乙炔在Ge(001)表面吸附的反应路径

引用本文: 范晓丽, 刘燕, 刘崇, 刘焕明. 乙炔在Ge(001)表面吸附的反应路径[J]. 物理化学学报, 2012, 28(05): 1107-1112. doi: 10.3866/PKU.WHXB201203011 shu

Citation: FAN Xiao-Li, LIU Yan, LIU Chong, LAU Woon-Ming. Reaction Pathways of Acetylene Adsorption on the Ge(001) Surface[J]. Acta Physico-Chimica Sinica, 2012, 28(05): 1107-1112. doi: 10.3866/PKU.WHXB201203011 shu

乙炔在Ge(001)表面吸附的反应路径

基金项目:
国家自然科学基金(20903075) (20903075)

高等学校学科创新引智计划(111) (B08040)资助项目 (111) (B08040)

摘要: 采用第一性原理方法研究了乙炔分子在Ge(001)表面的吸附反应. 通过系统考察0.5 和1.0 ML覆盖度时形成di-σ和end-bridge构型的反应路径, 研究在表面形成di-σ和paired-end-bridge 构型的反应几率. 除了表面反应以外, 本文还涉及了亚表层Ge 原子参与的吸附反应, 乙炔在亚表层原子上吸附形成的亚稳态结构sub-di-σ, 是形成end-bridge 结构的第二条途径, 此反应机理对于表面吸附结构的形成起重要的作用. 与乙炔分子不同的是, 表面以下原子参与时乙烯分子的吸附反应为吸热反应. 综合热力学和动力学的分析表明,paired-end-bridge 构型是乙炔分子吸附的主要构型, 此结论解释了乙炔分子在Ge(001)表面吸附构型的实验结果. 对于乙烯和乙炔两分子在Ge(001)表面吸附的分析比较揭示了导致两者之间差异的原因.

关键词:

English

Reaction Pathways of Acetylene Adsorption on the Ge(001) Surface

1.
1. School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an 710072, P. R. China;
2. Beijing Computational Science Research Center, Beijing 100084, P. R. China;
3. Chengdu Green Energy and Green Manufacturing Technology Research and Development Center, Chengdu 610207, P. R. China
Received Date: 12 December 2011
Available Online: 26 April 2012
Fund Project:
国家自然科学基金(20903075)

高等学校学科创新引智计划(111) (B08040)资助项目

Abstract: The adsorption reaction of acetylene on the Ge(001) surface is investigated by first-principles calculations. In order to understand the relative populations of the di-σ and paired-end-bridge structures, we calculated the adsorption reaction paths leading to their formation at 0.5 and 1.0 ML coverage. More importantly, we studied the adsorption channel involving sublayer Ge atoms by forming a metastable subdi- σ structure. This sub-di-σ structure represents second reaction pathway that results in the end-bridge structure, which plays an important role in the formation of the adsorption configurations. In contrast to C₂H₂, the adsorption of C₂H₄ on the Ge(001) surface involving subsurface Ge atoms, is endothermic. Our calculations show from both kinetic and thermodynamic standpoints that the paired-end-bridge structure is the primary adsorption configuration that explains the experimental observations. Our work also helps to understand the fundamental differences between the adsorption of C₂H₂ and C₂H₄ on the Ge(001) surface.

Key words:

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乙炔在Ge(001)表面吸附的反应路径

English

Reaction Pathways of Acetylene Adsorption on the Ge(001) Surface

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

乙炔在Ge(001)表面吸附的反应路径

English

Reaction Pathways of Acetylene Adsorption on the Ge(001) Surface

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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