xNi–yCu–ZrO2 catalysts for the hydrogenation of levulinic acid to gamma valorlactone

Jones, Daniel; Iqbal, Sarwat; Thomas, Lloyd E.; Ishikawa, Satoshi; Reece, Christian; Miedziak, Peter J.; Morgan, David; Bartley, Jonathan K.; Willock, David J.; Ueda, Wataru; Hutchings, Graham J.

doi:10.1080/2055074x.2018.1433598

Cited by 11 publications

(9 citation statements)

References 55 publications

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“…In previous work, we have shown how incorporating significantly higher amounts of Ni at the coprecipitation preparation stage can lead to enhanced performance. The most active materials in this case consist of 45% Ni and 5% Cu coprecipitated with ZrO 2 using the oxalate gel approach . Interestingly, the doping of Mn onto the Cu–ZrO 2 was found to significantly increase the yield of GVL produced (GVL yield = 82%).…”

Section: Resultsmentioning

confidence: 97%

“…The most active materials in this case consist of 45% Ni and 5% Cu coprecipitated with ZrO 2 using the oxalate gel approach. 35 Interestingly, the doping of Mn onto the Cu−ZrO 2 was found to significantly increase the yield of GVL produced (GVL yield = 82%). The doping of Ti and V onto the catalyst was found to completely deactivate the Cu− ZrO 2 catalyst.…”

Section: Resultsmentioning

confidence: 99%

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The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid

et al. 2018

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Catalytic hydrogenation of levulinic acid to form γ-valerolactone was studied over Cu-ZrO2 catalysts doped with metal oxides from the first row transition metals. The Cu-ZrO2 material was prepared by oxalate gel co-precipitation and dopants were added by an incipient wetness approach. The addition of 1% Mn into Cu-ZrO2 significantly increases the yield of γ-valerolactone and the catalytic activity of Mn/Cu-ZrO2 was found to be 1.6 times higher than that of the undoped Cu-ZrO2 catalyst. Catalyst characterization suggests that the Mn dopant improves the dispersion of Cu on the surface of ZrO2. Kinetic studies show that the reaction order with respect to the substrate concentration is approximately zero. However, the order of reaction with respect to the partial pressure of H2 is different for the Mn/Cu-ZrO2 and Cu-ZrO2 catalysts. Comparison of reaction products from reactions carried out in H2O and D2O solvents using 1 H NMR and 13 C NMR show that there is a pre-equilibrium keto-enol isomerisation step under our reaction conditions. DFT calculations show that the enol isomers have a higher affinity for the Cu surface which may improve the availability of the substrate in the hydrogenation step of the reaction.

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Section: Resultsmentioning

confidence: 97%

Section: Resultsmentioning

confidence: 99%

The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid

et al. 2018

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“…8, the Co@C NPs can work at 200 o C with 10 bar of H 2 , which are milder than those reports using Au-, Ru-and Cu-based catalysts. [27][28][29] Over 98% yield of γ-valerolactone was obtained within 45 min in the first run. The stability of non-noble metal catalysts is an important issue for the hydrogenation of levulinic acid.…”

Section: Comparison Of Non-noble Metal Catalysts Prepared By Differenmentioning

confidence: 99%

A new strategy to transform mono and bimetallic non-noble metal nanoparticles into highly active and chemoselective hydrogenation catalysts

Liu

Gao

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et al. 2017

Journal of Catalysis

102

106

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A new strategy to transform non-noble metal oxide nanoparticles (NPs) into highly active and selective metallic NPs as hydrogenation catalysts by a simple carbon coating process based on hydrothermal treatment with glucose is presented. During the carbon coating process, metal oxide NPs will be reduced to metallic NPs and covered by thin carbon layers, resulting in formation of Metal@C NPs. Through this method, monometallic Co@C has been prepared, which show excellent activity and selectivity for chemoselectivity hydrogenation of substituted nitroarenes to corresponding anilines under mild conditions. Kinetic, isotopic and spectroscopic studies indicate that hydrogen dissociation-addition is the controlling step in chemoselective hydrogenation reaction with Co@C NPs. Stabilization and the reaction rate of metallic Co is improved by preparing bimetallic CoNi@C catalyst, leading to almost five-fold improved activity. Our preparation method enables to synthesize non-noble bimetallic CoNi@C nanoparticles with nearly one-order magnitude higher activity than any Co-based non-noble metal catalysts prepared by other methods, without necessity to involve the promoting role of metal-N interactions. At last, we also show the application of of Co@C NPs for hydrogenation of levulinic acid to γ-valerolactone.

