Selective Hydrogenation of Glycolic Acid to Renewable Ethylene Glycol over Supported Ruthenium Catalysts

Harth, Florian M.; Goepel, Michael; Gläser, Roger

doi:10.1002/cctc.202101275

Cited by 4 publications

(13 citation statements)

References 44 publications

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“…For deeper characterization of the ruthenium species on the surface of MCF, the H 2 chemisorption analyses were performed [ 31 , 32 ]. Based on these measurements, the ruthenium dispersion, particle size distribution and metal surface area were estimated.…”

Section: Resultsmentioning

confidence: 99%

Impact of Cerium Oxide on the State and Hydrogenation Activity of Ruthenium Species Incorporated on Mesocellular Foam Silica

2022

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Herein, the impact of cerium species loaded on mesoporous silica of MCF type on the state and catalytic activity of ruthenium species was studied. Up to 20 wt.% of cerium was incorporated on the silica surface, whereas the same 1 wt.% of Ru loading was applied. The samples prepared were examined by low temperature N2 adsorption/desorption, XRD, XRF, ICP-OES, XPS and H2 chemisorption. The catalytic activity of the materials obtained was investigated in the transformation of levulinic acid to γ-valerolactone. It was documented that the presence of Ce favored an increase in the dispersion of ruthenium species, which had a positive impact on the hydrogenation activity for up to 10 wt.% of Ce. Nevertheless, the highest cerium loading had a negative influence on the textural parameters of the support.

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Section: Resultsmentioning

confidence: 99%

Impact of Cerium Oxide on the State and Hydrogenation Activity of Ruthenium Species Incorporated on Mesocellular Foam Silica

2022

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“…Diluted GA solutions can be almost quantitatively converted into EG (up to 90 % yield) applying a suitable catalyst (Ru/TiO 2 or commercial Ru/C) at mild reaction conditions (105 °C, 60 bar H 2 ). [18] These results serve as the starting point of the present investigation.…”

Section: Introductionmentioning

confidence: 81%

“…For all experiments, a commercially available carbon‐supported Ru catalyst with a nominal Ru loading of 5 wt.% was used (Ru/C, ABCR). The same catalyst was already used in our previous study containing detailed characterization data and information on the corresponding characterization methods [18] . An overview of the key material properties (textural properties and metal dispersion) is shown in Table S1.…”

Section: Methodsmentioning

confidence: 99%

“…The same catalyst was already used in our previous study containing detailed characterization data and information on the corresponding characterization methods. [18] An overview of the key material properties (textural properties and metal dispersion) is shown in Table S1. Ru/C was reduced directly before every catalytic experiment in a tubular furnace.…”

Section: Analysis Of the Algal Mediummentioning

confidence: 99%

“…In a recent study, [18] we systematically investigated supported metal catalysts for the hydrogenation of diluted aqueous GA model solutions (GA concentration of 70 mmol L −1 , i. e., in the range of state‐of‐the‐art algal media). Ru is an especially suited catalyst among other metals (Pt, Pd, Re) and the support material has a considerable influence on both catalytic activity and selectivity.…”

Section: Introductionmentioning

confidence: 99%

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Ru/C‐Catalyzed Hydrogenation of Aqueous Glycolic Acid from Microalgae – Influence of pH and Biologically Relevant Additives

et al. 2022

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Ethylene glycol (EG) is obtained by a novel, two‐step approach combining a biotechnological and a heterogeneously catalyzed step. First, microalgae are cultivated to photobiocatalytically yield glycolic acid (GA) by means of photosynthesis from CO2 and water. GA is continuously excreted into the surrounding medium. In the second step, the GA‐containing algal medium is used as feedstock for catalytic reduction with H2 to EG over a Ru/C catalyst. The present study focuses on the conversion of an authentic algae‐derived GA solution. After identification of the key characteristics of the algal medium (compared to pure aqueous GA), the influence of pH, numerous salt additives, pH buffers and other relevant organic molecules on the catalytic GA reduction was investigated. Nitrogen‐ and sulfur‐containing organic molecules can strongly inhibit the reaction. Moreover, pH adjustment by acidification is required, for which H2SO4 is found most suitable. In combination with a modification of the biotechnological process to mitigate the use of inhibitory compounds, and after acidifying the algal medium, over Ru/C a EG yield of up to 21 % even at non‐optimized reaction conditions was achieved.

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Microkinetic Modelling of the Heterogeneously Catalyzed Hydrogenation of Glycolic Acid over Ru/C

Harth,

Kojčinović,

Likozar

et al. 2024

ChemCatChem

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The heterogeneously catalyzed hydrogenation of biomass‐or CO2‐derived glycolic acid (GA) is a renewable pathway for obtaining the bulk chemical ethylene glycol (EG). In this study, the reaction network of the aqueous‐phase hydrogenation of GA is investigated over a Ru/C catalyst. As previous studies indicated, several parallel and consecutive reactions can occur in addition to the desired reaction to EG. These reactions are experimentally assessed by employing different (possible) reaction intermediates and products as reactants. The data for all individual reactions and GA hydrogenation at different reaction temperatures (120‐180°C) is combined to propose a catalytic reaction pathway network and to develop a corresponding microkinetic model. The model describes the catalytic data in the range up to 150°C, where EG is the main reaction product, with high accuracy. It is shown that selectivity for EG is highest at 120°C and decreases strongly with increasing temperatures both due to the parallel reaction of GA into AcA, which has a significantly higher activation energy than the overall hydrogenation of GA into EG, and due to degradation of EG into ethanol and volatile products. Temperatures exceeding 150°C predominantly yield volatile products, suggesting low yields of EG or AcA at higher temperatures despite enhanced GA conversion.

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Selective Hydrogenation of Glycolic Acid to Renewable Ethylene Glycol over Supported Ruthenium Catalysts

Cited by 4 publications

References 44 publications

Impact of Cerium Oxide on the State and Hydrogenation Activity of Ruthenium Species Incorporated on Mesocellular Foam Silica

Impact of Cerium Oxide on the State and Hydrogenation Activity of Ruthenium Species Incorporated on Mesocellular Foam Silica

Ru/C‐Catalyzed Hydrogenation of Aqueous Glycolic Acid from Microalgae – Influence of pH and Biologically Relevant Additives

Microkinetic Modelling of the Heterogeneously Catalyzed Hydrogenation of Glycolic Acid over Ru/C

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