Re-Doped Ni/TiO₂ Catalyst with Enhanced Active Site Dispersion and Optimized Adsorption Behavior for High-Efficiency Hydrogenation of Dimethyl Oxalate To Methyl Glycolate

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-10-18 DOI:10.1007/s10562-025-05203-5

Hao Wang, Ni Zhang, Jiang Gong, Fengling Zheng, Jianwei Li, Zhoulin Hu, Chuancai Zhang

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Abstract

The Ni-Re/TiO₂ catalyst was synthesized via the impregnation method, exhibiting exceptional catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG). With low Ni and Re loadings (2.5Ni0.5Re/TiO₂), the catalyst achieved 94% DMO conversion and 96% MG selectivity, maintaining impressive stability for over 200 h, highlighting its potential for industrial applications. Characterization studies demonstrated that Re doping promotes strong electronic interactions between Ni and Re, stabilizing and enhancing the dispersion of Ni nanoparticles, which facilitates H₂ activation. Concurrently, the presence of ReOx species introduces abundant Lewis acid sites, which enhance the adsorption and activation of C = O groups, thus facilitating DMO adsorption and dissociation. The superior catalytic performance arises from the synergistic interactions between ReOx and Ni species, providing valuable insights into the development of low-loading, high-activity catalysts for DMO hydrogenation.

Graphical Abstract

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重掺杂Ni/TiO 2催化剂活性位点分散性增强及对草酸二甲酯高效加氢制乙醇酸甲酯吸附行为的优化

采用浸渍法制备了Ni-Re/TiO2催化剂，对草酸二甲酯（DMO）加氢制乙醇酸甲酯（MG）表现出优异的催化性能。在低Ni和Re负载（2.5Ni0.5Re/TiO2）的情况下，该催化剂实现了94%的DMO转化率和96%的MG选择性，并在超过200小时的时间内保持了令人印象深刻的稳定性，突出了其工业应用潜力。表征研究表明，Re掺杂促进了Ni和Re之间的强电子相互作用，稳定并增强了Ni纳米粒子的分散性，有利于H2的活化。同时，ReOx物种的存在引入了丰富的Lewis酸位点，增强了C = O基团的吸附和活化，从而促进了DMO的吸附和解离。优异的催化性能源于ReOx和Ni之间的协同作用，为开发低负荷、高活性的DMO加氢催化剂提供了有价值的见解。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.