Iridium, Rhodium, and Ruthenium Catalysts for the “Aldehyde–Water Shift” Reaction

Brewster, Timothy P.; Ou, William C.; Tran, Jeremy C.; Goldberg, Karen I.; Hanson, Susan K.; Cundari, Thomas R.; Heinekey, D. Michael

doi:10.1021/cs500843a

Cited by 51 publications

(60 citation statements)

References 22 publications

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“…The rst is dehydrogenation of ethanol to acetaldehyde, and the second is the reaction of acetaldehyde with water which named "aldehyde-water shi" (AWS) reaction to acetic acid. 17,18 As the reaction results of Fig. 3 shows, pure Cr 2 O 3 exhibits none of catalytic activity which indicates at least the rst step of dehydrogenation can only proceed on copper species.…”

Section: Results Of Characterizationmentioning

confidence: 96%

“…20,21 Recently, Heinekey et al reported that a series of (p-cymene) ruthenium(II) diamine complexes and p-arene (or cyclopentadienyl) complexes of iridium, rhodium, and ruthenium were shown to be active catalysts for the conversion of aldehydes and water to carboxylic acids. 17,18 However, all these homogeneous reaction systems have the obvious disadvantages on the separation of products and the recycling of catalyst. Thus a more attractive process for industrial application would be heterogeneous reaction system especially over the base metal catalysts, because of the convenience of catalyst separation, facile continuous process operation and cost effectiveness.…”

Section: -19mentioning

confidence: 99%

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Production of acetic acid from ethanol over CuCr catalysts via dehydrogenation-(aldehyde–water shift) reaction

Xiang

Ran

et al. 2017

RSC Adv.

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A series of CuCr catalysts were prepared by co-precipitation method and used to produce acetic acid from ethanol via dehydrogenation-(aldehyde-water shift) reaction. The catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller analysis (BET), inductively coupled plasma atomic emission spectroscopy (ICP-AES), and temperature programmed reduction (TPR). The effects of copper contents and atmosphere on catalytic performance were investigated. The enhanced catalytic performance can be ascribed to the existence of chromium oxide.

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Section: Results Of Characterizationmentioning

confidence: 96%

Section: -19mentioning

confidence: 99%

Production of acetic acid from ethanol over CuCr catalysts via dehydrogenation-(aldehyde–water shift) reaction

Xiang

Ran

et al. 2017

RSC Adv.

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“…The strong interest in catalysis and electrocatalysis in aqueous medium has pushed ahead the study of metal hydrides in water. 54,[69][70][71][72][73][74][75][76][77][78][79][80][81][82][83] The close thermodynamic links between redox potentials and hydrogen ion concentration should provide a particularly strong framework for understanding the chemistry of transition metal hydrides in buffered solutions. A wide range of acid-base indicators can be used in titrations.…”

Section: Water and Methanolmentioning

confidence: 99%

“…Similarly the complex [Ru(H 2 )(PPh 3 ) 2 (tpm)] 2+ , where tpm is tris(pyrazolyl)methane, has a pK a DCM 2.8. 182 Several bipyridine complexes have been studied (entries 11,14,15,33,81,136,157) with pK a LAC ranging from -4 to 26. The bipyridine ligand contributes 8 pK a units to a metal hydride complex according to the LAC system.…”

Section: Complexes With Nitrogen Donorsmentioning

confidence: 99%

Brønsted–Lowry Acid Strength of Metal Hydride and Dihydrogen Complexes

2016

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Transition metal hydride complexes are usually amphoteric, not only acting as hydride donors, but also as Brønsted-Lowry acids. A simple additive ligand acidity constant equation (LAC for short) allows the estimation of the acid dissociation constant Ka(LAC) of diamagnetic transition metal hydride and dihydrogen complexes. It is remarkably successful in systematizing diverse reports of over 450 reactions of acids with metal complexes and bases with metal hydrides and dihydrogen complexes, including catalytic cycles where these reactions are proposed or observed. There are links between pKa(LAC) and pKa(THF), pKa(DCM), pKa(MeCN) for neutral and cationic acids. For the groups from chromium to nickel, tables are provided that order the acidity of metal hydride and dihydrogen complexes from most acidic (pKa(LAC) -18) to least acidic (pKa(LAC) 50). Figures are constructed showing metal acids above the solvent pKa scales and organic acids below to summarize a large amount of information. Acid-base features are analyzed for catalysts from chromium to gold for ionic hydrogenations, bifunctional catalysts for hydrogen oxidation and evolution electrocatalysis, H/D exchange, olefin hydrogenation and isomerization, hydrogenation of ketones, aldehydes, imines, and carbon dioxide, hydrogenases and their model complexes, and palladium catalysts with hydride intermediates.

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“…Recent papers have focused on the production of hydrogen from the aqueous reforming of methanol which, whilst presenting its own unique challenges, results in very high atom efficiencies for hydrogen production. Ruthenium has shown itself to be the most widely investigated and flexible metal for alcohol dehydrogenation reactions although others, including for example; iron [87,89], cobalt [90], osmium [70,91] and iridium [92][93][94], have also been investigated with varying success.…”

Section: Resultsmentioning

confidence: 99%

Advances in Ruthenium Catalysed Hydrogen Release from C1 Storage Materials

Waals¹

2015

Recyclable Catalysis

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Recent years have seen an increasing demand for fossil-fuels and consequent mounting damage to the environment. With this increasing demand the need for a renewable alternative source of energy is required. Hydrogen has been highlighted as an interesting alternative energy carrier showing both practical and economic advantages, particularly when used in conjunction with a hydrogen fuel cell [1]. Whilst there has been much progression in the clean and renewable production of hydrogen through; biomass gasification, photoelectrolysis and also electrolysis using energy derived from renewable sources [2,3], a challenge remains for the storage and delivery of hydrogen for small and mobile applications. This mini-review discusses a range of viable C1 hydrogen storage materials and focuses on the key publications, as well as recent additions to the literature, related to the ruthenium catalysed release of hydrogen as this is one of most intensively researched areas of the field. Current progress in the homogeneous ruthenium catalysed reduction of CO2 is also discussed.

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Iridium, Rhodium, and Ruthenium Catalysts for the “Aldehyde–Water Shift” Reaction

Cited by 51 publications

References 22 publications

Production of acetic acid from ethanol over CuCr catalysts via dehydrogenation-(aldehyde–water shift) reaction

Production of acetic acid from ethanol over CuCr catalysts via dehydrogenation-(aldehyde–water shift) reaction

Brønsted–Lowry Acid Strength of Metal Hydride and Dihydrogen Complexes

Advances in Ruthenium Catalysed Hydrogen Release from C1 Storage Materials

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