期刊
CHEMICAL ENGINEERING JOURNAL
卷 478, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2023.147288
关键词
Selective methanol oxidation; Oxygen vacancies; Methanol-assisted water electrolysis; Cold plasma
This study develops a high-performance Pt-free electrocatalyst for the electro-oxidation of methanol into high-value-added formate in alkaline media. The electrocatalyst, treated by an O-2 cold plasma, exhibits efficient formate electrosynthesis. Additionally, a coupled reaction system of methanol electro-oxidation and hydrogen evolution is established, further improving the energy conversion efficiency.
Developing high-performance Pt-free electrocatalysts for the electro-oxidation of methanol (MeOH) into highvalue-added formate in alkaline media offers a sustainable avenue for synchronous biomass valorization and MeOH oxidation-assisted hydrogen production. Herein, electrodeposited Co(OH)(2) on Ni foam (NF) was treated by an O-2 cold plasma to obtain oxygen vacancies enriched Co3O4-x/NF-P. The resultant Co3O4-x/NF-P only requires a potential of 1.318 V vs. RHE to upgrade MeOH into formate at 10 mA center dot cm(-2). Characterization and calculation results reveal that oxygen vacancy induced irreversible phase transformation of Co3O4-x/NF-P, facilitating the deprotonation of MeOH, and suppressing further oxidation of HCOO* for selective and efficient formate electrosynthesis. Impressively, a Co3O4-x/NF-P||Co3O4-x/NF-P pair was built to couple the MeOH electrooxidation with H-2 evolution, where it only supplies a cell voltage of 1.540 V at 10 mA center dot cm(-2) and the anodic Faraday efficiency exceeds 95 %. This work clarifies in-depth insight the underlying mechanism of MeOH selective oxidation into formate.
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