Enhancing H 2 O 2 Electrosynthesis at Industrial-Relevant Current in Acidic Media on Diatomic Cobalt Sites.
Helai HuangMingze SunShuwei LiShengbo ZhangYiyang LeeZhengwen LiJinjie FangChengjin ChenYu-Xiao ZhangYanfen WuYizhen CheShuairen QianWei ZhuCheng TangZhongbin ZhuangLiang ZhangZhiqiang NiuPublished in: Journal of the American Chemical Society (2024)
Electrocatalytic synthesis of hydrogen peroxide (H 2 O 2 ) in acidic media is an efficient and eco-friendly approach to produce inherently stable H 2 O 2 , but limited by the lack of selective and stable catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction to efficiently produce H 2 O 2 at 50-400 mA cm -2 in acid. Electrode kinetics study shows a >95% selectivity for two-electron oxygen reduction on the diatomic cobalt sites. In a flow cell device, a record-high production rate of 11.72 mol g cat -1 h -1 and exceptional long-term stability (100 h) are realized under high current densities. In situ spectroscopic studies and theoretical calculations reveal that introducing a second metal into the coordination sphere of the cobalt site can optimize the binding strength of key H 2 O 2 intermediates due to the downshifted d-band center of cobalt. We also demonstrate the feasibility of processing municipal plastic wastes through decentralized H 2 O 2 production.
Keyphrases
- reduced graphene oxide
- metal organic framework
- hydrogen peroxide
- carbon nanotubes
- wastewater treatment
- gold nanoparticles
- ionic liquid
- single cell
- heavy metals
- nitric oxide
- highly efficient
- sewage sludge
- genome wide
- dna methylation
- bone marrow
- risk assessment
- binding protein
- mesenchymal stem cells
- carbon dioxide
- electron microscopy
- structural basis