Role of point defects on the reactivity of reconstructed anatase titanium dioxide (001) surface.
Role of point defects on the reactivity of reconstructed anatase titanium dioxide (001) surface.
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点缺陷对重构锐钛矿型二氧化钛（001）表面反应性的影响
DOI：
10.1038/ncomms3214
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发表时间：
2013
影响因子：
16.6
通讯作者：
Hou, J. G.
中科院分区：
文献类型：
--
作者：
Wang, Yang;Sun, Huijuan;Tan, Shijing;Feng, Hao;Cheng, Zhengwang;Zhao, Jin;Zhao, Aidi;Wang, Bing;Luo, Yi;Yang, Jinlong;Hou, J. G.
二氧化钛（TiO2）不同表面的化学反应性是近几十年来广泛研究的课题。锐钛矿TiO2（001）及其（1 × 4）重构表面在理论上被认为是最具活性的，并受到合成化学家的大力研究。然而，缺乏直接的实验验证或确定这些表面上的活性位点引起了争议和争论。本文采用显微和光谱技术结合第一性原理计算对锐钛矿TiO2(001)-（1 × 4）表面进行了系统的研究。发现了两类本征点缺陷，其中只有还原表面的Ti3+缺陷位点表现出相当大的化学活性。完美的表面本身可以被充分氧化，但没有明显的活性。我们的研究结果表明，锐钛矿TiO2（001）表面的反应性应该取决于其还原状态，类似于金红石TiO2表面的反应性。理论表明锐钛矿（001）表面是二氧化钛所有晶体表面中催化活性最强的。Wang等人的研究表明，活性位点是四配位钛态，在没有它们的情况下，该表面在室温下对水的吸附甚至是惰性的。
The chemical reactivity of different surfaces of titanium dioxide (TiO2) has been the subject of extensive studies in recent decades. The anatase TiO2(001) and its (1 × 4) reconstructed surfaces were theoretically considered to be the most reactive and have been heavily pursued by synthetic chemists. However, the lack of direct experimental verification or determination of the active sites on these surfaces has caused controversy and debate. Here we report a systematic study on an anatase TiO2(001)-(1 × 4) surface by means of microscopic and spectroscopic techniques in combination with first-principles calculations. Two types of intrinsic point defects are identified, among which only the Ti3+ defect site on the reduced surface demonstrates considerable chemical activity. The perfect surface itself can be fully oxidized, but shows no obvious activity. Our findings suggest that the reactivity of the anatase TiO2(001) surface should depend on its reduction status, similar to that of rutile TiO2 surfaces. Theory suggests that the anatase (001) surface is the most catalytically reactive of all the crystal facets of titanium dioxide. Wang et al. show that the active sites are four-coordinated titanium states and in their absence this surface is even inert for water adsorption at room temperature.
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影响因子：
3.7
作者：
Lazzeri, M;Vittadini, A;Selloni, A
通讯作者：
Selloni, A
影响因子：
3.7
作者：
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作者：
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通讯作者：
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