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摘要以K2PdCl4、CoCl2•6H2O、NiCl2•6H2O等为原料，乙二醇为溶剂，采用NaBH4一步还原法制备纯Co、Pd（Co、Ni）-石墨烯、PdxCoy-石墨烯以及PdxNiy-石墨烯催化剂（x:y=3:1、1:1、1:3、1:6），采用水合肼还原法制备纯Ni催化剂，除Pd-石墨烯外其余催化剂均具有磁性。X射线粉末衍射结果表明纯Co及其石墨烯负载型催化剂为无定形结构、而Ni及其石墨烯负载型催化剂结晶性较好。研究了甲醇+水合肼、水+水合肼、甲醇+NaBH4、水+NaBH4体系中催化剂分别对2-NP、3-NP、4-NP的催化活性。结果表明：水合肼体系中含Co催化剂性能优于含Ni催化剂，PdCo3-石墨烯对2-NP显示出最佳的催化活性。NaBH4体系中含Ni催化剂性能优于含Co催化剂，其中PdNi3-石墨烯在甲醇+NaBH4体系中以及PdNi6-石墨烯在水+NaBH4体系中具有最佳的催化活性。PdCo3-石墨烯与PdNi3-石墨烯的X射线粉末衍射结果表明在石墨烯上确实负载有Pd-Co或Pd-Ni双金属。Raman表征结果证明了该结果的正确性。TEM结果表明纯Co、纯Ni粒径较大，而负载到石墨烯上，粒径将减小。与Pd形成双金属催化剂，金属粒子粒径进一步减小，在20 nm以内。最后催化剂循环性能测试结果显示，这两种催化剂循环性能较差。63939
毕业论文关键词：磁性；双金属催化剂；硝基苯酚；催化加氢
毕业设计说明书（论文）外文摘要
Title Catalytic Hydrogenation of Nitrophenol in the Presence of Pd-M(M=Co、Ni)-Graphene Catalysts
Abstract Pure Co、Pd（Co、Ni）-G、PdxCoy-G and PdxNiy-G Catalysts（x:y=3:1、1:1、1:3、1:6） have been synthesized successfully via a facile one-pot route by the use of NaBH4 as reducing agent, ethylene glycol as solvent and raw materials of K2PdCl4、CoCl2•6H2O and NiCl2•6H2O. Pure Ni has been synthesized by the use of hydrazine hydrate as reducing agent, and all of the catalysts have magnetism except Pd-G. The powder X-ray diffeaction (XRD) pattern shows that pure Co and Co-G catalysts are amorphous, but Ni and Ni-G catalysts are better crystallographic. Catalystic activity of all the catalysts were studied via catalytic hydrogenation of nitrophenol respectively in four different systems, such as methyalcohol+ hydrazine hydrate, water+ hydrazine hydrate, methy alcohol+NaBH4, water+ NaBH4. The results show that catalysts containing Co have better cataylstic activity for 2-NP in the system of hydrazine hydrate than that which contains Ni. And PdCo3-G has the best cataylstic activity. But in the system of NaBH4, catalysts containing Ni have better cataylstic activity for 3-NP than that which contains Co. PdNi3-G in the system of methy alcohol+NaBH4 and PdNi6-G in the system of water+NaBH4 show the best cataylstic activity. XRD pattern of PdCo3-G and PdNi3-G shows that Pd-Co or Pd-Ni bimetallic catalysts were really loaded on graphene. And Raman characterization results prove the conclusions above. Pure Co and Ni have the largest particle size, but it will be reduced when Co or Ni was loaded on graphene. What’s more, the particle size of the matel is further reduced to less than 20 nm by the formation of bimetallic catalysts with Pd. Finally, these two catalysts have poor cycling performance in the cycling tests.
Key words: Magnetism; Bimetallic catalyst; Nitrophenol; Catalytic hydrogenation
1 绪论 1
1.1 硝基苯酚催化加氢 1
1.1.1 硝基苯酚简介 1
1.1.2 硝基苯酚催化加氢及其应用 1
1.2 双（多）金属催化剂 2
1.3 石墨烯负载型双（多）金属催化剂 2
1.3.1 石墨烯简介 2
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