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

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.