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The Photochemical Water-gas Shift Reaction Catalysed by Bis(2,2′-bipyridyl)(carbonyl)chlororuthenium(II) Chloride
Cl are shown to be active catalytic species for the water-gas shift reaction under mild conditions (1-3 atm CO, 100-160 deg C) and under illumination with white light.Turnover numbers of up to 20 1/h are observed.Stoicheiometric reactions, including labelling studies, shown that CO2 is produced thermally, whilst H2 is produced in a photochemical step.Mechanistic and kinetic data are presented for the catalytic reaction and they show that the reaction has a mechanism similar to those previously reported for the water-gas shift reaction and it does not involve formate decomposition.The rate-determaning step at all pH is photochemical loss of H2 from (1+) and different activation energies at high and low pH are attributed to different contributions from pre-equilibria involving attack of OH(1-) on co-ordinated CO (dominant at low pH) or protonation of (dominant at high pH).Experiments at high conversin show that at 140 deg C CO can be completely converted to products.Attempts to catalyse related reactions using unsaturated substrates are also described.
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Reference：
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI