期刊
ADVANCED MATERIALS
卷 34, 期 2, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202107185
关键词
biomass upgrading; electrocatalysts; oxygen vacancy; spinel oxide
类别
资金
- National Key R&D Program of China [2020YFA0710000]
- National Natural Science Foundation of China [22122901, 21902047, 21825201, U19A2017]
- Provincial Natural Science Foundation of Hunan [2020JJ5045]
The electrooxidation of 5-hydroxymethylfurfural (HMF) provides a green route to obtain high-value chemicals from biomass. The study reveals the adsorption behavior of HMF and OH- on Co3O4, with oxygen vacancy playing a crucial role. Modulating adsorption sites leads to excellent activity for the HMFOR process.
The electrooxidation of 5-hydroxymethylfurfural (HMF) offers a promising green route to attain high-value chemicals from biomass. The HMF electrooxidation reaction (HMFOR) is a complicated process involving the combined adsorption and coupling of organic molecules and OH- on the electrode surface. An in-depth understanding of these adsorption sites and reaction processes on electrocatalysts is fundamentally important. Herein, the adsorption behavior of HMF and OH-, and the role of oxygen vacancy on Co3O4 are initially unraveled. Correspondingly, instead of the competitive adsorption of OH- and HMF on the metal sites, it is observed that the OH- can fill into oxygen vacancy (Vo) prior to couple with organic molecules through lattice oxygen oxidation reaction process, which could accelerate the rate-determining step of the dehydrogenation of 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) intermediates. With the modulated adsorption sites, the as-designed Vo-Co3O4 shows excellent activity for HMFOR with the earlier potential of 90 and 120 mV at 10 mA cm(-2) in 1 m KOH and 1 m PBS solution. This work sheds insight on the catalytic mechanism of oxygen vacancy, which benefits designing a novel electrocatalysts to modulate the multi-molecules combined adsorption behaviors.
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