Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation
Hydrogen-free reductive catalytic fractionation (RCF) is a promising method to extract and depolymerize lignin from native biomass without the use of external hydrogen gas. Here, we show that Pt/C and Pd/C achieve comparable monomer yields regardless of hydrogen pressure, whereas Ru/C and Ni/C show...
| Main Authors: | , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
Royal Society of Chemistry (RSC)
2022
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| Online Access: | https://hdl.handle.net/1721.1/146874 |
| _version_ | 1826217041576591360 |
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| author | Kenny, Jacob K Brandner, David G Neefe, Sasha R Michener, William E Román-Leshkov, Yuriy Beckham, Gregg T Medlin, J Will |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Kenny, Jacob K Brandner, David G Neefe, Sasha R Michener, William E Román-Leshkov, Yuriy Beckham, Gregg T Medlin, J Will |
| author_sort | Kenny, Jacob K |
| collection | MIT |
| description | Hydrogen-free reductive catalytic fractionation (RCF) is a promising method to extract and depolymerize lignin from native biomass without the use of external hydrogen gas. Here, we show that Pt/C and Pd/C achieve comparable monomer yields regardless of hydrogen pressure, whereas Ru/C and Ni/C show lower yields under H2-free conditions. Ru/C and Ni/C primarily perform hydrodeoxygenation regardless of the hydrogen pressure, but Pt/C and Pd/C demonstrated the ability to form both ethyl products from dehydrogenation and propanol products through hydrogenation depending on the presence of external H2. Adding water to the solvent increased HDO selectivity to propyl products for both Pt/C and Pd/C. Monomer yields from poplar RCF showed similar trends in yield and selectivity to reactions with the model compound coniferyl alcohol, suggesting that H2-free RCF performance is dictated by the stabilization rate of reactive monomer intermediates. |
| first_indexed | 2024-09-23T16:57:23Z |
| format | Article |
| id | mit-1721.1/146874 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T16:57:23Z |
| publishDate | 2022 |
| publisher | Royal Society of Chemistry (RSC) |
| record_format | dspace |
| spelling | mit-1721.1/1468742022-12-15T03:01:14Z Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation Kenny, Jacob K Brandner, David G Neefe, Sasha R Michener, William E Román-Leshkov, Yuriy Beckham, Gregg T Medlin, J Will Massachusetts Institute of Technology. Department of Chemical Engineering Hydrogen-free reductive catalytic fractionation (RCF) is a promising method to extract and depolymerize lignin from native biomass without the use of external hydrogen gas. Here, we show that Pt/C and Pd/C achieve comparable monomer yields regardless of hydrogen pressure, whereas Ru/C and Ni/C show lower yields under H2-free conditions. Ru/C and Ni/C primarily perform hydrodeoxygenation regardless of the hydrogen pressure, but Pt/C and Pd/C demonstrated the ability to form both ethyl products from dehydrogenation and propanol products through hydrogenation depending on the presence of external H2. Adding water to the solvent increased HDO selectivity to propyl products for both Pt/C and Pd/C. Monomer yields from poplar RCF showed similar trends in yield and selectivity to reactions with the model compound coniferyl alcohol, suggesting that H2-free RCF performance is dictated by the stabilization rate of reactive monomer intermediates. 2022-12-14T16:54:47Z 2022-12-14T16:54:47Z 2022-08-16 2022-12-14T15:11:52Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/146874 Kenny, Jacob K, Brandner, David G, Neefe, Sasha R, Michener, William E, Román-Leshkov, Yuriy et al. 2022. "Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation." Reaction Chemistry & Engineering, 7 (12). en 10.1039/d2re00275b Reaction Chemistry & Engineering Creative Commons Attribution 3.0 unported license https://creativecommons.org/licenses/by/3.0/ application/pdf Royal Society of Chemistry (RSC) Royal Society of Chemistry (RSC) |
| spellingShingle | Kenny, Jacob K Brandner, David G Neefe, Sasha R Michener, William E Román-Leshkov, Yuriy Beckham, Gregg T Medlin, J Will Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title | Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title_full | Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title_fullStr | Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title_full_unstemmed | Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title_short | Catalyst choice impacts aromatic monomer yields and selectivity in hydrogen-free reductive catalytic fractionation |
| title_sort | catalyst choice impacts aromatic monomer yields and selectivity in hydrogen free reductive catalytic fractionation |
| url | https://hdl.handle.net/1721.1/146874 |
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