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Rh 1 /γ‐Al 2 O 3 Single‐Atom Catalysis of O 2 Activation and CO Oxidation: Mechanism, Effects of Hydration, Oxidation State, and Cluster Size
Author(s) -
Ghosh Tushar K.,
Nair Nisanth N.
Publication year - 2013
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201200799
Subject(s) - catalysis , reactivity (psychology) , chemistry , oxidation state , cluster (spacecraft) , kinetics , heterogeneous catalysis , catalytic cycle , atom (system on chip) , catalytic oxidation , crystallography , organic chemistry , physics , alternative medicine , quantum mechanics , computer science , embedded system , programming language , medicine , pathology
The single‐atom catalysis of O 2 activation and CO oxidation with Rh 1 supported on γ‐Al 2 O 3 is investigated here through ab initio molecular dynamics techniques. We scrutinize the molecular details of the mechanism for the full catalytic cycle that involves the oxidation of two CO molecules in succession. The effect of the surface hydration and oxidation state of Rh on the kinetics of O 2 activation and CO oxidation is presented. We also report here the catalytic activity of experimentally intercepted Rh I (CO) 2 on γ‐Al 2 O 3 . Furthermore, we delineate the importance of single‐atom catalysis by comparing the performance of the Rh 6 /Al 2 O 3 catalyst. A molecular level understanding of the differential reactivity on hydration, on oxidation, and of a larger Rh cluster size is reported.