Selective Hydrodeoxygenation of γ -Valerolactone over Silica-supported Rh-based Bimetallic Catalysts

Xin Huang; Shinji Kudo; U. P.M. Ashik; Hisahiro Einaga; Jun Ichiro Hayashi

doi:10.1021/acs.energyfuels.0c01290

Selective Hydrodeoxygenation of γ -Valerolactone over Silica-supported Rh-based Bimetallic Catalysts

Xin Huang, Shinji Kudo, U. P.M. Ashik, Hisahiro Einaga, Jun Ichiro Hayashi

Research output: Contribution to journal › Article › peer-review

11 Citations (Scopus)

Abstract

2-Methyltetrahydrofuran (2-MTHF) is a promising fuel additive and renewable solvent. Herein, we report a selective hydrodeoxygenation of cellulose-derived γ-valerolactone (GVL) to 2-MTHF under mild conditions over silica-supported RhRe and RhMo bimetallic catalysts. RhMo/SiO2 showed the best performance for the target 2-MTHF with a high selectivity of 86% in heptane at 120 °C. The high catalytic performance of Rh-based catalyst was attributed to an acidity induced by the presence of additional metals such as Mo or Re. However, the acidity in aqueous phase was weaker than that in heptane, requiring additional acid sites. ZSM-5 performed best in combination with the bimetallic catalysts, resulting in the selectivity of 76% to 2-MTHF even in water at 120 °C. Moreover, a high reaction temperature (160 °C) caused hydrodeoxygenation of 2-MTHF and enabled perfectly selective production of alkanes with butane and pentane as predominant products.

Original language	English
Pages (from-to)	7190-7197
Number of pages	8
Journal	Energy and Fuels
Volume	34
Issue number	6
DOIs	https://doi.org/10.1021/acs.energyfuels.0c01290
Publication status	Published - Jun 18 2020

All Science Journal Classification (ASJC) codes

Chemical Engineering(all)
Fuel Technology
Energy Engineering and Power Technology

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acs.energyfuels.0c01290

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@article{57489759e7b541e18416a5c3aff4d43d,

title = "Selective Hydrodeoxygenation of γ -Valerolactone over Silica-supported Rh-based Bimetallic Catalysts",

abstract = "2-Methyltetrahydrofuran (2-MTHF) is a promising fuel additive and renewable solvent. Herein, we report a selective hydrodeoxygenation of cellulose-derived γ-valerolactone (GVL) to 2-MTHF under mild conditions over silica-supported RhRe and RhMo bimetallic catalysts. RhMo/SiO2 showed the best performance for the target 2-MTHF with a high selectivity of 86% in heptane at 120 °C. The high catalytic performance of Rh-based catalyst was attributed to an acidity induced by the presence of additional metals such as Mo or Re. However, the acidity in aqueous phase was weaker than that in heptane, requiring additional acid sites. ZSM-5 performed best in combination with the bimetallic catalysts, resulting in the selectivity of 76% to 2-MTHF even in water at 120 °C. Moreover, a high reaction temperature (160 °C) caused hydrodeoxygenation of 2-MTHF and enabled perfectly selective production of alkanes with butane and pentane as predominant products.",

author = "Xin Huang and Shinji Kudo and Ashik, {U. P.M.} and Hisahiro Einaga and Hayashi, {Jun Ichiro}",

note = "Funding Information: This work was financially supported by MEXT/JSPS KAKENHI (JP16K06845). A part of this work was also supported by the Cross-Ministerial Strategic Innovation Promotion Program (SIP) {"}Technologies for smart bio-industry and agriculture{"} administered by Bio-oriented Technology Research Advancement Institution, National Agriculture and Food Research Organization (NARO). Xin Huang thanks the China Scholarship Council (201606420055) for financial support. The authors are also grateful to the Cooperative Research Program of the “Network Joint Research Center for Materials and Devices”. Publisher Copyright: {\textcopyright} 2020 American Chemical Society.",

year = "2020",

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doi = "10.1021/acs.energyfuels.0c01290",

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T1 - Selective Hydrodeoxygenation of γ -Valerolactone over Silica-supported Rh-based Bimetallic Catalysts

AU - Huang, Xin

AU - Kudo, Shinji

AU - Ashik, U. P.M.

AU - Einaga, Hisahiro

AU - Hayashi, Jun Ichiro

N1 - Funding Information: This work was financially supported by MEXT/JSPS KAKENHI (JP16K06845). A part of this work was also supported by the Cross-Ministerial Strategic Innovation Promotion Program (SIP) "Technologies for smart bio-industry and agriculture" administered by Bio-oriented Technology Research Advancement Institution, National Agriculture and Food Research Organization (NARO). Xin Huang thanks the China Scholarship Council (201606420055) for financial support. The authors are also grateful to the Cooperative Research Program of the “Network Joint Research Center for Materials and Devices”. Publisher Copyright: © 2020 American Chemical Society.

PY - 2020/6/18

Y1 - 2020/6/18

N2 - 2-Methyltetrahydrofuran (2-MTHF) is a promising fuel additive and renewable solvent. Herein, we report a selective hydrodeoxygenation of cellulose-derived γ-valerolactone (GVL) to 2-MTHF under mild conditions over silica-supported RhRe and RhMo bimetallic catalysts. RhMo/SiO2 showed the best performance for the target 2-MTHF with a high selectivity of 86% in heptane at 120 °C. The high catalytic performance of Rh-based catalyst was attributed to an acidity induced by the presence of additional metals such as Mo or Re. However, the acidity in aqueous phase was weaker than that in heptane, requiring additional acid sites. ZSM-5 performed best in combination with the bimetallic catalysts, resulting in the selectivity of 76% to 2-MTHF even in water at 120 °C. Moreover, a high reaction temperature (160 °C) caused hydrodeoxygenation of 2-MTHF and enabled perfectly selective production of alkanes with butane and pentane as predominant products.

AB - 2-Methyltetrahydrofuran (2-MTHF) is a promising fuel additive and renewable solvent. Herein, we report a selective hydrodeoxygenation of cellulose-derived γ-valerolactone (GVL) to 2-MTHF under mild conditions over silica-supported RhRe and RhMo bimetallic catalysts. RhMo/SiO2 showed the best performance for the target 2-MTHF with a high selectivity of 86% in heptane at 120 °C. The high catalytic performance of Rh-based catalyst was attributed to an acidity induced by the presence of additional metals such as Mo or Re. However, the acidity in aqueous phase was weaker than that in heptane, requiring additional acid sites. ZSM-5 performed best in combination with the bimetallic catalysts, resulting in the selectivity of 76% to 2-MTHF even in water at 120 °C. Moreover, a high reaction temperature (160 °C) caused hydrodeoxygenation of 2-MTHF and enabled perfectly selective production of alkanes with butane and pentane as predominant products.

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Selective Hydrodeoxygenation of γ -Valerolactone over Silica-supported Rh-based Bimetallic Catalysts

Abstract

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