Energetics of C-N coupling reactions on Pt(111) and Ni(111) surfaces from application of density-functional theory

Wei Jia Chen, Chen Hao Yeh, Chun Chih Chang, Jia-Jen Ho*

*此作品的通信作者

研究成果: 雜誌貢獻期刊論文同行評審

3 引文 斯高帕斯(Scopus)

摘要

We applied density-functional theory (DFT) with the projector-augmented- wave method (PAW) to investigate systematically the energetics of C-N coupling reactions on Pt(111) and Ni(111)surfaces. Our approach includes several steps: the adsorption of reactants and products (CHx, NHy and CHxNHy, x = 0-3, y = 0-2), movement of molecular fragments on the surface, and then C-N coupling. According to our calculations, the energies (ignoring the conventional negative sign) of adsorption of CH x and NHy on Pt(111)/Ni(111) surfaces decrease in the order C > CH > CH2 > CH3 and N > NH > NH2, with values 7.41/6.91, 6.97/6.52, 4.58/4.39, 2.19/2.01 eV and 5.10/5.49, 4.12/4.79, 2.75/2.87 eV, respectively. Regarding the adsorption energies among CHxNHy, the adsorption energy of CNH 2 species is the highest on the Pt(111) surface, whereas on the Ni(111) surface CH3N is the most stable. The C-N coupling barriers differ on the two metallic surfaces despite the structures of initial, transition and final states being similar. On the Pt(111) surface, the coupling reaction of CH2 + NH2 has the smallest barrier, whereas CH + NH2 is the most favorable on the Ni(111) surface. The detailed local density of states (LDOS) and electron-localization functions (ELF) were investigated to rationalize the calculated outcomes.

原文英語
頁(從 - 到)10395-10401
頁數7
期刊Physical Chemistry Chemical Physics
15
發行號25
DOIs
出版狀態已發佈 - 2013 七月 7

ASJC Scopus subject areas

  • 物理與天文學 (全部)
  • 物理與理論化學

指紋

深入研究「Energetics of C-N coupling reactions on Pt(111) and Ni(111) surfaces from application of density-functional theory」主題。共同形成了獨特的指紋。

引用此