Reverse oxygen spillover triggered by CO adsorption on Sn-doped Pt/TiO₂ for low-temperature CO oxidation.

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2023-06-13 DOI:10.1038/s41467-023-39226-6

Jianjun Chen, Shangchao Xiong, Haiyan Liu, Jianqiang Shi, Jinxing Mi, Hao Liu, Zhengjun Gong, Laetitia Oliviero, Françoise Maugé, Junhua Li

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引用次数: 2

Abstract

The spillover of oxygen species is fundamentally important in redox reactions, but the spillover mechanism has been less understood compared to that of hydrogen spillover. Herein Sn is doped into TiO₂ to activate low-temperature (<100 °C) reverse oxygen spillover in Pt/TiO₂ catalyst, leading to CO oxidation activity much higher than that of most oxide-supported Pt catalysts. A combination of near-ambient-pressure X-ray photoelectron spectroscopy, in situ Raman/Infrared spectroscopies, and ab initio molecular dynamics simulations reveal that the reverse oxygen spillover is triggered by CO adsorption at Pt²⁺ sites, followed by bond cleavage of Ti-O-Sn moieties nearby and the appearance of Pt⁴⁺ species. The O in the catalytically indispensable Pt-O species is energetically more favourable to be originated from Ti-O-Sn. This work clearly depicts the interfacial chemistry of reverse oxygen spillover that is triggered by CO adsorption, and the understanding is helpful for the design of platinum/titania catalysts suitable for reactions of various reactants.

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锡掺杂Pt/TiO2上CO吸附引发的低温CO氧化反氧溢出

氧的溢出在氧化还原反应中起着至关重要的作用，但与氢的溢出相比，人们对其溢出机制的了解较少。本文将Sn掺杂到TiO2中激活低温(2)催化剂，使得CO的氧化活性远远高于大多数氧化负载的Pt催化剂。近大气压x射线光电子能谱、原位拉曼/红外光谱和从头算分子动力学模拟的结合表明，氧的反向溢出是由CO在Pt2+位点的吸附引发的，随后是附近Ti-O-Sn基团的键断裂和Pt4+物质的出现。催化不可缺少的Pt-O中的O在能量上更倾向于来自Ti-O-Sn。本工作清晰地描述了CO吸附引发的反氧溢出的界面化学，有助于设计适合各种反应物反应的铂/钛催化剂。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.