Metal-acid nanoplate-supported ultrafine Ru nanoclusters for efficient catalytic fractionation of lignin into aromatic alcohols
The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal-acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium pho...
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Published in | Green chemistry : an international journal and green chemistry resource : GC Vol. 21; no. 1; pp. 2739 - 2751 |
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Main Authors | , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Cambridge
Royal Society of Chemistry
2019
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Subjects | |
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Abstract | The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal-acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium phosphate nanoplates (α-HfP NPs) to effectively depolymerise lignocellulosic biomass. A native lignin fraction of pine lignocellulose was promptly depolymerised into 19.86 wt% yield (lignin based) of valuable phenolic monomers (with dihydroeugenol as the main compound with high selectivity) and few cyclic ketones through one-pot catalytic reductive fractionation under mild conditions (190 °C, 3.5 MPa H
2
). Detailed scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and temperature-programmed desorption ammonia investigation correlated with the obtained results revealed that the metal-acid synergistic influence and the presence of Brønsted acid sites in the support for dehydration and the well-dispersed metallic role of Ru NCs for hydrodeoxygenation were responsible for the cleavage of lignin-carbohydrate (ester and ether linkages) bonds. Moreover, treating commercial lignin as a substrate in an organic solvent generated 4-hydroxy-3-methoxybenzaldehyde (vanillin) in high yield, as well as other functionalised phenolic monomers up to 85% selectivity, illustrating the high susceptibility of Ru/α-HfP NPs towards C-O bond cleavage through reductive fractionation. Multiple recycling tests of the catalyst were performed without any apparent loss of activity. Overall, this report highlighted the potential of the synthesis strategy of the metal-acid supported catalyst to immediately depolymerise untreated biomass and can thus encourage the green, cost-efficient, large-scale production of intermediate chemicals.
A novel metal-acid strategy that affords dual functionalities in the one-pot fractionation of lignin to phenolic compounds with excellent selectivity. |
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AbstractList | The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal-acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium phosphate nanoplates (α-HfP NPs) to effectively depolymerise lignocellulosic biomass. A native lignin fraction of pine lignocellulose was promptly depolymerised into 19.86 wt% yield (lignin based) of valuable phenolic monomers (with dihydroeugenol as the main compound with high selectivity) and few cyclic ketones through one-pot catalytic reductive fractionation under mild conditions (190 °C, 3.5 MPa H
2
). Detailed scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and temperature-programmed desorption ammonia investigation correlated with the obtained results revealed that the metal-acid synergistic influence and the presence of Brønsted acid sites in the support for dehydration and the well-dispersed metallic role of Ru NCs for hydrodeoxygenation were responsible for the cleavage of lignin-carbohydrate (ester and ether linkages) bonds. Moreover, treating commercial lignin as a substrate in an organic solvent generated 4-hydroxy-3-methoxybenzaldehyde (vanillin) in high yield, as well as other functionalised phenolic monomers up to 85% selectivity, illustrating the high susceptibility of Ru/α-HfP NPs towards C-O bond cleavage through reductive fractionation. Multiple recycling tests of the catalyst were performed without any apparent loss of activity. Overall, this report highlighted the potential of the synthesis strategy of the metal-acid supported catalyst to immediately depolymerise untreated biomass and can thus encourage the green, cost-efficient, large-scale production of intermediate chemicals.
