Chemically activated ruthenium mono(bipyridine)/SiO2 catalysts in water–gas shift reaction

Haukka, Matti; Venäläinen, Tapani; Kallinen, Mirja; Pakkanen, Tapani A.

doi:10.1016/s1381-1169(98)00052-1

Cited by 44 publications

(17 citation statements)

References 19 publications

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“…[ 6 ] We identified three different reasons for the observed enhanced catalytic performance after salt coating: a) alkali doping has been demonstrated to be relevant for the increased CO 2 selectivity; b) the hygroscopic nature of the applied salt was assumed to be relevant for increasing water availability at the catalytic site; and c) the basicity of the salt was regarded to be important for the promotion of the water–gas-shift reaction step, that is, the conversion of CO and water into CO 2 and hydrogen. [ 13 ] The latter reaction forms an important part of the methanol steam reforming reaction sequence.…”

Section: Resultsmentioning

confidence: 99%

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

et al. 2014

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We herein describe a straight forward procedure to increase the performance of platinum-on-alumina catalysts in methanol steam reforming by applying an alkali hydroxide coating according to the “solid catalyst with ionic liquid layer” (SCILL) approach. We demonstrate by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and temperature-programmed desorption (TPD) studies that potassium doping plays an important role in the catalyst activation. Moreover, the hygroscopic nature and the basicity of the salt modification contribute to the considerable enhancement in catalytic performance. During reaction, a partly liquid film of alkali hydroxides/carbonates forms on the catalyst/alumina surface, thus significantly enhancing the availability of water at the catalytically active sites. Too high catalyst pore fillings with salt introduce a considerable mass transfer barrier into the system as indicated by kinetic studies. Thus, the optimum interplay between beneficial catalyst modification and detrimental mass transfer effects had to be identified and was found on the applied platinum-on-alumina catalyst at KOH loadings around 7.5 mass %.

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Section: Resultsmentioning

confidence: 99%

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

et al. 2014

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“…Ruthenium(II)–carbonyl compounds with one or two diimine chelating ligands ( N – N ), such as [Ru(bpy)Cl 2 (CO) 2 ] and [Ru(bpy) 2 (CO)(X)] n + {bpy = 2,2′‐bipyridine, X = Cl, CO, CO 2 , C(O)OH, CHO, CH 2 OH, and CH 3 ; n = 1, 2 depending on X}, have been extensively investigated as catalysts or key intermediates for the photochemical, electrochemical, and photo‐electrochemical reduction of CO 2 ,1–9 and for the water–gas shift reaction 10–13. These compounds were also tested as catalysts in the hydroformylation of 1‐hexene and hydrogenation of 1‐heptanal,14,15 and in hydrogen‐transfer reactions 16.…”

Section: Introductionmentioning

confidence: 99%

New Insight into a Deceptively Simple Reaction: The Coordination of bpy to Ru^II–Carbonyl Precursors – The Central Role of the fac‐[Ru(bpy)Cl(CO)₃]⁺ Intermediate and the Chloride Rebound Mechanism

et al. 2015

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This work demonstrates how a careful reexamination of welltrodden fields can fill conceptual gaps that previously escaped full understanding. The coordination of 2,2Ј-bipyridine (bpy) to the known Ru II -chlorido-carbonyl precursors -the dinuclear [RuCl 2 (CO) 3 ] 2 (P1) and the polymeric [RuCl 2 -(CO) 2 ] n (P2) -has been investigated by several groups in the past, and a remarkably large number of rutheniummono(bpy)-carbonyl compounds were identified and fully characterized. Many were investigated as catalysts or key intermediates for the photochemical, electrochemical, and photo-electrochemical reduction of CO 2 , and for the watergas shift reaction. Nevertheless, even though most -if not all -of the reaction products are known already, a careful examination of the literature led us to believe that a convincing general scheme interconnecting them all was still missing and important questions remained unanswered. For this reason, we investigated the reactivity of two mononuclear4304 Scheme 20. The slow spontaneous conversion of hydrido complex 5 into a mixture of 1 and 2 in CDCl 3 .

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“…The trans(CO),cis(Cl) complex is thermodynamically unfavorable and has not been isolated. [8] Complex 1 has been synthesized mostly by reaction of bpy with the so-called "red carbonyl solution" [4a,5b-5e,5g,5h,9] or [Ru(CO) 3 Cl 2 ] 2 , [1,8,10] the latter of which is commercially available. Although these synthetic procedures afford a mixture of trans(Cl)-1 and cis(Cl)-1, a ruthenium precursor of [Ru(CO) 2 Cl 2 ] n , which was prepared by heating RuCl 3 at reflux in formic acid, selectively produces trans(Cl)-1 in the reaction with bpy in methanol.…”

Section: "] Cis(co)cis(cl) ["Cis(cl)-1"] and Trans(co)cis(cl)mentioning

confidence: 99%

“…The ruthenium mono(bipyridine) dicarbonyl dichloride complex Ru(bpy)(CO) 2 Cl 2 (1) has been widely studied from the viewpoint of its photochemical decarbonylation, [1] the catalytic activities for epoxidation of olefins, [2] the watergas shift reaction, [3] and the photochemical [4] /electrochemical reduction of CO 2 .…”

Section: Introductionmentioning

confidence: 99%

Chain Reaction for Isomerization from trans(Cl) to cis(Cl)‐Ru(bpy)(CO)₂Cl₂ (bpy = 2,2′‐Bipyridine) Induced by NaBH₄

2012

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Chemically activated ruthenium mono(bipyridine)/SiO2 catalysts in water–gas shift reaction

Cited by 44 publications

References 19 publications

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

New Insight into a Deceptively Simple Reaction: The Coordination of bpy to Ru^II–Carbonyl Precursors – The Central Role of the fac‐[Ru(bpy)Cl(CO)₃]⁺ Intermediate and the Chloride Rebound Mechanism

Chain Reaction for Isomerization from trans(Cl) to cis(Cl)‐Ru(bpy)(CO)₂Cl₂ (bpy = 2,2′‐Bipyridine) Induced by NaBH₄

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Chemically activated ruthenium mono(bipyridine)/SiO2 catalysts in water–gas shift reaction

Cited by 44 publications

References 19 publications

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

Methanol Steam Reforming Promoted by Molten Salt‐Modified Platinum on Alumina Catalysts

New Insight into a Deceptively Simple Reaction: The Coordination of bpy to RuII–Carbonyl Precursors – The Central Role of the fac‐[Ru(bpy)Cl(CO)3]+ Intermediate and the Chloride Rebound Mechanism

Chain Reaction for Isomerization from trans(Cl) to cis(Cl)‐Ru(bpy)(CO)2Cl2 (bpy = 2,2′‐Bipyridine) Induced by NaBH4

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New Insight into a Deceptively Simple Reaction: The Coordination of bpy to Ru^II–Carbonyl Precursors – The Central Role of the fac‐[Ru(bpy)Cl(CO)₃]⁺ Intermediate and the Chloride Rebound Mechanism

Chain Reaction for Isomerization from trans(Cl) to cis(Cl)‐Ru(bpy)(CO)₂Cl₂ (bpy = 2,2′‐Bipyridine) Induced by NaBH₄