The Effect of Precursor Temperature on the Surface and Interface Structure of Ni/ZSM-5 Hydrogenation Catalyst

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-04-04 DOI:10.1007/s10562-025-05004-w

Guixian Li, Pengju Lei, Guang Chen, Xinhong Zhao, Zhibin Liu, Shoudeng Wang, Jichong Xia, Chengrong Kong, Dong Ji, Hongwei Li

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Abstract

A series of Ni/ZSM-5 catalysts with different physical and chemical properties were prepared by immersion-precipitation method by adjusting the temperature of the precursor. The structure and properties of the catalyst were characterized by XRD, TEM, N₂ adsorption-desorption, H₂-TPR, NH₃-TPD and XPS. The influence of precursor temperature on the hydrogenation performance of m-dinitrobenzene was investigated, and the effects of reaction temperature and hydrogen pressure on the reaction were also examined, as well as the stability of the optimal catalyst. The results show that the particle size reduces gradually and the dispersion degree of Ni nanoparticles on ZSM-5 support becomes better as the precursor temperature is increased, which is conducive to improving the catalytic reaction rate. When the precursor temperature was 60 °C, the reaction temperature was 115 °C, the hydrogen pressure was 2.6 MPa, and a mixed solvent of ethanol and deionized water was employed. After 10 min of reaction, both the conversion rate of m-dinitrobenzene and the selectivity of m-phenylenediamine reached 100%. Under the same conditions, the conversion rate of m-dinitrobenzene was 44.73% and the selectivity of m-phenylenediamine was 9.83% after 60 min of reaction for Raney-Ni. The catalyst in this study not only saves solvent costs but also exhibits excellent catalytic performance in tests. After ten cycles of the catalyst, the conversion rate of m-dinitrobenzene was 100%, and the selectivity of m-phenylenediamine was 97.66%.

Graphical Abstract

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前驱体温度对Ni/ZSM-5加氢催化剂表面和界面结构的影响

通过调节前驱体温度，采用浸没-沉淀法制备了一系列具有不同理化性能的Ni/ZSM-5催化剂。采用XRD、TEM、N2吸附-脱附、H2-TPR、NH3-TPD和XPS对催化剂的结构和性能进行了表征。考察了前驱体温度对间二硝基苯加氢性能的影响，考察了反应温度和氢气压力对反应的影响，以及最佳催化剂的稳定性。结果表明：随着前驱体温度的升高，Ni纳米颗粒在ZSM-5载体上的分散程度逐渐减小，有利于提高催化反应速率；前驱体温度为60℃，反应温度为115℃，氢气压力为2.6 MPa，溶剂为乙醇和去离子水。反应10 min后，间二硝基苯的转化率和间苯二胺的选择性均达到100%。在相同条件下，反应60 min后，间二硝基苯的转化率为44.73%，间苯二胺的选择性为9.83%。本研究的催化剂不仅节省了溶剂成本，而且在试验中表现出优异的催化性能。催化剂循环10次后，间二硝基苯的转化率为100%，对间苯二胺的选择性为97.66%。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.