Catalytic Hydrogenolysis\nof Lignin into Propenyl-monophenol\nover Ru Single Atoms Supported on CeO<sub>2</sub> with Rich Oxygen\nVacancies

Lignin is the most abundant aromatic source of natural\nproducts,\nbut developing efficient catalysts to depolymerize it into valuable\nmonophenol with high yield and unique selectivity remains a challenge.\nHerein, we report a Ru single-atom catalyst (SAC) supported on rod\nCeO<sub>2</sub> with oxygen vacancies (Ov) for the depolymerization\nof birch dioxane acidolysis lignin (DAL). A near-theoretical maximum\nmonophenol yield (14.8 wt %) with good selectivity to 4-<i>n</i>-propenyl guaiacol (51.4%), as well as high catalyst stability, was\nachieved. The calculated turnover (TON) was 387 mol<sub>aromatics</sub>/mol<sub>Ru</sub>, which is 55× higher than that of the Ru/C\ncatalyst. The possible reaction for this catalyst was proposed by\nstudying a series of lignin model compounds and in situ DRIFT measurements.\nThe mechanism involves the cleavage of C<sub>α</sub>–OH\nand C<sub>β</sub>–O bonds to produce coniferyl alcohol,\nfollowed by the removal of γ-OH to generate 4-<i>n</i>-propenyl guaiacol. The effects of some key parameters like solvent,\nRu content, temperature, reaction time, and H<sub>2</sub> pressure\nwere also investigated in terms of monophenol yields and average molecular\nweight. This work provides an economically feasible method for the\ndepolymerization of lignin into highly valuable monophenols.

Publication Details

Journal
Figshare
Published
2024-10-17
DOI
https://doi.org/10.1021/acscatal.4c03184.s001
Primary Topic
Genetic Mapping and Diversity in Plants and Animals
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article

Catalytic Hydrogenolysis\nof Lignin into Propenyl-monophenol\nover Ru Single Atoms Supported on CeO2 with Rich Oxygen\nVacancies

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Genetic Mapping and Diversity in Plants and Animals
article

Catalytic Hydrogenolysis\nof Lignin into Propenyl-monophenol\nover Ru Single Atoms Supported on CeO2 with Rich Oxygen\nVacancies

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Abstract

Lignin is the most abundant aromatic source of natural\nproducts,\nbut developing efficient catalysts to depolymerize it into valuable\nmonophenol with high yield and unique selectivity remains a challenge.\nHerein, we report a Ru single-atom catalyst (SAC) supported on rod\nCeO<sub>2</sub> with oxygen vacancies (Ov) for the depolymerization\nof birch dioxane acidolysis lignin (DAL). A near-theoretical maximum\nmonophenol yield (14.8 wt %) with good selectivity to 4-<i>n</i>-propenyl guaiacol (51.4%), as well as high catalyst stability, was\nachieved. The calculated turnover (TON) was 387 mol<sub>aromatics</sub>/mol<sub>Ru</sub>, which is 55× higher than that of the Ru/C\ncatalyst. The possible reaction for this catalyst was proposed by\nstudying a series of lignin model compounds and in situ DRIFT measurements.\nThe mechanism involves the cleavage of C<sub>α</sub>–OH\nand C<sub>β</sub>–O bonds to produce coniferyl alcohol,\nfollowed by the removal of γ-OH to generate 4-<i>n</i>-propenyl guaiacol. The effects of some key parameters like solvent,\nRu content, temperature, reaction time, and H<sub>2</sub> pressure\nwere also investigated in terms of monophenol yields and average molecular\nweight. This work provides an economically feasible method for the\ndepolymerization of lignin into highly valuable monophenols.

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