首页|One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts:A DFT study

One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts:A DFT study

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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.

Single-atomFrustrated Lewis pairsMethane conversionDual active sitesEthanol synthesis

Tao Ban、Xi-Yang Yu、Hai-Kuo Tian、Zheng-Qing Huang、Chun-Ran Chang

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Shaanxi Key Laboratory of Energy Chemical Process Intensification,School of Chemical Engineering and Technology,Xi'an Jiaotong University,Xi'an 710049,China

Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization,School of Chemistry and Chemical Engineering,Yulin University,Yulin 719000,China

国家自然科学基金国家自然科学基金国家自然科学基金中国博士后科学基金Joint Fund of the Yulin University and the Dalian National Laboratory for Clean EnergyYoung Talent Support Plan of Shaanxi Province

2207825722038011221082132021M692548YLU-DNL Fund 2022001

2024

10.1016/j.cclet.2023.108549

中国化学快报(英文版)
中国化学会

中国化学快报(英文版)

CSTPCD
影响因子：0.771
ISSN：1001-8417
年,卷(期)：2024.35(4)
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