Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces | |
Wang, Zhiguo ; Wang, Honglun ; Liu, Yonjun ; Suo, Yourui | |
刊名 | JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM ; Wang Zhiguo,Wang Honglun,Liu Yonjun,Suo Yourui. Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces.JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM,2008,850(1-3):72-78 |
2008-02-15 | |
英文摘要 | In this paper, the reactions of nitrone, N-methyl nitrone, N-phenyl nitrone and their hydroxylamine tautomers (vinyl-hydroxylamine, N-methyl-vinyl-hydroxylamine and N-phenyl-vinyl-hydroxylamine) on the reconstructed C(100)-2 x 1 surface have been investigated using hybrid density functional theory (B3LYP), Moller-Plesset second-order perturbation (MP2) and multi-configuration complete-active-space self-consistent-field (CASSCF) methods. The calculations showed that all the nitrones can react with the surface "dimer" via facile 1.3-dipolar cycloaddition with small activation barriers (less than 12.0 kJ/mol at B3LYP/6-31g(d) level). The [2+2] cycloaddition of hydroxylamine tautomers on the C(100) surface follows a diradical mechanism. Hydroxylamine tautomers first form diradical intermediates with the reconstructed C(I 00)-2 x I surface by overcoming a large activation barrier of 50-60 kJ/mol (B3LYP), then generate [2+2] cycloaddition products via diradical transition states with negligible activation barriers. The surface reactions result in hydroxyl or amino-terminated diamond surfaces, which offers new opportunity for further modifications. (C) 2007 Elsevier B.V. All rights reserved.; In this paper, the reactions of nitrone, N-methyl nitrone, N-phenyl nitrone and their hydroxylamine tautomers (vinyl-hydroxylamine, N-methyl-vinyl-hydroxylamine and N-phenyl-vinyl-hydroxylamine) on the reconstructed C(100)-2 x 1 surface have been investigated using hybrid density functional theory (B3LYP), Moller-Plesset second-order perturbation (MP2) and multi-configuration complete-active-space self-consistent-field (CASSCF) methods. The calculations showed that all the nitrones can react with the surface "dimer" via facile 1.3-dipolar cycloaddition with small activation barriers (less than 12.0 kJ/mol at B3LYP/6-31g(d) level). The [2+2] cycloaddition of hydroxylamine tautomers on the C(100) surface follows a diradical mechanism. Hydroxylamine tautomers first form diradical intermediates with the reconstructed C(I 00)-2 x I surface by overcoming a large activation barrier of 50-60 kJ/mol (B3LYP), then generate [2+2] cycloaddition products via diradical transition states with negligible activation barriers. The surface reactions result in hydroxyl or amino-terminated diamond surfaces, which offers new opportunity for further modifications. (C) 2007 Elsevier B.V. All rights reserved. |
内容类型 | 期刊论文 |
源URL | [http://ir.nwipb.ac.cn/handle/363003/1229] |
专题 | 西北高原生物研究所_中国科学院西北高原生物研究所 |
推荐引用方式 GB/T 7714 | Wang, Zhiguo,Wang, Honglun,Liu, Yonjun,et al. Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces[J]. JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM, Wang Zhiguo,Wang Honglun,Liu Yonjun,Suo Yourui. Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces.JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM,2008,850(1-3):72-78,2008. |
APA | Wang, Zhiguo,Wang, Honglun,Liu, Yonjun,&Suo, Yourui.(2008).Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces.JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM. |
MLA | Wang, Zhiguo,et al."Addition reactions of nitrones on the reconstructed C(100)-2 x 1 surfaces".JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM (2008). |
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