Influence of Catalyst Concentration on Activity and
Selectivity in Selective Methane Oxidation with Platinum Compounds
in Sulfuric Acid and Oleum
Tobias Zimmermann
Marius Bilke
Mario Soorholtz
Ferdi Schüth
10.1021/acscatal.8b01878.s001
https://acs.figshare.com/articles/journal_contribution/Influence_of_Catalyst_Concentration_on_Activity_and_Selectivity_in_Selective_Methane_Oxidation_with_Platinum_Compounds_in_Sulfuric_Acid_and_Oleum/7056521
Direct
catalytic functionalization of methane, a “dream
reaction”, is typically characterized by poorly active catalysts
and low product selectivity. Selectivity is particularly high for
the “Periana system”, in which methane is oxidized to
methyl bisulfate in sulfuric acid/oleum using a η<sup>2</sup>-(2,2′-bipyrimidyl)dichloroplatinum(II) ((bpym)PtCl<sub>2</sub>, <b>1</b>) catalyst. Recently it was shown that well-chosen
reaction conditions result in not only high selectivity but also remarkably
high activity, previously considered to be the prohibiting factor
regarding commercialization. The high activity apparently contradicts
the original report. Detailed studies of the dependence of activity
and selectivity on the catalyst concentration resolve this contradiction
and reveal solubility, transformation of catalyst precursors, speciation,
and solubility of methane as crucial factors for the observed reaction
rates. Additionally, the selectivity pattern clearly discloses the
consecutive nature of the reaction network.
2018-08-27 00:00:00
catalyst precursors
selectivity pattern
factor
methyl bisulfate
Selective Methane Oxidation
Platinum Compounds
catalyst concentration
reaction rates
reaction network
solubility
product selectivity
Selectivity
Catalyst Concentration
well-chosen reaction conditions result