Transfer hydrogenation from glycerol over a Ni-Co/CeO2 catalyst: A highly efficient and sustainable route to produce lactic acid

[Display omitted] •Efficient conversion of glycerol to lactate with concomitant transfer to various H2 acceptors.•A bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic counterparts.•The NiCo/CeO2 catalyst achieved very high yield of lactic acid salt (93%) at 97% glycerol...

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Published in:Applied catalysis. B, Environmental Vol. 263; p. 118273
Main Authors: Tang, Zhenchen, Cao, Huatang, Tao, Yehan, Heeres, Hero J., Pescarmona, Paolo P.
Format: Journal Article
Language:English
Published: Amsterdam Elsevier B.V 01.04.2020
Elsevier BV
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ISSN:0926-3373, 1873-3883
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Abstract [Display omitted] •Efficient conversion of glycerol to lactate with concomitant transfer to various H2 acceptors.•A bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic counterparts.•The NiCo/CeO2 catalyst achieved very high yield of lactic acid salt (93%) at 97% glycerol conversion.•The NiCo/CeO2 catalyst also gave high activity and selectivity in the transfer hydrogenation. Bimetallic Ni-Co catalysts supported on nanosized CeO2 were prepared and investigated as heterogeneous catalysts for the transfer hydrogenation between glycerol and various H2 acceptors (levulinic acid, benzene, nitrobenzene, 1-decene, cyclohexene) to selectively produce lactic acid (salt) and the target hydrogenated compound. The bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic Ni or Co counterparts (with equal total metal mass), thus indicating strong synergetic effects. The interaction between the metallic sites and the CeO2 support was thoroughly characterised by means of transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDX) mapping, X-ray photoelectron spectroscopy (XPS), hydrogen-temperature programmed reduction (H2-TPR) and X-ray diffraction (XRD). Combining characterisation and catalytic results proved that the Ni species are intrinsically more active than Co species, but that incorporating Co into the catalyst formulation prevented the formation of large Ni particles and led to highly dispersed metal nanoparticles on CeO2, thus leading to the observed enhanced activity for the bimetallic system. The highest yield of lactic acid (salt) achieved in this work was 93% at 97% glycerol conversion (160 °C, 6.5 h at 20 bar N2, NaOH: glycerol = 1.5). The NiCo/CeO2 catalyst also exhibited high activity and selectivity towards the target hydrogenated products in the transfer hydrogenation reactions between glycerol and various H2 acceptors. Batch recycle experiments showed good reusability, with retention of 80% of the original activity after 5 runs.
AbstractList Bimetallic Ni-Co catalysts supported on nanosized CeO2 were prepared and investigated as heterogeneous catalysts for the transfer hydrogenation between glycerol and various H2 acceptors (levulinic acid, benzene, nitrobenzene, 1-decene, cyclohexene) to selectively produce lactic acid (salt) and the target hydrogenated compound. The bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic Ni or Co counterparts (with equal total metal mass), thus indicating strong synergetic effects. The interaction between the metallic sites and the CeO2 support was thoroughly characterised by means of transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDX) mapping, X-ray photoelectron spectroscopy (XPS), hydrogen-temperature programmed reduction (H2-TPR) and X-ray diffraction (XRD). Combining characterisation and catalytic results proved that the Ni species are intrinsically more active than Co species, but that incorporating Co into the catalyst formulation prevented the formation of large Ni particles and led to highly dispersed metal nanoparticles on CeO2, thus leading to the observed enhanced activity for the bimetallic system. The highest yield of lactic acid (salt) achieved in this work was 93% at 97% glycerol conversion (160 °C, 6.5 h at 20 bar N2, NaOH: glycerol = 1.5). The NiCo/CeO2 catalyst also exhibited high activity and selectivity towards the target hydrogenated products in the transfer hydrogenation reactions between glycerol and various H2 acceptors. Batch recycle experiments showed good reusability, with retention of 80% of the original activity after 5 runs.
