Interfacial electron interactions governed photoactivity and selectivity evolution of carbon dioxide photoreduction with spinel cobalt oxide based hollow hetero-nanocubes

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-06 DOI:10.1016/j.apcatb.2024.123705

Chao Cheng , Hengyue Xu , Maomao Ni , Changfa Guo , Yuanyuan Zhao , Yong Hu

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Abstract

In this work, an efficient CO₂ photoreduction catalyst based on Co₃O₄/ZnIn₂S₄ hollow hetero-nanocubes is precisely constructed via an in-situ transformation of cobalt-organic framework followed by a solvothermal reaction. Comprehensive in-situ spectroscopic analyses and theoretical calculations have revealed that the critical interfacial electron interactions (IEIs) effects on both photoactivity evolution and selectivity modulation in the Co₃O₄/ZnIn₂S₄ hetero-structure. As the content of ZnIn₂S₄ increases in the hetero-structure, the photoactivity exhibits a volcano-like evolution profile but the CH₄ selectivity reduces monotonously. The improved photoactivity is attributed to the IEIs-promoted charge separation as well as the specific-surface-area effect in terms of electron unitization rate, and the electronic structure of Co₃O₄ is tuned and the energy barrier for the key reaction intermediate *CHO is reduced, leading to improved CH₄ selection in comparison with bare Co₃O₄. The IEIs-mediated production selectivity is further verified by a Co₃O₄/CeO₂ heterojunction, indicating a certain universality of the IEI effect.

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基于尖晶石氧化钴的空心异质纳米管在二氧化碳光电还原过程中受界面电子相互作用影响的光活性和选择性演化

在这项工作中，通过钴有机框架的原位转化和溶热反应，精确地构建了一种基于 Co3O4/ZnIn2S4 空心异质纳米管的高效二氧化碳光还原催化剂。全面的原位光谱分析和理论计算揭示了临界界面电子相互作用（IEIs）对 Co3O4/ZnIn2S4 异质结构中光活性演变和选择性调节的影响。随着异质结构中 ZnIn2S4 含量的增加，光活度呈现出类似火山喷发的演化曲线，但 CH4 选择性却单调降低。与裸 Co3O4 相比，光活性的提高归因于 IEIs 促进的电荷分离以及电子单元化率方面的比表面效应，而且 Co3O4 的电子结构得到调整，关键反应中间体 *CHO 的能垒降低，从而提高了对 CH4 的选择性。Co3O4/CeO2 异质结进一步验证了 IEIs 介导的生产选择性，表明 IEI 效应具有一定的普遍性。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.