Abstract
One-step conversion of methane and formaldehyde into ethanol is a 100％atom-efficient process for car-bon resources utilization and environment protection but still faces eminent challenges due to the lack-ing of efficient catalysts.Therefore,developing active and stable catalysts is crucial for the co-conversion of methane and formaldehyde.Herein,twelve kinds of"Single-Atom"-"Frustrated Lewis Pair"(SA-FLP)dual-active-site catalysts are designed for the direct conversion of methane and formaldehyde to ethanol based on density functional theory(DFT)calculations and microkinetic simulations.The results show that the SA-FLP dual active sites can simultaneously activate methane at the SA site and activate formalde-hyde at the FLP site.Among the twelve designed SA-FLP catalysts,Fe1-FLP shows the best performance in the co-conversion of methane and formaldehyde to ethanol with the rate-determining barrier of 1.15 eV.Ethanol is proved as the main product with the turnover frequency of 1.32 × 10-4 s-1 at 573K and 3 bar.This work provides a universal strategy to design dual active sites on metal oxide materials and offers new insights into the effective conversion of methane and formaldehyde to desired C2 chemicals.
基金项目
国家自然科学基金(22078257)
国家自然科学基金(22038011)
国家自然科学基金(22108213)
中国博士后科学基金(2021M692548)
Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2022001)
Young Talent Support Plan of Shaanxi Province()
NETL
NSTL
万方数据