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Electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural and furfural over oxygen vacancy-rich NiCoMn-layered double hydroxides nanosheets

DOI: 10.1039/D1GC00901J DOI Help

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

Type: Journal Paper
Journal: Green Chemistry

State: Published (Approved)
Published: April 2021
Diamond Proposal Number(s): 19850

Abstract: Rational design of low-cost and active electrocatalysts is crucial for upgrading of biomass-derived chemicals into value-added products. Here, we report highly efficient catalysts of ternary NiCoMn-layered double hydroxides (NiCoMn-LDHs) nanosheets which are oxygen vacancy-rich, produced under controllable conditions for the electrocatalytic oxidation of both biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) and furfural to furoic acid (FurAc) in mild conditions, respectively. Electrochemical tests showed that the oxidation of HMF and furfural were preferential over the oxidation of water at the lower applied potentials with NiCoMn-LDHs catalysts. The high yields of FDCA (91.7%) and FurAc (92.4%) were achieved in 2.5 h using 1.15 nm thick NiCoMn-LDHs nanosheets with a NiCo:Mn ratio of 2:1 at 35 oC and atmospheric pressure. The mechanism for the superior performance, high durability, and good Faradaic efficiency of the catalysts has been elucidated by a comprehensive characterization, which confirmed the ultrathin nanosheets expose more Co-NiOOH active sites with oxygen vacancies, facilitating the synergistic effect between HMF as well as furfural oxidation reaction on Co-Ni and Mn2+ states. The oxygen vacancy-rich NiCoMn-LDHs nanosheets catalysts present a novel and energy-efficient solution to achieve a high yield of value-added chemicals from renewable sources.

Subject Areas: Chemistry, Environment

Instruments: B18-Core EXAFS , B22-Multimode InfraRed imaging And Microspectroscopy

Added On: 06/05/2021 08:55

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Inorganic Chemistry Nanoscience/Nanotechnology

Technical Tags:

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