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  

Preparation and Catalytic Performance Evaluation of Multi-metal Catalysts for Conversion of Tetrachloromethaneto Trichloromethane by Liquid Phase Hydrogenation

作　　者：朱一明[1] 张豪[1] 张军[1] 米刚[1] 宋帮才[1] 杜西刚[1] 

机构地区：[1]河南科技大学化工与制药学院,河南洛阳471203

出　　处：《应用化学》2017年第2期242-244,共3页Chinese Journal of Applied Chemistry

基　　金：国家自然科学基金资助项目(21576073;21076063)~~

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CC_l4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CC_l497.6%的转化率以及接近100%氯仿的选择性。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 CC14 to CHC13 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 CC14 and nearly 100% selectivity for CHCl3 at 393 K for 5 h.

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 

分 类 号：O643.3[理学—物理化学] TQ222.2[理学—化学]