异质结构增强的单原子钯催化剂的金属-负载相互作用使CO和VOC氧化的氧活化效率提高

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-09-05 DOI:10.1016/j.apcatb.2023.122753

Bin Wang , Qilei Yang , Bing Li , Hongyuan Ma , Yue Xuan , Chuan Gao , Yanjie Liang , Kaihang Zhang , Qiaowan Chang , Osvaldo Broesicke , Houlin Wang , Dong Wang , Tao Luan , Kuihua Han , Chunmei Lu , John Crittenden

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引用次数: 5

摘要

空气污染物的催化氧化依赖于活性氧的种类，这需要对负责氧活化的活性位点有深入的了解。在这项研究中，我们利用异质结构载体(ZnMn2O4@MnO2)来调节单原子钯催化剂中的金属-载体相互作用(msi)，实现了吸附氧(Oads)和晶格氧(Olatt)的有效活化。具体而言，定制的msi诱导了CO氧化的有效氧化还原对pd103和pd105，促进O2对Oads的活化，从而在室温下实现90%的CO转化率，并形成了一种新的“mvk诱导L-H”反应机制。此外，定制的msi诱导了Mn-O键的拉伸，促进了Olatt参与甲苯氧化。我们的研究结果展示了一种在单原子催化剂(SACs)中调节msi的新方法，并强调了异质结构载体引入的强msi对氧活化的优越性。

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Heterostructure-strengthened metal-support interaction of single-atom Pd catalysts enabling efficient oxygen activation for CO and VOC oxidation

Catalytic oxidation of air pollutants depends on the active oxygen species, which requires a deep understanding of the active sites responsible for oxygen activation. In this study, we utilized a heterostructured support (ZnMn₂O₄@MnO₂) to modulate the metal-support interactions (MSIs) in single-atom Pd catalysts, achieving efficient activation of both adsorbed oxygen (O_ads) and lattice oxygen (O_latt). Specifically, the tailored MSIs induced an efficient redox pair for CO oxidation, i.e., Pd₁O₃ and Pd₁O₅, promoting the activation of O₂ to O_ads, which led to 90% CO conversion at room temperature and a novel “MvK-induced L-H” reaction mechanism. Moreover, the tailored MSIs induced the stretching of the Mn-O bond, facilitating the participation of O_latt in toluene oxidation. Our results demonstrate a novel approach to modulating MSIs in single-atom catalysts (SACs) and highlight the superiority of the strong MSIs introduced by heterostructured supports for oxygen activation.

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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.