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Designed TiS 2 nanosheets for efficient electrocatalytic reductive amination of biomass-derived furfurals

DOI: 10.1039/D2GC03234A DOI Help

Authors: Man Zhang (Sun Yat-sen University) , Shaojun Xu (Cardiff University; K Catalysis Hub, Research Complex at Harwell) , Mebrouka Boubeche (Sun Yat-sen University) , Donato Decarolis (Cardiff University; UK Catalysis Hub, Research Complex at Harwell) , Yizhe Huang (Sun Yat-sen University) , Biying Liu (Sun Yat-sen University) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Xin Li (Sun Yat-sen University) , Yuchen Wang (Sun Yat-sen University) , Huixia Luo (Sun Yat-sen University) , C. Richard A. Catlow (Cardiff University; UK Catalysis Hub, Research Complex at Harwell; University College London) , Kai Yan (Sun Yat-sen University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Green Chemistry , VOL 9

State: Published (Approved)
Published: November 2022
Diamond Proposal Number(s): 19850

Abstract: Green and highly selective synthesis of organonitrogen chemicals (ONCs) using the renewable energy source biomass over noble-metal free solid catalysts under common room temperature and pressure conditions is still a major challenge. Here, we report a sustainable electrochemical method for selective synthesis of several valuable ONCs with high yields using biomass-derived furanic aldehydes over greenly fabricated TiS2 nanosheets through a facile synthesis. Based on a range of characterization techniques including high-resolution transmission electron microscopy and X-ray absorption fine structure, a well-defined structure of the TiS2 nanosheets (3.86 nm with 1T phase) was constructed. These as-prepared catalysts were applied to the electrochemical reductive amination (ERA) of three biomass-derived aldehydes, i.e. furfural (FF), 5-methylfurfural (MF) and 5-hydroxymethylfurfural (HMF), and exhibited superior performance whereby over 95% conversion of each furanic aldehyde and nearly perfect selectivity of ONCs were achieved. TiS2 nanosheets, in particular, exhibited a marked ∼2-fold increase in conversion (∼49%) compared with the monometallic Ti electrode. Besides, the reaction kinetics and rational pathway were also studied. In addition, these exfoliated TiS2 nanosheets maintained high durability over 6 h, providing a promising and versatile route for the sustainable upgrading of biomass-derived sources.

Subject Areas: Chemistry, Environment

Instruments: B18-Core EXAFS

Added On: 17/11/2022 10:32

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)