[Display omitted] •Efficient conversion of glycerol to lactate with concomitant transfer to various H2 acceptors.•A bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic counterparts.•The NiCo/CeO2 catalyst achieved very high yield of lactic acid salt (93%) at 97% glycerol conversion.•The NiCo/CeO2 catalyst also gave high activity and selectivity in the transfer hydrogenation. Bimetallic Ni-Co catalysts supported on nanosized CeO2 were prepared and investigated as heterogeneous catalysts for the transfer hydrogenation between glycerol and various H2 acceptors (levulinic acid, benzene, nitrobenzene, 1-decene, cyclohexene) to selectively produce lactic acid (salt) and the target hydrogenated compound. The bimetallic NiCo/CeO2 catalyst showed much higher activity than the monometallic Ni or Co counterparts (with equal total metal mass), thus indicating strong synergetic effects. The interaction between the metallic sites and the CeO2 support was thoroughly characterised by means of transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDX) mapping, X-ray photoelectron spectroscopy (XPS), hydrogen-temperature programmed reduction (H2-TPR) and X-ray diffraction (XRD). Combining characterisation and catalytic results proved that the Ni species are intrinsically more active than Co species, but that incorporating Co into the catalyst formulation prevented the formation of large Ni particles and led to highly dispersed metal nanoparticles on CeO2, thus leading to the observed enhanced activity for the bimetallic system. The highest yield of lactic acid (salt) achieved in this work was 93% at 97% glycerol conversion (160 °C, 6.5 h at 20 bar N2, NaOH: glycerol = 1.5). The NiCo/CeO2 catalyst also exhibited high activity and selectivity towards the target hydrogenated products in the transfer hydrogenation reactions between glycerol and various H2 acceptors. Batch recycle experiments showed good reusability, with retention of 80% of the original activity after 5 runs.
ArticleNumber 118273
Author Pescarmona, Paolo P.
Tang, Zhenchen
Heeres, Hero J.
Cao, Huatang
Tao, Yehan
Author_xml – sequence: 1
  givenname: Zhenchen
  surname: Tang
  fullname: Tang, Zhenchen
  organization: Chemical Engineering Group, Engineering and Technology Institute Groningen, University of Groningen, Nijenborgh 4, 9747 AG Groningen, the Netherlands
– sequence: 2
  givenname: Huatang
  surname: Cao
  fullname: Cao, Huatang
  organization: School of Materials, University of Manchester, Manchester M139PL, United Kingdom
– sequence: 3
  givenname: Yehan
  surname: Tao
  fullname: Tao, Yehan
  organization: Chemical Engineering Group, Engineering and Technology Institute Groningen, University of Groningen, Nijenborgh 4, 9747 AG Groningen, the Netherlands
– sequence: 4
  givenname: Hero J.
  surname: Heeres
  fullname: Heeres, Hero J.
  organization: Chemical Engineering Group, Engineering and Technology Institute Groningen, University of Groningen, Nijenborgh 4, 9747 AG Groningen, the Netherlands
– sequence: 5
  givenname: Paolo P.
  orcidid: 0000-0003-3608-6400
  surname: Pescarmona
  fullname: Pescarmona, Paolo P.
  email: p.p.pescarmona@rug.nl
  organization: Chemical Engineering Group, Engineering and Technology Institute Groningen, University of Groningen, Nijenborgh 4, 9747 AG Groningen, the Netherlands
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Keywords Co catalyst
Glycerol
Transfer hydrogenation
Lactic acid
Alloy effects
Ni catalyst
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Snippet [Display omitted] •Efficient conversion of glycerol to lactate with concomitant transfer to various H2 acceptors.•A bimetallic NiCo/CeO2 catalyst showed much...
Bimetallic Ni-Co catalysts supported on nanosized CeO2 were prepared and investigated as heterogeneous catalysts for the transfer hydrogenation between...
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StartPage 118273
SubjectTerms Acids
Alloy effects
Benzene
Bimetals
Catalysts
Cerium oxides
Co catalyst
Cyclohexene
Glycerol
Hydrogen storage
Hydrogenation
Intermetallic compounds
Lactic acid
Levulinic acid
Mapping
Nanoparticles
Ni catalyst
Nickel
Nitrobenzene
Photoelectron spectroscopy
Photoelectrons
Scanning transmission electron microscopy
Selectivity
Sodium hydroxide
Spectrum analysis
Transfer hydrogenation
Transmission electron microscopy
X ray photoelectron spectroscopy
X-ray diffraction
X-ray spectroscopy
Title Transfer hydrogenation from glycerol over a Ni-Co/CeO2 catalyst: A highly efficient and sustainable route to produce lactic acid
URI https://dx.doi.org/10.1016/j.apcatb.2019.118273
https://www.proquest.com/docview/2343106068
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