Citation: Jiang Gong, Fengling Zheng, Hanqing Zhang, Weihan Shu, Hao Wang, Ni Zhang, Pengbing Huang, Chuancai Zhang, Bin Dai. The interfacial effect of SiO₂-Ni₃Mo₃N efficiently catalyzes the low-temperature hydrogenation of dimethyl oxalate to ethanol[J]. Chinese Chemical Letters, ;2025, 36(8): 111122. doi: 10.1016/j.cclet.2025.111122 shu

The interfacial effect of SiO₂-Ni₃Mo₃N efficiently catalyzes the low-temperature hydrogenation of dimethyl oxalate to ethanol

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School of Chemistry and Chemical Engineering / State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi 832003, China

zhangchuanc111@126.com

db_tea@shzu.edu.cn

Received Date: 21 November 2024
Revised Date: 18 March 2025
Accepted Date: 19 March 2025
Available Online: 20 March 2025

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The hydrogenation of dimethyl oxalate (DMO) to ethanol (EtOH) represents a promising avenue for syngas conversion and plays a pivotal role in advancing sustainable energy economies. Nevertheless, designing catalysts with high EtOH yields at low temperatures remains a significant challenge. This study introduces an efficient catalyst featuring a rich SiO₂-Ni₃Mo₃N interface, which achieved a remarkable 97.5% EtOH yield at 210 °C and 2 MPa. Impressively, an EtOH yield of 95% was also obtained at 210 °C and 1.5 MPa. The research demonstrates that the addition of SiO₂ fosters the development of a rich SiO₂-Ni₃Mo₃N interface, which enhances the concentration of Lewis acid sites (L-acid) and Brønsted acids sites (B-acid) within the catalyst. This enhancement promotes the adsorption of raw material and intermediate products while increasing H₂ adsorption, thereby boosting the catalyst's deep hydrogenation capacity. Density functional theory (DFT) simulations indicate that SiO₂ incorporation modifies the catalyst's metal d-band center through electron transfer, increasing its adsorption capability for raw materials and intermediates and facilitating EtOH production. Consequently, this study achieves high EtOH yields at low temperatures, advances the industrialization process of syngas to EtOH conversion, and offers novel insights into constructing highly active catalytic interfaces for DMO hydrogenation.
- Dimethyl oxalate,
- Ethanol,
- SiO₂-Ni₃Mo₃N interface,
- Low temperature,
- Acid sites,
- d-band center
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沈阳化工大学材料科学与工程学院沈阳 110142

The interfacial effect of SiO2-Ni3Mo3N efficiently catalyzes the low-temperature hydrogenation of dimethyl oxalate to ethanol

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通讯作者: 陈斌, bchen63@163.com

The interfacial effect of SiO₂-Ni₃Mo₃N efficiently catalyzes the low-temperature hydrogenation of dimethyl oxalate to ethanol