MoS2-catalyzed selective electrocatalytic hydrogenation of aromatic aldehydes in an aqueous environment

The development of an active earth-abundant metal electrocatalyst for biomass-derived organic materials valorization can greatly benefit the growth of a sustainable biorefinery. Herein, we report a transition metal dichalcogenide catalyst, MoS2, as a great electrocatalytic hydrogenation catalyst in...

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Bibliographic Details
Published in:Green chemistry : an international journal and green chemistry resource : GC 2022-10, Vol.24 (20), p.7974-7987
Main Authors: Huang, Shuquan, Jin, Yangxin, Zhang, Man, Yan, Kai, Shien-Ping Feng, Jason Chun-Ho Lam
Format: Article
Language:English
Subjects:
Aldehydes
Aqueous environments
Base metal
Biorefineries
Carbonyl compounds
Carbonyls
Catalysts
Deposition
Electrocatalysts
Electrolysis
Furfural
Furfuryl alcohol
Green chemistry
Heat treatment
Hydrogenation
Molybdenum disulfide
Organic materials
Selectivity
Substrates
Transition metal compounds
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Summary:The development of an active earth-abundant metal electrocatalyst for biomass-derived organic materials valorization can greatly benefit the growth of a sustainable biorefinery. Herein, we report a transition metal dichalcogenide catalyst, MoS2, as a great electrocatalytic hydrogenation catalyst in converting a highly versatile platform chemical furfural to furfuryl alcohol, with over 82.4% yield and 92.1% selectivity, and its catalytic performance surpassed those of 11 other base metal electrocatalysts. The durable layer of 1T-rich MoS2 was fabricated on a carbon cloth support via a novel seeded-solvothermal deposition, followed by a thermal treatment. Reaction mechanistic investigation via underpotential hydrogen desorption (HUPD) studies and substrate scope expansion showed that MoS2 delivered the mechanism in a stage-wise manner, where the reduction of the carbonyl occurred to yield a radical intermediate in the vicinity of the MoS2 catalyst, followed by an abstraction of a surface adsorbed hydrogen (Hads). The conversion of reactants benefited from the presence of electron-withdrawing substituents, and the product selectivity was inert to the influence of the substituents. The MoS2 can be prepared easily through electrocatalytic and solvothermal deposition. The resulting catalyst layer demonstrated great stability throughout the repeated application in bulk electrolysis.
ISSN:1463-9262
1463-9270
DOI:10.1039/d2gc02166h