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Efficient electrooxidation of biomass-derived aldehydes over ultrathin Ni V-layered double hydroxides films

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摘要 Selective upgrading of C=O bonds to afford carboxylic acid is significant for the petrochemical industry and biomass utilization.Here we declared the efficient electrooxidation of biomass-derived aldehydes family over NiV-layered double hydroxides(LDHs) thin films.Mechanistic studies confirmed the hydroxyl active intermediate(-OH*) generated on the surface of NiV-LDHs films by employing electrochemical impedance spectroscopy and the electron paramagnetic resonance spectroscopy.By using advanced techniques,e.g.,extended X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy,NiV-LDHs films with 2.6 nm could expose larger specific surface area.Taking benzaldehyde as a model,high current density of 200 mA cm^(-2)at 1.8 V vs.RHE,81.1% conversion,77.6% yield of benzoic acid and 90.8% Faradaic efficiency were reached,which was superior to most of previous studies.Theoretical DFT analysis was well matched with experimental findings and documented that NiV-LDHs had high adsorption capacity for the aldehydes to suppress the side reaction,and the aldehydes were oxidized by the electrophilic hydroxyl radicals formed on NiV-LDHs.Our findings offer a universal strategy for the robust upgrading of diverse biomass-derived platform chemicals.
出处 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第3期412-421,I0012,共11页 能源化学(英文版)
基金 supported by the National Natural Science Foundation of China(22078374,21776324) the Scientific and Technological Planning Project of Guangzhou(202206010145) the National Ten Thousand Talent Plan,Key-Area Research and Development Program of Guangdong Province(2019B110209003) the Guangdong Basic and Applied Basic Research Foundation(2019B1515120058,2020A1515011149) the Start-up Fund for Senior Talents in Jiangsu University(21JDG060)。
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