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膨润土作为用于甲苯二胺合成的Pd/CoFeO催化剂的环保型天然矿物载体。

Bentonite as eco-friendly natural mineral support for Pd/CoFeO catalyst applied in toluene diamine synthesis.

作者信息

Hatvani-Nagy Alpár F, Hajdu Viktória, Ilosvai Ágnes Mária, Muránszky Gábor, Sikora Emőke, Kristály Ferenc, Daróczi Lajos, Viskolcz Béla, Fiser Béla, Vanyorek László

机构信息

Higher Education and Industrial Cooperation Centre, University of Miskolc, Miskolc-Egyetemváros, 3515, Hungary.

Institute of Chemistry, University of Miskolc, Miskolc-Egyetemváros, 3515, Hungary.

出版信息

Sci Rep. 2024 Feb 20;14(1):4193. doi: 10.1038/s41598-024-54792-5.

Abstract

Toluene diamine (TDA) is a major raw material in the polyurethane industry and thus, its production is highly important. TDA is obtained through the catalytic hydrogenation of 2,4-dinitrotoluene (2,4-DNT). In this study a special hydrogenation catalyst has been developed by decomposition cobalt ferrite nanoparticles onto a natural clay-oxide nanocomposite (bentonite) surface using a microwave-assisted solvothermal method. The catalyst particles were examined by TEM and X-ray diffraction. The palladium immobilized on the bentonite crystal surface was identified using an XRD and HRTEM device. The obtained catalyst possesses the advantageous property of being easily separable due to its magnetizability on a natural mineral support largely available and obtained through low carbon- and energy footprint methods. The catalyst demonstrated outstanding performance with a 2,4-DNT conversion rate exceeding 99% along with high yields and selectivity towards 2,4-TDA and all of this achieved within a short reaction time. Furthermore, the developed catalyst exhibited excellent stability, attributed to the strong interaction between the catalytically active metal and its support. Even after four cycles of reuse, the catalytic activity remained unaffected and the Pd content of the catalyst did not change, which indicates that the palladium component remained firmly attached to the magnetic support's surface.

摘要

甲苯二胺(TDA)是聚氨酯工业中的一种主要原料,因此其生产至关重要。TDA是通过2,4-二硝基甲苯(2,4-DNT)的催化氢化制得的。在本研究中,采用微波辅助溶剂热法将钴铁氧体纳米颗粒分解到天然粘土氧化物纳米复合材料(膨润土)表面,开发了一种特殊的氢化催化剂。通过透射电子显微镜(TEM)和X射线衍射对催化剂颗粒进行了检测。使用X射线衍射仪(XRD)和高分辨率透射电子显微镜(HRTEM)设备鉴定了固定在膨润土晶体表面的钯。所制备的催化剂具有易于分离的优点,这是由于其在天然矿物载体上具有磁性,该载体大量可得且通过低碳和低能耗方法制备。该催化剂表现出优异的性能,2,4-DNT转化率超过99%,同时对2,4-TDA具有高收率和选择性,且所有这些均在短反应时间内实现。此外,所开发的催化剂表现出优异的稳定性,这归因于催化活性金属与其载体之间的强相互作用。即使经过四个循环的重复使用,催化活性仍未受影响,且催化剂的钯含量未发生变化,这表明钯组分牢固地附着在磁性载体表面上。

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