Dynamic Cu/Zn Interaction in SiO2 Supported Methanol Synthesis Catalysts Unraveled by in Situ XAFS Научная публикация
Журнал |
The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455 |
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Вых. Данные | Год: 2011, Том: 115, Номер: 41, Страницы: 20175-20191 Страниц : 17 DOI: 10.1021/jp201839s | ||||||||
Ключевые слова | Absorption spectroscopy; Calcination; Catalyst activity; Copper; Methanol; Phase interfaces; Silica; Silicon compounds; Synthesis gas manufacture; Ternary systems; Zinc; Zinc oxide | ||||||||
Авторы |
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Организации |
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Информация о финансировании (2)
1 | Netherlands Organisation for Scientific Research | 047.005.03.96 |
2 | Netherlands Organisation for Scientific Research | 047.015.004 |
Реферат:
In situ X-ray absorption spectroscopy XAFS at the Cu and Zn K-edge has been used to unravel the Cu/Zn interaction and identify the possible active site of Cu-based methanol synthesis catalysts in the Cu/ZnO/SiO2 ternary system. These highly dispersed silica supported catalysts, whose activity increases sharply as a function of the reduction temperature, were studied calcined, reduced at 200, 300, and 400 C, and for each reduction temperature under passivation/rereduction and methanol synthesis conditions. Results showed that the calcined form consists mainly of a mixed Cu/Zn hydrosilicate that is progressively transformed as the reduction temperature increases into (i) Cu metal particles, (ii) increasingly dispersed ZnO species on SiO2, and (iii) finally a Zn metallic phase forming segregated bimetallic CuZn α-brass alloy particles. These different structures and Cu/Zn interfaces may correspond to different active phases and activities in methanol synthesis. After reduction at 200 and 300 C, Cu0 is likely composing most of the active phase, whereas above 300 C, the sharp increase in the number Zn0-based sites formed as a function of
the reduction temperature could explain the major role played by this parameter in controlling the activity of these catalysts. The dynamic Cu/Zn interaction as a function of the temperature and gas environment pointed out in this ternary system may be at the origin of the existence of different and sometimes contradictory models to account for the mechanisms of the methanol synthesis.
Библиографическая ссылка:
Grandjean D.
, Pelipenko V.
, Batyrev E.D.
, Heuvel J.C.v.d.
, Khassin A.A.
, Yurieva T.M.
, Weckhuysen B.M.
Dynamic Cu/Zn Interaction in SiO2 Supported Methanol Synthesis Catalysts Unraveled by in Situ XAFS
The Journal of Physical Chemistry C. 2011. V.115. N41. P.20175-20191. DOI: 10.1021/jp201839s WOS Scopus РИНЦ
Dynamic Cu/Zn Interaction in SiO2 Supported Methanol Synthesis Catalysts Unraveled by in Situ XAFS
The Journal of Physical Chemistry C. 2011. V.115. N41. P.20175-20191. DOI: 10.1021/jp201839s WOS Scopus РИНЦ
Файлы:
Полный текст от издателя
Даты:
Поступила в редакцию: | 24 февр. 2011 г. |
Принята к публикации: | 30 авг. 2011 г. |
Опубликована online: | 28 сент. 2011 г. |
Опубликована в печати: | 20 окт. 2011 г. |
Идентификаторы БД:
Web of science | WOS:000295700800018 |
Scopus | 2-s2.0-80054733622 |
РИНЦ | 18009759 |
Chemical Abstracts | 2011:1242681 |
Chemical Abstracts (print) | 155:546569 |
OpenAlex | W2158685795 |