Engineering Pt single atom catalyst with abundant lattice oxygen by dual nanospace confinement strategy for the efficient catalytic elimination of VOCs

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2023.123687

Weigao Han , Weitong Ling , Peng Gao , Fang Dong , Zhicheng Tang

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Abstract

Precisely constructing Pt single atom catalyst (SACs) with fine-tuned chemical environments is a vitally challenging issue, which has attracted peoples’ attentions. The activation of lattice oxygen linked to active sites is also a great challenge to heterogeneous catalysis. Herein, via a cage-encapsulating strategy, Pt single atom (SA) was accurately constructed by dual nanospace confinement of three-dimensional ordered macroporous (3DOM) CeO₂ pore and Ce-MOFs nanocages. During calcination, CeO₂ derived from Ce-MOF restricted the migration of Pt SA and prevented its agglomeration. With the construction of CeO₂ nanocage, more active Pt-O₂ bond was created. More active lattice oxygen was linked to Pt single atom. DFT calculation also confirmed VOCs molecules were more easily absorbed on the catalyst surface and CO was more easily oxidized to CO₂. The 90% conversion temperature (T₉₀) of Pt₁/CeO₂ @CeO₂-0.2 (T₉₀ = 268 °C) was 81 °C lower than the T₉₀ of Pt₁/CeO₂ (T₉₀ = 349 °C) on the catalytic combustion of benzene.

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通过双纳米空间致密化策略制造具有丰富晶格氧的铂单原子催化剂，以高效催化消除挥发性有机化合物

精确构建具有微调化学环境的铂单原子催化剂（SACs）是一个极具挑战性的问题，备受人们关注。与活性位点相连的晶格氧的活化也是异相催化面临的巨大挑战。本文采用笼封策略，通过三维有序大孔（3DOM）CeO2孔和Ce-MOFs纳米笼的双重纳米空间限制，精确构建了铂单原子（SA）。在煅烧过程中，Ce-MOF 衍生的 CeO2 限制了铂金小原子的迁移，并防止其团聚。随着 CeO2 纳米笼的形成，产生了更活跃的铂-O2 键。更活跃的晶格氧与铂单原子相连。DFT 计算也证实，催化剂表面更容易吸收 VOCs 分子，CO 更容易氧化成 CO2。在苯的催化燃烧中，Pt1/CeO2@CeO2-0.2 的 90% 转化温度（T90）（T90 = 268 oC）比 Pt1/CeO2 的 T90（T90 = 349 oC）低 81 oC。

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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.