Models of Active Sites in Supported Cu Metal Catalysts in 1,2-Dichloroethane Dechlorination. DFT Analysis Научная публикация
Журнал |
Journal of Structural Chemistry
ISSN: 0022-4766 , E-ISSN: 1573-8779 |
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Вых. Данные | Год: 2007, Том: 48, Номер: S7, Страницы: S160-S170 Страниц : 11 DOI: 10.1007/s10947-007-0159-9 | ||||
Ключевые слова | 1,2-dichloroethane, Active sites, Cu catalysts, Dechlorination, DFT calculations, Reaction mechanism | ||||
Авторы |
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Организации |
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Информация о финансировании (3)
1 | Сибирское отделение Российской академии наук | |
2 | United States Department of Energy | DE-AC03-76SF00098 |
3 | United States Department of Energy | DE-FG02-95ER14539 |
Реферат:
It is suggested that a set of discrete Cu nanoclusters satisfying the conditions of structural and electron stability should be used as models of active sites on supported metal catalysts. The close-packed Cu20 tetrahedral nanocluster that satisfies these two conditions was taken as a base model of active sites on supported copper catalysts. Theoretical analysis of two possible mechanisms of C-Cl bond dissociation of 1,2-dichloroethane on copper catalysts was performed by the density functional theory method. The first mechanism involves sequential splitting of C-Cl bonds in the molecule in three stages with further stabilization of chloroalkyl intermediates (stepwise mechanism). All these stages are activated. The limiting stage is the one that corresponds to dissociation of the first C-Cl bond with an activation energy of E# = 34.3 kcal/mol. The second mechanism corresponds to the simultaneous elimination of two chlorine atoms from 1,2-dichloroethane with liberation of ethylene in the phase; this is a one-stage process with an activation energy of E# = 26.1 kcal/mol (direct mechanism). A comparison of the two reaction routes shows that the direct mechanism is most probable on copper catalysts.
Библиографическая ссылка:
Avdeev V.I.
, Kovalchuk V.I.
, Zhidomirov G.M.
, d’Itri J.L.
Models of Active Sites in Supported Cu Metal Catalysts in 1,2-Dichloroethane Dechlorination. DFT Analysis
Journal of Structural Chemistry. 2007. V.48. NS7. P.S160-S170. DOI: 10.1007/s10947-007-0159-9 WOS Scopus РИНЦ
Models of Active Sites in Supported Cu Metal Catalysts in 1,2-Dichloroethane Dechlorination. DFT Analysis
Journal of Structural Chemistry. 2007. V.48. NS7. P.S160-S170. DOI: 10.1007/s10947-007-0159-9 WOS Scopus РИНЦ
Оригинальная:
Авдеев В.И.
, Ковальчук В.И.
, Жидомиров Г.М.
, Д'Итри Д.Л.
Модели активных центров металлических нанесенных Cu-катализаторов в реакции дехлорирования 1,2-дихлорэтана. Теоретический анализ методом DFT
Журнал структурной химии. 2007. Т.48. №7. С.S169-S179. RSCI РИНЦ
Модели активных центров металлических нанесенных Cu-катализаторов в реакции дехлорирования 1,2-дихлорэтана. Теоретический анализ методом DFT
Журнал структурной химии. 2007. Т.48. №7. С.S169-S179. RSCI РИНЦ
Даты:
Поступила в редакцию: | 7 нояб. 2006 г. |
Опубликована в печати: | 1 дек. 2007 г. |
Идентификаторы БД:
Web of science | WOS:000259612700013 |
Scopus | 2-s2.0-40249113336 |
РИНЦ | 14732945 |
Chemical Abstracts | 2008:1156965 |
Chemical Abstracts (print) | 150:97674 |
OpenAlex | W1973463436 |