摘要
苯基膦酸(C6H5PO3H2)作为磷源,在温和条件下与Na2MoO4·2H2O、2,2′-联咪唑(H2biim)反应,并借助H2biim质子化后形成的有机阳离子[H3biim]^+和杂多阴离子[(PhP)2Mo5O15]^4-(PhP=C6H5PO3)之间的电中和作用,在弱酸性水溶液中缓慢晶化,形成了1例以PhP为中心的Strandberg型苯基膦钼酸-联咪唑荷移盐(H3biim)4[(PhP)2Mo5O15]·H2O(1).利用单晶和粉末X射线衍射(SCXRD和PXRD)分析、元素分析、红外(IR)光谱等手段对化合物1进行了表征,并通过热重-差热分析(TG-DTA)考察了其热稳定性.以酸催化合成环己酮乙二醇缩酮为反应模型,探讨了化合物1的酸催化性能,同时考察了反应时间、反应物料比和催化剂用量对反应的影响.结果表明:化合物1作为固体多金属氧酸盐(POM)型催化剂,其催化活性高,结构稳定,可循环使用.
Phenylphosphonic acid(C6H5PO3H2)was used as the P source to react with Na2MoO4·2H2O,2,2′-diimidazole(H2biim)under mild conditions,and by the aid of charge neutralization between organic cation[H3biim]^+ formed by protonation of H2 biim and heteropolyoxoanion [(PhP)2Mo5O15]^4-(PhP = C6H5PO3),a Strandberg-type phenylphosphomolybdate-H2biim charge-transfer salt,(H)3biim)4[(PhP)2 Mo5 O15]·H2 O(1)with a PhP center,was obtained through slow crystallization in weak acidic aqueous solution.Compound 1 was characterized by single-crystal and powder Xray diffraction(SCXRD and PXRD)analysis,elemental analysis,IR spectroscopy.The thermal stability of compound 1 was also investigated by thermogravimetry and differential thermal analysis(TGDTA).The acid-catalytic synthesis of cyclohexanone ethylene ketal was selected as a model reaction,and the acid catalytic performance of compound 1 was evaluated,together with the effects of reaction time,material ratio and catalyst dosage on the reaction also were studied.The results show that compound 1 as a solid polyoxometalatc(POM)catalyst,has high catalytic activity,stable structure,and the catalyst can be recycled.
作者
张澜萃
李孟璇
王建平
陆影
ZHANG Lancui;LI Mengxuan;WANG Jianping;LU Ying(School of Chemistry and Chemical Engineering,Liaoning Normal University,Dalian 116029,China)
出处
《辽宁师范大学学报（自然科学版）》
CAS
2019年第2期197-203,共7页
Journal of Liaoning Normal University:Natural Science Edition
基金
国家自然科学基金资助项目(21671091)
