高稳定性和强氧化还原能力,有潜力成为高效的CO2还原光催化剂。本研究采用环氧丙烷开环诱导凝胶技术制备了一种新型的P-N Co3O4/ZnO异质结气凝胶光催化剂。所得的Co3O4/ZnO气凝胶具有相互连接的分层多孔结构,使其具有几十纳米左右的粒径和较大的bet比表面积,从而提供了丰富的暴露活性位点。在模拟太阳光谱条件下,在不添加牺牲剂和光敏剂的情况下,CH4和CO的产率分别可达18 μmol g-1 h-1和14.4 μmol g-1 h-1。这些数值分别是原始Co3O4气凝胶的12.0倍和5.8倍。基于密度泛函理论(DFT)计算,阐述了CO2在催化剂表面的活化机理。Co3O4/ZnO异质结形成后,CO2分子的C / O键长度分别从1.174和1.175 Å延长到1.376和1.259 Å,进一步证实了这一点,CO2吸附能更负。进一步研究表明,在异质结界面处形成的内嵌电场有效地促进了Co3O4导带中的电子与ZnO价带中的空穴的复合,显著提高了载流子分离效率,从而提高了CO2的光催化还原活性。这项工作不仅为设计高效的CO2还原光催化剂提供了新的策略,还将其影响扩展到推进气凝胶材料在光催化领域的应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Regulating a Co3O4/ZnO heterojunction aerogel with a built-in electric field for enhanced CO2 photoreduction to solar fuels from DFT insights.
P-N-type heterojunctions have the potential to serve as highly efficient photocatalysts for CO2 reduction, owing to their remarkable carrier separation efficiency, high stability, and strong redox capacity. In this study, a novel P-N Co3O4/ZnO heterojunction aerogel photocatalyst was fabricated through a process starting with the propylene oxide ring-opening-induced gelation technique. The resulting Co3O4/ZnO aerogel exhibits an interconnected, hierarchical porous structure, which endows it with a particle diameter size at around several tens of nanometers and a large BET-specific surface area, thereby providing abundant exposed active sites. Under simulated solar spectral conditions, the yields of CH4 and CO can attain 18 μmol g-1 h-1 and 14.4 μmol g-1 h-1, respectively, in the absence of any sacrificial agent and photosensitizer. These values are 12.0 times and 5.8 times higher than those of the pristine Co3O4 aerogel. Based on density functional theory (DFT) calculations, the activation mechanism of CO2 on the catalyst surface is illustrated. This is confirmed by the elongated CO bond length of the CO2 molecule from 1.174 and 1.175 Å to 1.376 and 1.259 Å, respectively, after forming the Co3O4/ZnO heterojunction, which is further confirmed by the more negative CO2 adsorption energy. Further research demonstrates that the built-in electric field formed at the heterojunction interface effectively promotes the recombination of electrons in the conduction band of Co3O4 with holes in the valence band of ZnO, significantly enhancing the carrier separation efficiency and thereby boosting the photocatalytic reduction activity of CO2. This work goes beyond providing new strategies for designing efficient CO2 reduction photocatalysts, extending its impact to advancing the utilization of aerogel materials in the field of photocatalysis.
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来源期刊
Nanoscale
Nanoscale CHEMISTRY, MULTIDISCIPLINARY-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
12.10
自引率
3.00%
发文量
1628
审稿时长
1.6 months
期刊介绍: Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.
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