Selective formation of formic acid from biomass-derived glycolaldehyde with supported ruthenium hydroxide catalysts

Modvig, Amalie; Riisager, Anders

doi:10.1039/c9cy00271e

Cited by 11 publications

(6 citation statements)

References 63 publications

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“…36,40 Ru(OH) 3 (463.0 eV) and RuO 2 (462.5 eV) were the predominant Ru component for the Ru(OH) 3 /AC and RuO 2 /AC, respectively, agreeing well with other supported ruthenium hydroxide and oxides prepared via a similar method. 42,43 As anticipated, RuCl 3 had the highest amount of Cl (3.7 wt %), which decreased dramatically to 0.4 wt % for Ru/AC after the reduction process. Ru(OH) 3 /AC and RuO 2 /AC showed lower Cl − content, as most of Cl − was washed during the catalyst preparation.…”

Section: = ×supporting

confidence: 57%

“…The hydrous ruthenium oxide and Cl – adsorbed on AC would be formed from the hydrolysis of RuCl 3 during the catalyst preparation. After treatment of RuCl 3 /AC in flowing H 2 at 773 K to prepare Ru/AC, around 84.3% of Ru 3+ was reduced to Ru 0 (462.0 eV) and the other ruthenium species were converted to RuO x (466.0 eV) due to the reoxidation of Ru 0 when the Ru/AC was exposed to air. , Ru(OH) 3 (463.0 eV) and RuO 2 (462.5 eV) were the predominant Ru component for the Ru(OH) 3 /AC and RuO 2 /AC, respectively, agreeing well with other supported ruthenium hydroxide and oxides prepared via a similar method. , As anticipated, RuCl 3 had the highest amount of Cl (3.7 wt %), which decreased dramatically to 0.4 wt % for Ru/AC after the reduction process. Ru(OH) 3 /AC and RuO 2 /AC showed lower Cl – content, as most of Cl – was washed during the catalyst preparation.…”

Section: Resultsmentioning

confidence: 99%

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Selective Oxidation of Methyl Lactate over Carbon-Supported Noble Metal Catalysts under Base-Free Conditions

Chu

Yan

Xia

et al. 2021

Ind. Eng. Chem. Res.

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The selective oxidation of biomass-derived alcohol-containing functional compounds with molecular oxygen over solid catalysts is a promising approach to renewably produce value-added ketones, aldehydes, and/or carboxylic acids. Activated carbon (AC) supported Pt, Pd, Rh, Ru, and Au nanoparticles at comparable sizes (average: 1.4–2.9 nm) were evaluated in the liquid-phase oxidative dehydrogenation of methyl lactate (ML) to methyl pyruvate (MP) with oxygen under base-free conditions. Ru/AC gives not only much higher MP selectivity (ca. 90%) but also an order of magnitude in the initial turnover frequency (TOF) of ML higher than other noble-metal catalysts for this ML-to-MP reaction. Metallic Ru (Ru/AC: 84.3% Ru0 and 15.7% RuO x ) is also found to be superior to other Ru species (RuCl3, RuO2, and Ru(OH)3) supported on AC in terms of higher activity and selectivity. The oxidative dehydrogenation of ML is always accompanied by the hydrolysis reactions of MP and ML and consecutive secondary reactions (decarboxylation, decarbonylation, oxidation, etc.) producing C1–C3 byproducts, which would be promoted by the surface acidic and basic sites. The effects of reaction variables (including ML concentration, O2 pressure, reaction temperature, and solvent) on ML oxidation were further examined on Ru/AC. A kinetic rate based on the Langmuir–Hinshelwood model was proposed, indicating that the rate-determining step of ML oxidation over the Ru/AC catalyst would be the surface reaction between independently adsorbed ML and oxygen species on active sites of different nature. γ-Valerolactone is identified as an efficient solvent for ML oxidation, producing high and stable activity and MP selectivity (87–94%) throughout 5 reaction runs.

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Section: = ×supporting

confidence: 57%

Section: Resultsmentioning

confidence: 99%

Selective Oxidation of Methyl Lactate over Carbon-Supported Noble Metal Catalysts under Base-Free Conditions

Chu

Yan

Xia

et al. 2021

Ind. Eng. Chem. Res.

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“…Glycolaldehyde is a renowned bio-based platform molecule which can be synthesised from retro-aldol reaction of glucose under subcritical hydrothermal conditions [176,177]. Glycolaldehyde shows promise as a key starting material raw for the synthesis of many interesting and important industrial chemicals, such as ethylene/propylene glycols, ethanolamine, glyoxal, formic acid, glycolic acid and tetrose sugars [178][179][180]. Among them, ethanolamine is a crucial chemical with an annual demand of over two million tons [181]; and the most attractive application of ethanolamine is application as an absorbent for CO 2 and SO 2 sequestration in power plants.…”

Section: Reductive Amination Of Glycolaldehydementioning

confidence: 99%

Sustainable access to renewable N-containing chemicals from reductive amination of biomass-derived platform compounds

et al. 2020

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“…30,31 The rise of temperature during the alkalinization step could catalyze this reaction. 32 All these findings clearly demonstrate that the matrix has a significant effect to orientate the products of the UEO, typically to obtain FA and OA instead of carbonate (as identified in the case of urea synthetic electrolysis).…”

Section: Electrolyzed Solutionmentioning

confidence: 76%

New Insights into Urea Electro-Oxidation: Complete Mass-Balances and Proof of Concept with Real-Matrix Effluent

Hopsort,

Latapie,

Groenen Serrano

et al. 2023

J. Electrochem. Soc.

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In the present work, all the by-products formed during the urea electrooxidation (UEO) by Ni(III) in alkaline medium are identified and quantified for the first time (e.g., OCN − , CO 3 2 − , NH 4 + , N 2 , NO 2 − ). Complete mass balances are simultaneously established in both aqueous and gas phases for large urea conversion rates (>80%). The results provide clear evidence (with a maximal deviation of 2%) that, in addition to N 2 , N-overoxidized by-products are produced during the UEO. Electrolyses conducted with human urine samples under identical operating conditions result in different distributions of N and C-by-products. In particular, the formation of formic and oxalic acids in these latter experiments suggests the presence of different and/or additional mechanistic pathways during the UEO process. The amount of H 2 generated at the cathode is also quantified, showing a reduction of 30% in energy consumption when compared with water electrolysis. Finally, this study assesses the energy efficiency of UEO with urea synthetic and real-matrix effluents, thereby contributing to the development of this sustainable process, which enables energy recovery from waste.

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Selective formation of formic acid from biomass-derived glycolaldehyde with supported ruthenium hydroxide catalysts

Abstract: Ceria-supported ruthenium hydroxide catalysts, Ru(OH)x/CeO2, with micro- and nanoparticle supports were applied for selective aerobic oxidation of glycolaldehyde (GAD) to formic acid (FA) in water under mild and base-free conditions.

Cited by 11 publications

References 63 publications

Selective Oxidation of Methyl Lactate over Carbon-Supported Noble Metal Catalysts under Base-Free Conditions

Selective Oxidation of Methyl Lactate over Carbon-Supported Noble Metal Catalysts under Base-Free Conditions

Sustainable access to renewable N-containing chemicals from reductive amination of biomass-derived platform compounds

New Insights into Urea Electro-Oxidation: Complete Mass-Balances and Proof of Concept with Real-Matrix Effluent

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