Citation: Tao Ban, Xi-Yang Yu, Hai-Kuo Tian, Zheng-Qing Huang, Chun-Ran Chang. One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts: A DFT study[J]. Chinese Chemical Letters, ;2024, 35(4): 108549. doi: 10.1016/j.cclet.2023.108549 shu

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

Tao Ban ^a ,
Xi-Yang Yu ^a ,
Hai-Kuo Tian ^a ,
Zheng-Qing Huang ^a ,
Chun-Ran Chang ^{a, b, *,}

a.
Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China
b.
Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization, School of Chemistry and Chemical Engineering, Yulin University, Yulin 719000, China

changcr@mail.xjtu.edu.cn

Received Date: 12 April 2023
Revised Date: 25 April 2023
Accepted Date: 8 May 2023
Available Online: 9 May 2023

Figures(4)

One-step conversion of methane and formaldehyde into ethanol is a 100% atom-efficient process for carbon resources utilization and environment protection but still faces eminent challenges due to the lacking 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 formaldehyde 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 573 K 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-atom,
- Frustrated Lewis pairs,
- Methane conversion,
- Dual active sites,
- Ethanol synthesis
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