ZIF-67-derived FeCoNi-LDH with a 3D nanoflower hierarchical structure for highly efficient oxidation of 5-Hydroxymethylfurfural and coupling seawater splitting hydrogen production

CHEMICAL ENGINEERING JOURNAL(2024)

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摘要
To achieve clean and sustainable energy development, the thermodynamically favourable electrocatalytic oxidation reaction of biomass derivatives can be combined with electrolysis for hydrogen production. This process simultaneously generates high-value 2,5-furandicarboxylic acid and green energy (i.e., hydrogen). The present thesis focuses on the synthesis of a novel Fe-Co-Ni nanosheet catalyst foam using impregnation methods and one-pot hydrothermal techniques. Subsequently, the 3D nanoflower FeCoNi-S@NF catalysts are subsequently prepared by sulfurizing the FeCoNi-LDH@NF precursors. These catalysts were then employed for electrolytic seawater hydrogen production coupled with the electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR). This strategy is expected to address the slow kinetics of the oxygen evolution reaction (OER). The 3D nanoflower structure of the FeCoNi-S@NF catalyst enhances the exposure of catalytically active sites, while sulfur doping further improves the electron transfer ability. At a low reaction potential of 1.45 V vs. RHE, FeCoNi-S@NF exhibited remarkable performance with a 95.68 % conversion rate for 5-hydroxymethylfurfural (HMF), a 94.83 % yield for 2,5-furandicarboxylic acid (FDCA), and a Faraday efficiency of 94.71 %. Furthermore, FeCoNi-S@NF exhibits a remarkable response in terms of hydrogen evolution in seawater. By utilizing HMFOR as the anodic reaction and low-cost seawater as the cathodic electrolyte for the hydrogen evolution reaction (HER), simultaneous biomass upgrading and hydrogen production can be achieved. Incorporating HMFOR into a two-electrode system for the electrolytic seawater hydrogen production process significantly reduces the needed voltage (1.70 V@10 mA cm-2), thereby potentially decreasing the cost of this process.
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关键词
Zeolitic imidazolate framework,5-hydroxymethylfurfural,Coupled oxidation,Overall seawater splitting,Hydrogen production
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