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High Photoreactivity on a Reconstructed Anatase TiO2(001) Surface Predicted by Ab Initio Nonadiabatic Molecular Dynamics
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2022-06-20 , DOI: 10.1021/acs.jpclett.2c01417 Youyou Tu 1 , Weibin Chu 2 , Yongliang Shi 3 , Wenguang Zhu 1 , Qijing Zheng 1 , Jin Zhao 1, 1, 4
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2022-06-20 , DOI: 10.1021/acs.jpclett.2c01417 Youyou Tu 1 , Weibin Chu 2 , Yongliang Shi 3 , Wenguang Zhu 1 , Qijing Zheng 1 , Jin Zhao 1, 1, 4
Affiliation
Anatase TiO2(001) surface with (4 × 1) reconstruction is proposed to be a highly active catalytic surface. In this work, using time-domain ab initio nonadiabatic molecular dynamics, we reveal that the ridge structure formed by anatase(001) surface reconstruction is the photoreactive site for hole migration and trapping. Moreover, the ridge structure is destroyed by low-coverage CH3OH adsorption, leading to the suppression of its high photoreactivity. However, when the CH3OH coverage is increased and intermolecular hydrogen bonds (H-bonds) form, the ridge structure and its high photoreactivity are restored. Furthermore, the hole trapping dynamics is strongly coherent with intermolecular proton transfer in structures with intermolecular H-bonds. Our study proves that anatase TiO2(001)-(4 × 1) is a highly photoreactive surface where the ridge is the photoreactive site for hole trapping, which is coherent with the proton transfer process.
中文翻译:
Ab Initio 非绝热分子动力学预测的重建锐钛矿 TiO2(001) 表面的高光反应性
具有(4×1)重建的锐钛矿TiO 2(001)表面被认为是一种高活性催化表面。在这项工作中,我们利用时域从头算非绝热分子动力学,揭示了锐钛矿(001)表面重建形成的脊结构是空穴迁移和捕获的光反应位点。此外,低覆盖率的 CH 3 OH 吸附破坏了脊结构,导致其高光反应性受到抑制。然而,当 CH 3OH 覆盖率增加并形成分子间氢键 (H-bonds),恢复脊结构及其高光反应性。此外,空穴捕获动力学与分子间氢键结构中的分子间质子转移密切相关。我们的研究证明锐钛矿型 TiO 2 (001)-(4 × 1) 是一种高度光反应性表面,其中脊是空穴捕获的光反应性位点,与质子转移过程相一致。
更新日期:2022-06-20
中文翻译:
Ab Initio 非绝热分子动力学预测的重建锐钛矿 TiO2(001) 表面的高光反应性
具有(4×1)重建的锐钛矿TiO 2(001)表面被认为是一种高活性催化表面。在这项工作中,我们利用时域从头算非绝热分子动力学,揭示了锐钛矿(001)表面重建形成的脊结构是空穴迁移和捕获的光反应位点。此外,低覆盖率的 CH 3 OH 吸附破坏了脊结构,导致其高光反应性受到抑制。然而,当 CH 3OH 覆盖率增加并形成分子间氢键 (H-bonds),恢复脊结构及其高光反应性。此外,空穴捕获动力学与分子间氢键结构中的分子间质子转移密切相关。我们的研究证明锐钛矿型 TiO 2 (001)-(4 × 1) 是一种高度光反应性表面,其中脊是空穴捕获的光反应性位点,与质子转移过程相一致。