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Nanoreactors based on hydrophobized tubular aluminosilicates decorated with ruthenium: highly active and stable catalysts for aromatics hydrogenation
Catalysis Today ( IF 5.3 ) Pub Date : 2020-10-12 , DOI: 10.1016/j.cattod.2020.10.001
Aleksandr Glotov , Andrei Novikov , Anna Stavitskaya , Vladimir Nedolivko , Dmitry Kopitsyn , Alexandra Kuchierskaya , Evgenii Ivanov , Valentine Stytsenko , Vladimir Vinokurov , Yuri Lvov

Industrial hydrogenation catalysts must be not only selective and active but also resistant to feedstock impurities, including water. We report the strategy of preparing catalytic core-shell nanoreactors based on hydrophobized aluminosilicate nanotubes loaded with ruthenium. The modification of halloysite with alkyltriethoxysilanes enhances hydrophobicity of the clay nanotubes (water contact angle up to 122°) and enables their selective loading with 4-nm ruthenium particles. Such a core-shell tubular nanoreactors provide shielding of active sites from deactivation by admixed water and prevent metal leaching. Produced mesoscale catalysts were active in the hydrogenation of aromatics both in organic and aqueous media at 80 °C and a hydrogen pressure of 3 MPa. Benzene hydrogenation in the biphasic system with water resulted in a complete conversion with 100% selectivity to cyclohexane over halloysite modified by C18-triethoxysilane supported ruthenium catalyst with turnover frequency (TOF) of 4371 h-1. This catalytic system remained stable after ten cycles of benzene hydrogenation, providing 98 % conversion. The demonstrated synthetic strategy is promising for the design of industrial catalysts for the hydroprocessing water-containing organic feedstock and may be upscaled due to the abundant availability of halloysite clay nanotubes.



中文翻译:

纳米级反应器,基于疏水性管状铝硅酸盐并装饰有钌:高活性且稳定的芳烃加氢催化剂

工业加氢催化剂不仅必须具有选择性和活性,而且还必须能抵抗原料杂质(包括水)。我们报告了基于负载钌的疏水化硅铝酸盐纳米管制备催化核-壳纳米反应器的策略。用烷基三乙氧基硅烷对埃洛石进行改性可增强粘土纳米管的疏水性(水接触角高达122°),并使其选择性地负载4纳米钌粒子。这样的核-壳管状纳米反应器提供了保护活性位点免受混合水失活的作用,并防止了金属的浸出。生产的中尺度催化剂在80°C和3 MPa的氢气压力下,在有机介质和水性介质中的芳烃加氢中均具有活性。18-三乙氧基硅烷负载的钌催化剂,其周转频率(TOF)为4371 h -1。在十次苯加氢循环后,该催化体系保持稳定,提供98%的转化率。所证明的合成策略对于设计用于加氢处理含水有机原料的工业催化剂是有前途的,并且由于埃洛石粘土纳米管的丰富可用性而可以扩大规模。

更新日期:2020-10-13
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