操纵具有各种表面特征的原始无相钛白氧化物上的 H2O2 反应活性及其在氧化反应中的影响

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2024-11-12 DOI:10.1021/acs.jpclett.4c02742
Guohan Sun, Quan Wang, Yin-Song Liao, Yifan Cui, Linyuan Tian, Jyh-Pin Chou, Yufei Zhao, Yung-Kang Peng
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引用次数: 0

摘要

在涉及 H2O2 的反应中,无性氧化钛通常被用作催化剂/支持物,但人们对普通氧化钛表面与 H2O2 之间相互作用的了解仍然有限。在此,我们合成了具有 (101)、(001) 和氟修饰 (001) [F-(001)] 表面的定义明确的 TiO2 晶体,以研究表面特征(包括五配位 Ti (Ti5c) 位点的排列和氟的存在)如何影响 H2O2 的活化。我们的研究结果表明,这些表面特征极大地影响了吸附 H2O2 的理化性质。具体来说,与 (101) 和 (001) 表面相比,F-(001) 表面上的氟为 Ti5c-peroxo 物种引入了额外的氢键,从而改变了 H2O2 的电子结构。利用环己烯作为探针底物,我们成功地区分了 Ti5c 过氧化物的反应活性。F-(001)表面上的物种的活性明显高于(001)表面上的物种,而(101)表面上的物种的氧化活性几乎可以忽略不计。这些见解可指导设计用于 H2O2 相关反应的基于 TiO2 的催化剂。
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Manipulating the H2O2 Reactivity on Pristine Anatase TiO2 with Various Surface Features and Implications in Oxidation Reactions
Anatase TiO2 is commonly used as a catalyst/support in reactions involving H2O2, yet the understanding of interactions between common TiO2 surfaces and H2O2 remains limited. Herein, we synthesized well-defined TiO2 crystallites with (101), (001), and fluorine-modified (001) [F-(001)] surfaces to examine how surface features, including the arrangement of five-coordinated Ti (Ti5c) sites and the presence of fluorine, influence H2O2 activation. Our findings reveal that these surface features significantly affect the physiochemical properties of adsorbed H2O2. Specifically, fluorine on the F-(001) surface introduces an additional hydrogen bond to the Ti5c-peroxo species, altering the electronic structure of H2O2 compared to those with the (101) and (001) surfaces. Using cyclohexene as a probe substrate, we successfully distinguished the reactivities of the Ti5c-peroxo species. The activity of those on the F-(001) surface was significantly higher than the activity of those on the (001) surface, while the (101) surface showed negligible oxidation activity. These insights can guide the design of TiO2-based catalysts for H2O2-related reactions.
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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