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Methanol carboxylation over zirconium dioxide: Effect of catalyst phase composition on its acid‐base spectrum and direction of catalytic transformations
Author(s) -
Kochkin Yuri N.,
Vlasenko Nina V.,
Struzhko Vira L.,
Puziy Alexander M.,
Strizhak Peter E.
Publication year - 2016
Publication title -
the canadian journal of chemical engineering
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.404
H-Index - 67
eISSN - 1939-019X
pISSN - 0008-4034
DOI - 10.1002/cjce.22435
Subject(s) - catalysis , calcination , zirconium dioxide , carboxylation , methanol , chemistry , base (topology) , inorganic chemistry , tetragonal crystal system , zirconium , selectivity , acid–base reaction , phase (matter) , bicarbonate , chemical engineering , organic chemistry , mathematical analysis , mathematics , engineering
The effect of ZrO 2 calcination temperature on its structure and acid‐base characteristics was investigated to elucidate their relation to catalytic behaviour in methanol carboxylation. Varying the calcination temperature causes changes in ZrO 2 phase composition and acid‐base characteristics. The base properties of ZrO 2 play a prominent role in dimethyl carbonate synthesis. Strong base sites (E CO2 > 78 kJ/mol) are needed to activate СО 2 . Tetragonal modification of zirconium dioxide has a higher basicity than the monoclinic. Thus, the greater the contribution of t‐ZrO 2 in the catalyst, the greater its ability to activate СО 2 and therefore result in higher catalytic activity for methanol carboxylation. DMC selectivity was determined by the ratio of catalyst base site to acid site concentration.