活性基团的空间分布对混合磷酸锆-钯催化剂羰化反应催化活性的影响

The effect of the distribution of the active groups in the surface and interlayer on the catalytic reactivity of the carbonylation with the zirconium Phosphate-Phosphonate-Pd Catalysts

用二苯基氯化膦对三乙烯四胺乙基膦酸 磷酸氢锆载体Zr(HPO4 ) 2 -2x[O3 PCH2 CH2 (NHCH2 CH2 ) 3 NH2 ]x·H2 O(简称ZP TETAEPA)表面进行二苯基膦化 ,制得了二苯基膦化的载体ZP TETAEPA DPP和相应的负载络合钯催化剂ZP TETAEPA DPP Pd ,用IR ,TG ,DTA及元素分析对它们进行了表征 ,着重研究了x值所反映的活性基团在载体表面的空间分布对ZP TETAEPA DPP Pd催化剂羰化反应催化活性的影响 ,并讨论了这种影响因素在其它混合磷酸锆类催化剂中存在的普遍性 .

It is reported in this paper the diphenylphosphinization of the groups of NH, NH2 on the surface of Zirconium ( tri\|ethylenetetraaminoethylphosphonate\|phosphate) supports Zr(HPO4)\-\{2- x \}[O3PCH 2CH 2 (NHCH 2CH 2) 3NH 2] x ·H2O(ZP\|TETAEPA)with chlorodiphenylphosphine as the phosphining agent, the diphenylphosphinized support ZP\|TETAEPA\|DPP and its corre\|sponding supported\|palladium catalysts ZP\|TETAEPA\|DPP\|Pd are prepared. and characterized by IR, TG , DTA and elementary analysis . In this paper, it is put stress on the investigation of the effect of the x value which is implicate the distribution of the active groups in the surface and interlayer on the catalytic reactivity of the carbonylation with the ZP\|TETAEPA\|DPP\|Pd catalysts. The generalization of this effect existing in other zirconium phosphate\|phosphonate catalysts was also discussed.