2-氨基-6-甲基吡啶/Keggin型多酸超分子化合物的合成、结构及催化氧化碘离子研究  

Synthesis,structure and catalytic Iodide oxidation of 2-amino-6-methylpyridine/Keggin-typepolyacid supramolecular compounds

作　　者：郭军[1,2] 冯潇 张丹 袁常梅 GUO Jun;FENG Xiao;ZHANG Dan;YUAN Chang-mei(School of Chemistry and Materials Science,Guizhou Normal University,Guiyang 550001,China;State Key Laboratory and Postdoctoral Workstation for Efficient Utilization of Medium and Low Grade Phosphate Rock and Its Associated Resources,Wengfu(Group)Co.,LTD,Guiyang 550014,China)

机构地区：[1]贵州师范大学化学与材料科学学院,贵州贵阳550001 [2]瓮福(集团)有限责任公司中低品位磷矿及其共伴生资源高效利用国家重点实验室·博士后工作站,贵州贵阳550014

出　　处：《化学研究与应用》2021年第9期1706-1711,共6页Chemical Research and Application

基　　金：国家自然科学基金项目(21862005)资助;贵州省科技厅计划项目(黔科合LH字、黔合基础、黔科合支撑、黔科合平台人才)([2017]7336、[2019]1457、[2019]2835、[2018]5769)资助;贵州省教育厅青年科技人才成长项目(黔教合KY字[2018]126)资助;中低品位磷矿及其共伴生资源高效利用国家重点实验室开放课题(WFKF2017-03)资助。

摘　　要：本论文采用水热法合成了一种新型多酸基超分子化合物,通过元素分析、X-射线单晶衍射IR、XRD、TG对化合物进行了表征,结果表明:化合物的结构式为(C6H9N2)3[PMo12O40]·2H2O(PMo-12),属正交晶系,Pnma空间群,晶胞参数a=14.5600(2),b=19.4862(3),c=17.7475,α=β=γ=90°,V=5035.30(12)3,Z=4,R1=0.0387,wR2=0.0997。以过氧化氢为氧化剂,用PMo-12催化碘离子氧化,结果表明:该催化剂在催化过氧化氢氧化碘离子中表现出较为优异的催化活性且具有稳定的可重复性,25℃条件下,当m(PMo-12)=0.01g,c(I^(-))=2.5×10^(-3) mol·L^(-1),c(H_(2)O_(2))=1.25×10^(-3) mol·L^(-1),c(H^(+))=2.5×10^(-3) mol·L^(-1)时其反应速率达到1.8043×10^(-6)mol·L^(-1)·S^(-1),比未加催化剂的反应速率提高了106倍。In this paper,a new supramolecular polyacid compound was synthesized by hydrothermal method,and characterized by elemental analysis,X-ray single crystal diffraction,IR,XRD and TG.The results showed thatthe structural formula of the compound is(C6H9N2)3[PMo12O40]2H2O,which belongs to orthorhombic crystal system and Pnma space group.The cell parameters are a=14.5600(2),b=19.4862(3),c=17.7475,α=β=γ=90°,V=5035.30(12)3,Z=4,R1=0.0387,wR2=0.0997.With hydrogen peroxide as the oxidant,PMo-12 was used to catalyze the oxidation of iodine ion by hydrogen peroxide.The results showed that the catalyst showed goodcatalytic activity and stable repeatability in the process of iodine ion oxidation by hydrogen peroxide.When m(PMo-12)=0.01g,c(I^(-))=2.5×10^(-3) mol·L^(-1),c(H_(2)O_(2))=1.25×10^(-3) mol·L^(-1),c(H^(+))=2.5×10^(-3) mol·L^(-1),the reaction rate reached 1.8043×10^(-6)mol·L^(-1)·S^(-1),106 times higher than the reaction rate without catalyst.

关 键 词：多金属氧酸盐 晶体结构 催化氧化 

分 类 号：O611.2[理学—无机化学] O611.3[理学—化学]