Ligand-induced reaction mechanism regulation on Sr/Nb2O5 for high-efficiency selective photocatalytic NO oxidation

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2023.123688

Tianjiao Wu , Bibo Ma , Huanhuan Bai , Lin Wang , Yumei Zhang , Qingzhi Luo , Jing An , Huiying Mu , Desong Wang , Yandong Duan

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Abstract

Developing highly efficient photocatalysts that selectively convert NO pollutants to NO₃¯ while storing metabolic nitrogen for crops remains a great challenge. Simultaneously, there is a dearth of research investigating the relationship between the chemical environment and the activity of catalytic sites. Herein, an efficient impregnation approach to access atomically dispersed Sr single atoms supported on Nb₂O₅ is reported; meanwhile, various ligands (-Cl, -Br, -OH) are employed to customize the local structure. The results show that Cl-Sr/Nb₂O₅ exhibits excellent catalytic performance in eliminating NO, which is significantly superior to other catalysts. The introduction of Sr atom and ligand increases the energy barrier of NO₂ formation, thus improving the selectivity of converting NO to NO₃¯. This study highlights the importance of precisely designing the catalytic site at the atomic level, and the obtained insights may serve as a valuable guide for developing future catalyst designs.

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Sr/Nb2O5 上配体诱导的反应机制调节，实现高效选择性光催化氧化 NO

开发高效光催化剂，选择性地将 NO 污染物转化为 NO3'，同时为农作物储存代谢氮，仍然是一项巨大的挑战。与此同时，有关化学环境与催化位点活性之间关系的研究也十分匮乏。本文报告了一种高效的浸渍方法，以获得支撑在 Nb2O5 上的原子分散的 Sr 单原子；同时，还采用了各种配体（-Cl、-Br、-OH）来定制局部结构。结果表明，Cl-Sr/Nb2O5 在消除 NO 方面表现出优异的催化性能，明显优于其他催化剂。Sr 原子和配体的引入增加了 NO2 形成的能垒，从而提高了将 NO 转化为 NO3¯ 的选择性。这项研究强调了在原子水平上精确设计催化位点的重要性，所获得的见解可作为开发未来催化剂设计的宝贵指导。

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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.