化学
催化作用
草酸
激进的
草酸盐
过氧化氢
化学工程
等离子体
光化学
无机化学
化学物理
有机化学
量子力学
物理
工程类
作者
Tianqi Zhang,Josip Knežević,Mengying Zhu,Jungmi Hong,Rusen Zhou,Sheng Qiang,Luyao Ding,Jing Sun,Dingxin Liu,Kostya Ken Ostrikov,Renwu Zhou,Patrick J. Cullen
摘要
By inducing CO2-pulsed discharges within microchannel bubbles and regulating thus-forming plasma microbubbles, we observe high-performance, catalyst-free coformation of hydrogen peroxide (H2O2) and oxalate directly from CO2 and water. With isotope-labeled C18O2 as the feedstock, peaks of H218O16O and H216O2 observed by ex situ surface-enhanced Raman spectra indicate that single-atom oxygen (O) from CO2 dissociations and H2O-derived OH radicals both contribute to H2O2 formation. The global plasma chemistry modeling suggests that high-density, energy-intense electron supply enables high-density CO2- (aq) and HCO2- (aq) formation and their subsequent coupling to produce oxalate. The enhanced solvation of CO2, facilitated by the efficient transport of CxOy ionic species and CO, is demonstrated as a crucial benefit of spark discharges interacting with water at the bubble interface. We expect this plasma microbubble approach to provide a novel power-to-chemical avenue to convert CO2 into valuable H2O2 and oxalic acid platform chemicals, thus leveraging renewable energy resources.
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