二维表面扭曲增强电子自由度,实现高效的高级氧化过程

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL
Ximeng Xu , Shujing Zhang , Yuhao Wang , Nana Wang , Qinli Jiang , Xiaohong Liu , Qingqing Guan , Wei Zhang
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引用次数: 0

摘要

为设计有效的富电子催化剂中心而进行的二维(2D)表面工程在操纵催化行为和活性方面至关重要,但仍然具有挑战性。在这里,我们成功地扭曲了二维层状 FeOCl 的表面,实现了对其铁位点的目标微调。所获得的新催化剂能以更低的能障促进过一硫酸盐对活性物种的活化,并高效氧化目标有机物,其反应动力学比原始的 FeOCl 快近 41 个数量级。Fe位点周围电子自由度的增加被认为是关键的驱动因素。铁周围扭曲的几何结构增加了电荷分布的极化,使电子价云的对称性降低,电子迁移率提高。因此,扭曲表面大大增强了铁基点与缺电子的过一硫酸盐之间的界面电荷转移。这项工作强调了扭曲表面结构的概念,以实现高效的高级氧化催化剂设计。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

2D surfaces twisted to enhance electron freedom toward efficient advanced oxidation processes

2D surfaces twisted to enhance electron freedom toward efficient advanced oxidation processes

Two-dimensional (2D)-interface engineering for designing effective electron-rich catalyst center is pivotal in manipulating the catalytic behaviors and activity, but still challenging. Here, we’ve successfully twisted the surfaces of the 2D layered FeOCl, fulfilling the targeted fine-tuning of its Fe sites. The obtained new catalyst can boost peroxymonosulfate activation for reactive species with much lower energy barriers and efficiently oxidized target organic with almost 41 orders of magnitude faster reaction kinetics than pristine FeOCl. The increased degree of freedom of electron around Fe site has been identified as the key driver. The distorted geometry structure around Fe has led to an increased polarization of charge distribution, associating with less symmetric electron valence cloud and higher electron mobility. Thus, the twisted surfaces enable a much enhanced interfacial charge transfer between Fe site and the electron-deficient peroxymonosulfate. This work highlights the concept of twisted surface construction toward efficient advanced oxidation catalyst design.

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来源期刊
Applied Catalysis B: Environmental
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.
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