【摘要】 用氯化二苯基膦（Ｐｈ２ＰＣｌ）为膦化试剂， 首次对多乙烯多胺乙基膦酸－磷酸氢锆Ｚｒ（ＨＰＯ４）１．３５［Ｏ３ＰＣＨ２ＣＨ２（ＮＨＣＨ２ＣＨ２）ｍ ＮＨ２］０．６５·Ｈ２Ｏ （ＺＰ－ＰＥＰＡＥＰＡ， ｍ ＝ ０、１、２、３、４）载体表面进行二苯基膦化， 合成了一类含膦氮配体的新型混合膦酸锆载体及负载钯催化剂． 研究了有机膦酸侧链不同链长（ｍ ）和Ｐｈ２ＰＣｌ用量对配体载体制备的影响， 并用ＩＲ、ＴＧ、ＤＴＧ、ＤＴＡ 对这类载体及催化剂进行表征． 常压催化加氢实验表明， 这类催化剂对丙烯腈的加氢活性高于对硝基苯的加氢活性， 比较了膦化与未膦化的载体－钯催化剂的催化加氢活性， 并作了讨论． 催化羰化实验表明， 这类催化剂对羰化反应有较高的催化活性和选择性， 催化剂可以重复使用４～６ 次．更多还原

【Abstract】 The diphenylphosphinization of the groups NH,NH 2, P\|OH on the surface of zirconium(polyethylenepolyaminoethylphosphonate\|phosphate) supports \{Zr(HPO 4) 1.35 \|\}[O 3PCH 2CH 2(NHCH 2CH 2) m NH 2] 0.65 ·H 2O (ZP\|PEPAEPA, m=0, 1, 2, 3, 4) with chlorodiphenylphosphine as phosphining agent was reported. A new type of zirconium mixed phosphonate\|phosphate supports containing P, N ligands and their corresponding supported\|palladium catalysts are prepared for the first time. The influence of different length of the organic side chain with -CH 2CH 2(NHCH 2CH 2) m NH 2 groups and the amount of chlorodiphenylphosphine used in the preparation of ligand supports was discussed. These supports and palladium\|catalysts were characterized by IR, TG, DTG and DTA. Hydrogenation under atmospheric pressure catalyzed by these palladium\|catalysts was carried out, which shows that the initial hydrogenation rate of acrylonitrile is faster than that of nitrobenzene over these catalysts. The catalytic hydrogenation activity of the phosphining supports\|palladium catalysts and that of the unphosphinized catalysts were compared and discussed. The catalytic carbonylation of benzyl chloride using these catalysts are carried out and their catalytic activities were discussed also. The new type of supports\|palladium catalysts containing P, N ligands shows high activity and selectivity for the carbonylation of benzyl chloried and can be reused for 4 to 6 times.更多还原