Penta-coordinated aluminum species: Anchoring Au single atoms for photocatalytic CO2 reduction

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-06 DOI:10.1016/j.apcatb.2024.123703

Shaoqiang Li , Yi-lei Li , Hui-min Bai , Dong-ying Zhou , Ying Liu , Rui-hong Liu , Bao-hang Han , Xinying Liu , Fa-tang Li

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Abstract

Searching substrate materials having inherent photocatalytic activity and interaction with single atoms remains challenge. Herein, amorphous Al₂O₃ containing penta-coordinated aluminum (Al^V) species is synthesized using the solvothermal method and the Au single atom is anchored by Al^V via the self-reduction strategy. The Al-O bond energy is weakened by introducing amorphous components, which benefits the release of oxygen atoms and the resultant change of Al coordination environment to a Al^V species. The electron transfer between Al^V and Au stabilizes the Au single atom. The introduction of the Au single atom occupying the position of O vacancy and anchored by Al^V strengthened the chemical absorption abilities for CO_2, lowered the energy barrier of CO generation and promoted the charge separation efficiency. The CO generation rate of the Au single atom anchored obtains extraordinary promotion in comparison with pristine Al₂O₃, resulting in an approximately 6-fold enhancement and 98% product CO selectivity.

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五配位铝物种：锚定金单质原子，实现光催化二氧化碳还原

寻找具有固有光催化活性并能与单原子相互作用的基底材料仍是一项挑战。在此，我们采用溶热法合成了含有五配位铝（AlV）物种的无定形 Al2O3，并通过自还原策略将金单质原子锚定在 AlV 上。通过引入无定形成分，Al-O 键的能量被削弱，这有利于氧原子的释放以及由此产生的铝配位环境向 AlV 物种的转变。AlV 和 Au 之间的电子转移稳定了 Au 单原子。占据 O 空位的 Au 单原子的引入和 AlV 的锚定增强了对 CO2 的化学吸收能力，降低了 CO 生成的能垒，提高了电荷分离效率。与原始的 Al2O3 相比，锚定金单质原子的 CO 生成率得到了显著提高，提高了约 6 倍，CO 产物选择性达到 98%。

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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.