碳化钼负载Ru基催化剂的5-硝基苯并噻唑加氢性能研究OA北大核心
Study on performances of molybdenum carbide supported Ru-based catalysts for 5-nitrobenzothiazole hydrogenation
使用负载型金属催化剂催化含硫底物加氢时,由于硫在金属表面的强吸附可导致催化剂活性变差甚至完全失活.采用过体积浸渍法制备了不同晶相碳化钼负载Ru基催化剂(Ru/α-MoC和Ru/β-Mo2C),并用于催化5-硝基苯并噻唑(5-NBT)加氢.利用SEM、XRD、HR-TEM和XPS等对催化剂进行了表征.结果表明,α-MoC上负载的Ru为原子级分散,而β-Mo2C上负载的Ru以纳米颗粒形式分散.在80 ℃、2.0 MPa H2、3 mL乙醇、10 mg底物和10 mg催化剂的条件下,当5-NBT转化率低于 30%时,Ru/α-MoC的5-NBT加氢反应速率为9113 μmol/(g·h);反应40 min时,Ru/α-MoC的5-NBT转化率为100%.氢-氘交换实验结果证实α-MoC对5-NBT硝基的活化(吸附活化)有重要作用,而Ru对H2解离有促进作用,这两方面作用的协同效应使Ru/α-MoC在5-NBT加氢中表现出相对更高的催化性能.
When the supported metal catalyst is used to catalyze the hydrogenation of sulfur-containing substrates,the activity of the catalyst can be deteriorated or even completely deactivated due to the strong adsorption of sulfur on the metal surface.Ru-based catalysts(Ru/α-MoC and Ru/β-Mo2C)supported by molybdenum carbide with different crystalline phases were prepared by over volume impregnation method and used to catalyze 5-nitrobenzothiazole(5-NBT)hydrogenation.The catalysts were characterized by SEM,XRD,HR-TEM and XPS,etc.The results show that the Ru loaded on α-MoC is atomically dispersed,while the Ru loaded on β-Mo2C is dispersed in the form of nanoparticles.Under the conditions of 80 ℃,2.0 MPa H2,3 mL ethanol,10 mg substrate and 10 mg catalyst,the 5-NBT hydrogenation rate of Ru/α-MoC is 9113 μmol/(g·h)when the 5-NBT conversion rate is lower than 30%.After reaction for 40 min,the 5-NBT conversion rate of Ru/α-MoC is 100%.The result of hydrogen-deium exchange experiment confirms that α-MoC plays an important role in the activation(adsorption activation)of 5-NBT nitro group,while Ru promotes H2 dissociation.The synergistic effect of these two effects makes Ru/α-MoC show relatively higher catalytic performance in 5-NBT hydrogenation.
黄佳怡;任小敏;马军;储伟;刘岳峰
四川大学 化学工程学院,四川成都 610065||中国科学院 大连化学物理研究所,辽宁 大连 116023中国科学院 大连化学物理研究所,辽宁 大连 116023||大连交通大学环境与化学工程学院,辽宁大连 116028四川大学 化学工程学院,四川成都 610065||中国科学院 大连化学物理研究所,辽宁 大连 116023四川大学 化学工程学院,四川成都 610065中国科学院 大连化学物理研究所,辽宁 大连 116023
化学工程
催化加氢Ru基催化剂碳化钼5-硝基苯并噻唑加氢
catalytic hydrogenationRu-based catalystsmolybdenum carbide5-nitrobenzothiazole hydrogenation
《低碳化学与化工》 2025 (1)
87-94,8
国家自然科学基金(22172161,22302027)大连市青年科技之星项目(2022RQ030).
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