Effect of the Proton Transfer Pathway on Selective Photoreforming of Lignin Models for Target Products Enabled by Sulfur Vacancy Engineering on Chalcogenide Nanosheets
ENERGY & FUELS（2023）
Edith Cowan Univ
Abstract
Photoreformingof lignin has been explored as a fascinating technologyto generate clean hydrogen energy and value-added aromatic monomersfrom biomass. However, its upscaling is impeded by unsatisfactoryselectivity due to the lack of mechanistic investigations in the uncontrollablereaction pathways. Herein, we successfully controlled the concentrationand position of sulfur vacancies within the ultrathin ZnIn2S4 nanosheets to optimize the photo-driven lignin modelreforming process. The competition of proton transfer between thehydrogen evolution and dissociation of the beta-O-4 linkage inthe model compound of lignin was identified, and the modulation ofthe proton migration pathway was realized through S vacancy engineeringin ZnIn2S4 nanosheets toward target products.As such, excellent selectivity for hydrogen and chemical monomerswas achieved with a high concentration of S vacancies in the bulkand on the surface of ZnIn2S4, respectively.This study endows new mechanistic insights into the biomass photoreformingprocess and elucidates the structure/chemistry-catalysis correlationof ZnIn2S4 photocatalysts, which are beneficialfor photocatalyst design and rational solar fuel production.
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Lignin Valorization
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