A novel metal-acid strategy that affords dual functionalities in the one-pot fractionation of lignin to phenolic compounds with excellent selectivity. The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal–acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium phosphate nanoplates (α-HfP NPs) to effectively depolymerise lignocellulosic biomass. A native lignin fraction of pine lignocellulose was promptly depolymerised into 19.86 wt% yield (lignin based) of valuable phenolic monomers (with dihydroeugenol as the main compound with high selectivity) and few cyclic ketones through one-pot catalytic reductive fractionation under mild conditions (190 °C, 3.5 MPa H 2 ). Detailed scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and temperature-programmed desorption ammonia investigation correlated with the obtained results revealed that the metal–acid synergistic influence and the presence of Brønsted acid sites in the support for dehydration and the well-dispersed metallic role of Ru NCs for hydrodeoxygenation were responsible for the cleavage of lignin–carbohydrate (ester and ether linkages) bonds. Moreover, treating commercial lignin as a substrate in an organic solvent generated 4-hydroxy-3-methoxybenzaldehyde (vanillin) in high yield, as well as other functionalised phenolic monomers up to 85% selectivity, illustrating the high susceptibility of Ru/α-HfP NPs towards C–O bond cleavage through reductive fractionation. Multiple recycling tests of the catalyst were performed without any apparent loss of activity. Overall, this report highlighted the potential of the synthesis strategy of the metal–acid supported catalyst to immediately depolymerise untreated biomass and can thus encourage the green, cost-efficient, large-scale production of intermediate chemicals. The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal–acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium phosphate nanoplates (α-HfP NPs) to effectively depolymerise lignocellulosic biomass. A native lignin fraction of pine lignocellulose was promptly depolymerised into 19.86 wt% yield (lignin based) of valuable phenolic monomers (with dihydroeugenol as the main compound with high selectivity) and few cyclic ketones through one-pot catalytic reductive fractionation under mild conditions (190 °C, 3.5 MPa H2). Detailed scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and temperature-programmed desorption ammonia investigation correlated with the obtained results revealed that the metal–acid synergistic influence and the presence of Brønsted acid sites in the support for dehydration and the well-dispersed metallic role of Ru NCs for hydrodeoxygenation were responsible for the cleavage of lignin–carbohydrate (ester and ether linkages) bonds. Moreover, treating commercial lignin as a substrate in an organic solvent generated 4-hydroxy-3-methoxybenzaldehyde (vanillin) in high yield, as well as other functionalised phenolic monomers up to 85% selectivity, illustrating the high susceptibility of Ru/α-HfP NPs towards C–O bond cleavage through reductive fractionation. Multiple recycling tests of the catalyst were performed without any apparent loss of activity. Overall, this report highlighted the potential of the synthesis strategy of the metal–acid supported catalyst to immediately depolymerise untreated biomass and can thus encourage the green, cost-efficient, large-scale production of intermediate chemicals. |
Author | Odda, Atheer Hameid Fang, Xiao-Xiang Ullah, Naseeb Ma, Liu-Bo Kombo, Miza Ali Liang, Kuang Sahar, Shafaq Xu, An-Wu |
AuthorAffiliation | Division of Nanomaterials and Chemistry University of Science and Technology of China Hefei National Laboratory for Physical Sciences at the Microscale |
AuthorAffiliation_xml | – name: University of Science and Technology of China – name: Division of Nanomaterials and Chemistry – name: Hefei National Laboratory for Physical Sciences at the Microscale |
Author_xml | – sequence: 1 givenname: Naseeb surname: Ullah fullname: Ullah, Naseeb – sequence: 2 givenname: Atheer Hameid surname: Odda fullname: Odda, Atheer Hameid – sequence: 3 givenname: Kuang surname: Liang fullname: Liang, Kuang – sequence: 4 givenname: Miza Ali surname: Kombo fullname: Kombo, Miza Ali – sequence: 5 givenname: Shafaq surname: Sahar fullname: Sahar, Shafaq – sequence: 6 givenname: Liu-Bo surname: Ma fullname: Ma, Liu-Bo – sequence: 7 givenname: Xiao-Xiang surname: Fang fullname: Fang, Xiao-Xiang – sequence: 8 givenname: An-Wu surname: Xu fullname: Xu, An-Wu |
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Notes | Electronic supplementary information (ESI) available: FT-IR spectrum, XPS spectra of P 2p and Ru 3p of the Ru/α-HfP catalyst, N adsorption-desorption isotherm, BJH pore-size distribution, TGA/DTG analysis of the α-HfP sample, schematic structural representation of α-HfP, elements determined by ICP-MS analysis, FTIR spectra of pine sawdust and solid residue. SEM images and XRD patterns of the recycled Ru/α-HfP nanoplate sample, substrate analysis, bio-oil product analysis. See DOI 2 10.1039/c8gc03440k |
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SubjectTerms | Acids Alcohols Ammonia Biomass Carbohydrates Catalysis Catalysts Chemicals Cleavage Dehydration Desorption Fractionation Green chemistry Hafnium Ketones Lignin Lignocellulose Metals Monomers Nanoclusters Nanocomposites Organic chemistry Phenolic compounds Phenols Photoelectron spectroscopy Photoelectrons Sawdust Scanning electron microscopy Selectivity Size distribution Spectrum analysis Substrates Transmission electron microscopy Ultrafines Vanillin X ray photoelectron spectroscopy |
Title | Metal-acid nanoplate-supported ultrafine Ru nanoclusters for efficient catalytic fractionation of lignin into aromatic alcohols |
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