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Reactivity of C 1 Surface Species Formed in Methane Activation on Zn‐Modified H‐ZSM‐5 Zeolite
Author(s) -
Wu Jian Feng,
Wang Wei David,
Xu Jun,
Deng Feng,
Wang Wei
Publication year - 2010
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201002258
Subject(s) - chemistry , catalysis , reactivity (psychology) , zeolite , inorganic chemistry , methyl formate , methanol , zinc , methane , formate , carbon monoxide , adsorption , organic chemistry , medicine , alternative medicine , pathology
Solid‐state 13 C magic angle spinning (MAS) NMR spectroscopy investigations identified zinc methyl species, formate species, and methoxy species as C 1 surface species formed in methane activation on the zeolite Zn/H‐ZSM‐5 catalyst at T ≤573 K. These C 1 surface species, which are possible intermediates in further transformations of methane, were prepared separately by adsorption of 13 C‐enriched methane, carbon monoxide, and methanol onto zinc‐containing catalysts, respectively. Successful isolation of each surface species allowed convenient investigations into their chemical nature on the working catalyst by solid‐state 13 C MAS NMR spectroscopy. The reactivity of zinc methyl species with diverse probe molecules (i.e., water, methanol, hydrochloride, oxygen, or carbon dioxide) is correlated with that of organozinc compounds in organometallic chemistry. Moreover, surface formate and surface methoxy species possess distinct reactivity towards water, hydrochloride, ammonia, or hydrogen as probe molecules. To explain these and other observations, we propose that the C 1 surface species interconvert on zeolite Zn/H‐ZSM‐5. As implied by the reactivity information, potential applications of methane co‐conversion on zinc‐containing zeolites might, therefore, be possible by further transformation of these C 1 surface species with rationally designed co‐reactants (i.e., probe molecules) under optimized reaction conditions.