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Pt Catalyst Supported on Multi-Walled Carbon Nanotubes for Hydrogenation-Dearomatization of Toluene and Tetralin

机译:多孔碳纳米管上负载的Pt催化剂用于甲苯和Tetralin的加氢-脱芳烃

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摘要

A type of MWCNT-supported Pt catalysts for the hydrogenation-dearomatization (HDA) of aromatics was developed, which displays excellent performance for HDA of two model compounds, toluene and tetralin. Over the 1% Pt/CNTs catalyst, near 100% conversion of toluene or tetralin was observed under the reaction temperature of 373 K. The specific reaction rate of HDA of toluene and tetralin reached 0.0524 and 0.0174 mmol s(-1) (m(-surf.)(2) (Pt))(-1), respectively. Both of the values were 1.18 times those (0.0444 and 0.0148 mmol s(-1) (m(-surf. Pt)(2))(-1), respectively) of the 2.4% Pt/AC catalyst with the optimal Pt loading under the same reaction conditions. It was experimentally found that using the CNTs in place of AC as the support of the catalyst did not cause a significant change in the apparent activation energy for the HDA reaction of toluene or tetralin, but led to a certain increase in the molar percentage of catalytically active Pt-species (Pt-0) in the total Pt-amount at the surface of the functioning catalyst. In addition, the Pt/CNTs catalyst could reversibly adsorb a greater amount of hydrogen under atmospheric pressure and temperatures ranging from room temperature to 773 K. This unique feature would help to generate a microenvironment with higher stationary state concentration of active hydrogen-adspecies at the surface of the functioning catalyst. These effects favored increasing the rate of the HDA reaction of toluene or tetralin.
机译:开发了一种用于芳香族化合物加氢脱芳香化(HDA)的MWCNT负载的Pt催化剂,该催化剂对两种模型化合物甲苯和四氢萘的HDA表现出优异的性能。在1%Pt / CNTs催化剂上,在373 K的反应温度下,观察到甲苯或四氢萘的转化率接近100%。甲苯和四氢萘的HDA比反应速率分别为0.0524和0.0174 mmol s(-1)(m( -surf。)(2)(Pt))(-1)。这两个值都是具有最佳Pt载量的2.4%Pt / AC催化剂(分别为0.0444和0.0148 mmol s(-1)(分别为m(-surt.Pt)(2))(-1)的1.18倍在相同的反应条件下实验发现,使用碳纳米管代替交流电作为催化剂的载体,不会导致甲苯或四氢萘的HDA反应的表观活化能发生显着变化,但会导致催化反应的摩尔百分率有所增加。活性催化剂表面总Pt量中的活性Pt种类(Pt-0)。此外,Pt / CNTs催化剂可在大气压和室温至773 K的温度下可逆地吸附更多的氢气。这一独特功能将有助于在高温下生成具有较高静态氢浓度的微环境。功能催化剂的表面。这些作用有利于提高甲苯或四氢萘的HDA反应速率。

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