四氯化碳液相催化加氢制氯仿多元金属催化剂的制备及其催化性能

doi:10.11944/j.issn.1000-0518.2017.02.160251

摘要/Abstract

摘要：

以贵金属M(=Pd,Pt)为主要活性成分,掺加过渡金属Fe和Ni作为助剂,采取浸渍和氢气还原法制备了椰壳活性炭(ACcs)负载的单元金属(M/ACcs)、二元金属(M-Ni/ACcs、M-Fe/ACcs)和三元金属(M-Ni-Fe/ACcs)系列催化剂;通过CCl₄液相催化加氢制氯仿反应考察了这些催化剂的催化活性和选择性。结果表明,Pd基催化剂的催化活性明显高于Pt基催化剂,但后者对氯仿的选择性优于前者;在前5 h加氢反应时段,两系列催化剂的活性顺序为:Pd-Ni-Fe/ACcs>Pd-Fe/ACcs>Pd/ACcs>Pd-Ni/ACcs和Pt/ACcs≈Pt-Fe/ACcs>Pt-Ni/ACcs>Pt-Ni-Fe/ACcs;总体上,引入Fe对于催化性能的改善效果要优于Ni,Ni的单独引入则会不同程度地降低催化活性。综合考量成本、活性和选择性等因素,优选Pd-Ni-Fe/ACcs作为催化剂,在393 K下反应5 h,可实现CCl₄ 97.6%的转化率以及接近100%氯仿的选择性。

关键词: 四氯化碳, 氯仿, 液相加氢, Pd/Pt催化剂, 催化性能, 转化率

Abstract:

By using Pd/Pt as main active ingredients and Fe/Ni as auxiliary, coconut shell activated carbon(ACcs) loaded mono metal(M/ACcs), binary metal(M-Ni/ACcs, M-Fe/ACcs) and ternary metal(M-Ni-Fe/ACcs) catalysts have been prepared via metal impregnation and H₂ reduction. The catalytic activity and selectivity of the catalysts for conversion of CCl₄ to CHCl₃ by liquid-phase hydrogenation was evaluated. Compared with Pt-based catalysts, the Pd-based counterparts have higher activity, but lower CHCl₃ selectivity. During initial reaction time of 5 h, the catalytic activity order follows:Pd-Ni-Fe/ACcs>Pd-Fe/ACcs>Pd/ACcs>Pd-Ni/ACcs and Pt/ACcs≈Pt-Fe/ACcs>Pt-Ni/ACcs>Pt-Ni-Fe/ACcs. Addition of Fe component improves the activity while single addition of Ni lowers the catalytic performance. The Pd-Ni-Fe/ACcs catalyst can realize more than 97% conversion of CCl₄ and nearly 100% selectivity for CHCl₃ at 393 K for 5 h.

Key words: tetrachloromethane, trichloromethane, liquid-phase hydrogenation, Pd/Pt catalysts, catalytic performance, conversion rate

朱一明, 张豪, 张军, 米刚, 宋帮才, 杜西刚. 四氯化碳液相催化加氢制氯仿多元金属催化剂的制备及其催化性能[J]. 应用化学, 2017, 34(2): 242-244.

ZHU Yiming, ZHANG Hao, ZHANG Jun, MI Gang, SONG Bangcai, DU Xigang. Preparation and Catalytic Performance Evaluation of Multi-metal Catalysts for Conversion of Tetrachloromethaneto Trichloromethane by Liquid Phase Hydrogenation[J]. Chinese Journal of Applied Chemistry, 2017, 34(2): 242-244.

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