乙烯
析氧
密度泛函理论
动力学
生产(经济)
氧气
催化作用
化学
材料科学
热力学
物理化学
计算化学
物理
电极
生物化学
量子力学
宏观经济学
经济
有机化学
电化学
作者
Guiji Liu,Michelle Lee,Soonho Kwon,Guosong Zeng,Johanna Eichhorn,Aya K. Buckley,F. Dean Toste,William A. Goddard,Francesca M. Toma
标识
DOI:10.1073/pnas.2012649118
摘要
We elucidate the role of subsurface oxygen on the production of C2 products from CO2 reduction over Cu electrocatalysts using the newly developed grand canonical potential kinetics density functional theory method, which predicts that the rate of C2 production on pure Cu with no O is ∼500 times slower than H2 evolution. In contrast, starting with Cu2O, the rate of C2 production is >5,000 times faster than pure Cu(111) and comparable to H2 production. To validate these predictions experimentally, we combined time-dependent product detection with multiple characterization techniques to show that ethylene production decreases substantially with time and that a sufficiently prolonged reaction time (up to 20 h) leads only to H2 evolution with ethylene production ∼1,000 times slower, in agreement with theory. This result shows that maintaining substantial subsurface oxygen is essential for long-term C2 production with Cu catalysts.
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