Authors: Millar, Graeme J.; Newton, David; Bowmaker, Graham A.; Cooney, Ralph P.

Source: Applied Spectroscopy, Volume 48, Issue 7, Pages 14A-21A and 775-903 (July 1994) , pp. 827-832(6)

Publisher: Society for Applied Spectroscopy

Abstract:

An in situ infrared cell capable of studying reactions over heterogeneous catalysts in the temperature range 77 to 773 K has been designed. In particular, the adsorption of formic acid on a model Cu/SiO₂ methanol synthesis catalyst was investigated. Exposure of a reduced copper surface to formic acid at 300 K resulted in the formation of both formic acid molecules, which were ligated to the copper catalyst, and chemisorbed bidentate copper formate species. Under temperature-programming conditions, the bidentate species displayed a maximum rate of desorption at 433 K, which correlates to a desorption activation energy of 120 kJ mol^-1. In contrast, on the reoxidized catalyst, unidentate formate species were preferentially formed. These exhibited a maximum rate of desorption at a temperature of 408 K, and a desorption activation energy of 113 kJ mol^-1. A mechanism was postulated to explain this behavior, and evidence was presented to show that useful kinetic data can be obtained for desorption from a catalyst in the form of a pressed disk.

Keywords: In situ infrared; Copper catalyst; Formate adsorption

Document Type: Research article

DOI: http://dx.doi.org/10.1366/0003702944029893

Affiliations: 1: Department of Chemistry, University of Auckland, Private Bag 92019, Auckland, New Zealand

Publication date: 1994-07-01

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