Pd(111)和M/Pd(111)(M=Ni,Cu,Ru)上糠醛分子吸附及脱碳反应的理论研究

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摘要

By performing with density functional theory (DFT) method, the detailed adsorption process and the catalytic decarbonylation mechanisms of furfural over Pd(111) and M/Pd(111) (M = Ni, Cu, Ru) surfaces toward furan were clarified. The results of atomic size factor, formation energy and d-band center showed that Ru/Pd(111) surface was the most stable and active. The adsorption energies of furfural on the different surfaces followed the order Ru/Pd(111) > Cu/Pd(111) > Pd(111) ˃ Ni/Pd(111). After analyzing Mulliken atomic charge population and the deformation density, we can find that on Ru/Pd(111) surface, the number of charge transfer was the most and the interaction was the strongest. Therefore, its adsorption energy was the highest. Furthermore, the furfural decarbonylation pathway is more kinetically feasible on bimetallic surface, and the reaction is the most likely to occur on Ru/Pd(111).

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	夏盛杰
	方镭
	钱梦丹
	孟跃
	倪哲明

关键词 ： density functional theory, furfural, Pd(111), bimetallic catalyst, adsorption, decarbonylation mechanism

Abstract：

利用密度泛函理论(DFT)研究了Pd(111)面和M/Pd(111)(M=Ni,Cu,Ru)面上糠醛的吸附过程及其转化为呋喃的脱碳机理。通过分析原子尺寸因素、结合能和d带中心，发现Ru/Pd(111)面最为稳定且活性较优。糠醛在不同表面吸附能的排序为Ru/Pd(111) > Cu/Pd(111) > Pd(111) ˃ Ni/Pd(111)。分析密立根电荷得到Ru/Pd(111)面与糠醛分子之间存在强烈的相互作用且转移电荷较多，故吸附能最大。在合金表面上糠醛脱碳反应具有动力学可行性，且Ru/Pd(111)面对糠醛脱碳催化活性最优。

Key words： density functional theory furfural Pd(111) bimetallic catalyst adsorption decarbonylation mechanism

收稿日期: 2018-05-02 出版日期: 2019-01-24

基金资助:

This work was supported by the National Natural Science Foundation of China (No. 21503188).

通讯作者: jchx@zjut.edu.cn E-mail: jchx@zjut.edu.cn

引用本文:

夏盛杰;方镭;钱梦丹;孟跃;倪哲明. Pd(111)和M/Pd(111)(M=Ni,Cu,Ru)上糠醛分子吸附及脱碳反应的理论研究[J]. 结构化学, 2019, 38(2): 211-223.
XIA Sheng-Jie;FANG Lei;pQIAN Meng-Dan;MENG Yue;NI Zhe-Ming. Adsorption and Decarbonylation Reaction of Furfural on the Pd(111) and M/Pd(111)(M = Ni, Cu and Ru) Surfaces. CHINESE JOURNAL OF STRUCTURAL CHEMISTRY, 2019, 38(2): 211-223.

链接本文:

http://manu30.magtech.com.cn/jghx/CN/ 或 http://manu30.magtech.com.cn/jghx/CN/Y2019/V38/I2/211

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