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“…Previous studies have also reported that smaller particle sizes are favorable for LA conversion reactions. [51][52][53] Furthermore, the synergistic effect of Ni and Cu was greatly affected by the fabrication strategy, which influenced the interfacial properties of Ni and Cu. The H 2 -TPR results indicated that a NiÀ Cu alloy might have been formed during the preparation of NiÀ CuÀ OMA, indicating that the Ni and Cu species were simultaneously reduced to generate the NiÀ Cu alloy of the Ni δ Cu 1-δ Al 2 O 4 (0 � δ � 1) form.…”

Section: Chemsuschemmentioning

confidence: 99%

Enhanced Hydrogenation of Levulinic Acid over Ordered Mesoporous Alumina‐Supported Catalysts: Elucidating the Effect of Fabrication Strategy

et al. 2022

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In this work, three types of alumina‐supported bimetallic Ni−Cu catalysts [Ni−Cu/commercial non‐ordered mesoporous alumina (CMA), Ni−Cu/ordered MA (OMA), and Ni−Cu−OMA] were prepared via different fabrication strategies and investigated in the conversion of levulinic acid (LA) into γ‐valerolactone and 2‐methyltetrahydrofuran (2‐MTHF). This study employed characterization techniques and reactions to reveal the effects of the fabrication strategy on the activities of the catalysts. It was observed that the catalysts constructed on OM supports (Ni−Cu/OMA and Ni−Cu−OMA) displayed superior catalytic performance compared to those constructed on CM supports (Ni−Cu/CMA). Specifically, Ni−Cu−OMA, which was fabricated via the one‐pot evaporation‐induced self‐assembly strategy, exhibited the best catalytic performance, achieving a complete conversion of LA and a high selectivity of 73.0 % toward 2‐MTHF in a solvent‐free reaction environment. The promising activity of Ni−Cu−OMA was ascribed to the well‐dispersed active sites within the framework of the support, the enhanced metal‐support interaction, and the highly efficient exploitation of the synergistic effect between Ni and Cu. Detailed post‐characterization techniques were also employed to highlight the outstanding stability of Ni−Cu−OMA.

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xNi–yCu–ZrO₂ catalysts for the hydrogenation of levulinic acid to gamma valorlactone

Cited by 11 publications

References 55 publications

The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid

The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid

A new strategy to transform mono and bimetallic non-noble metal nanoparticles into highly active and chemoselective hydrogenation catalysts

Enhanced Hydrogenation of Levulinic Acid over Ordered Mesoporous Alumina‐Supported Catalysts: Elucidating the Effect of Fabrication Strategy

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xNi–yCu–ZrO2 catalysts for the hydrogenation of levulinic acid to gamma valorlactone

Cited by 11 publications

References 55 publications

The Effects of Dopants on the Cu–ZrO2 Catalyzed Hydrogenation of Levulinic Acid

The Effects of Dopants on the Cu–ZrO2 Catalyzed Hydrogenation of Levulinic Acid

A new strategy to transform mono and bimetallic non-noble metal nanoparticles into highly active and chemoselective hydrogenation catalysts

Enhanced Hydrogenation of Levulinic Acid over Ordered Mesoporous Alumina‐Supported Catalysts: Elucidating the Effect of Fabrication Strategy

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Product

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xNi–yCu–ZrO₂ catalysts for the hydrogenation of levulinic acid to gamma valorlactone

The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid

The Effects of Dopants on the Cu–ZrO₂ Catalyzed Hydrogenation of Levulinic Acid