期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 305, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121072
关键词
Selective electrooxidation; 5-hydroxymethylfurfural; Hydrogen production; NiOOH species; Operando technologies
资金
- National Natural Science Foundation of China (NSFC) [22076140, 21876128, 22071146]
- Shanghai Science and Technology Committee [20520711600]
- SJTU-MPI partner group
- National Key Basic Research Program of China [2017YFA0403402]
- National Natural Science Foundation of China [U1932119]
- Shanghai Large Scientific Facilities Center
Replacing water oxidation with the selective electrochemical conversion of HMF to FDCA is an efficient strategy to promote hydrogen production. High selectivity and Faradaic efficiency were achieved using a NiCo2O4 electrode, with the amount of generated hydrogen through coupling with HMF oxidation significantly higher than that of water splitting. The main active species for the selective electrooxidation of HMF to FDCA was identified as NiOOH.
It is an efficient strategy to replace sluggish water oxidation with a thermodynamically more favorable reaction, electrochemical selective conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), to promote hydrogen production. High selectivity and Faradaic efficiency (> 99%) for the conversion of HMF to FDCA and simultaneous hydrogen production were achieved under 220 mV overpotential on NiCo2O4 electrode. The addition of HMF decreased the anode overpotential, and the amount of generated hydrogen through coupling with HMF oxidation is 8.16 times higher than that of water splitting. Operando Raman identified that NiOOH as the main active species for selective electrooxidation of HMF to FDCA. Operando EXAFS demonstrates that the crystal-strain induced formation of NiOOH from Co-Co bond and such a crystal strain could be further enhanced by the electric field for the in situ formation of more NiOOH. The accelerated reaction pathway was confirmed by operando electrochemical infrared (EC-IR) and DFT calculations.
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