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用于硝基苯加氢的高效、玻碳泡沫负载钯催化剂的研制

Development of Highly Efficient, Glassy Carbon Foam Supported, Palladium Catalysts for Hydrogenation of Nitrobenzene.

作者信息

Prekob Ádám, Udayakumar Mahitha, Karacs Gábor, Kristály Ferenc, Muránszky Gábor, Leskó Anett Katalin, Németh Zoltán, Viskolcz Béla, Vanyorek László

机构信息

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

Advanced Materials and Intelligent Technologies Higher Education and Industrial Cooperation Centre, University of Miskolc, H-3515 Miskolc-Egyetemváros, Hungary.

出版信息

Nanomaterials (Basel). 2021 Apr 29;11(5):1172. doi: 10.3390/nano11051172.

Abstract

Glassy carbon foam (GCF) catalyst supports were synthesized from waste polyurethane elastomers by impregnating them in sucrose solution followed by pyrolysis and activation (AC) using N and CO gas. The palladium nanoparticles were formed from Pd(NO). The formed palladium nanoparticles are highly dispersive because the mean diameters are 8.0 ± 4.3 (Pd/GCF), 7.6 ± 4.2 (Pd/GCF-AC1) and 4.4 ± 1.6 nm (Pd/GCF-AC2). Oxidative post-treatment by CO of the supports resulted in the formation of hydroxyl groups on the GCF surfaces, leading to a decrease in zeta potential. The decreased zeta potential increased the wettability of the GCF supports. This, and the interactions between -OH groups and Pd ions, decreased the particle size of palladium. The catalysts were tested in the hydrogenation of nitrobenzene. The non-treated, glassy-carbon-supported catalyst (Pd/GCF) resulted in a 99.2% aniline yield at 293 K and 50 bar hydrogen pressure, but the reaction was slightly slower than other catalysts. The catalysts on the post-treated (activated) supports showed higher catalytic activity and the rate of hydrogenation was higher. The maximum attained aniline selectivities were 99.0% (Pd/GCF-AC1) at 293 K and 98.0% (Pd/GCF-AC2) at 323 K.

摘要

玻璃碳泡沫(GCF)催化剂载体由废弃聚氨酯弹性体制备而成,具体方法是将其浸渍在蔗糖溶液中,随后进行热解,并使用氮气和一氧化碳气体进行活化(AC)。钯纳米颗粒由硝酸钯(Pd(NO))形成。所形成的钯纳米颗粒具有高度分散性,因为其平均直径分别为8.0±4.3(Pd/GCF)、7.6±4.2(Pd/GCF - AC1)和4.4±1.6纳米(Pd/GCF - AC2)。载体经一氧化碳氧化后处理导致GCF表面形成羟基,从而使zeta电位降低。降低的zeta电位增加了GCF载体的润湿性。这以及-OH基团与钯离子之间的相互作用减小了钯的粒径。对这些催化剂进行了硝基苯加氢测试。未经处理的玻璃碳负载催化剂(Pd/GCF)在293 K和50巴氢气压力下苯胺产率为99.2%,但反应速度比其他催化剂稍慢。后处理(活化)载体上的催化剂表现出更高的催化活性,加氢速率更高。在293 K时,最大苯胺选择性为99.0%(Pd/GCF - AC1),在323 K时为98.0%(Pd/GCF - AC2)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be0f/8146346/cf6e3f8e35c0/nanomaterials-11-01172-g001.jpg

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