Catalytic Materials

Study on synthesis,structure and catalytic iodide oxidation of (C5H7N2O24(SiMo12O40

  • Xiao Feng ,
  • Jun Guo ,
  • Dan Zhang
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  • 1. School of Chemistry and Materials Science,Guizhou Normal University,Guiyang 550001,China
    2. State Key Laboratory and Postdoctoral Workstation for Efficient Utilization of Medium and Low Grade Phosphate Rock and Its Associated Resources,Wengfu(Group) Co.,LTD

Received date: 2020-11-05

  Online published: 2021-09-08

Abstract

A novel organic-inorganic hybrid polyoxometalate(C5H7N2O24(SiMo12O40)(short for SiMo-12) was synthesized by the conventional aqueous solution method.The compounds were characterized by infrared spectroscopy(IR),thermogravimetric analysis(TG),single crystal and powder X-ray diffraction(XRD) and elemental analysis.With hydrogen peroxide as oxidant,SiMo-12 was used to catalyze the oxidation of iodine ions.The effect of catalyst dosage,oxidant dosage,pH,temperature and other factors on the reaction rate were investigated.The results showed that the compound belonged to the triclinic crystal system,P-1 spatial group,cell parameters a=1.097 58(4) nm、b=1.144 88(4) nm、c=1.252 66(4) nm、α=64.665(1)°、β=64.804(1)°、γ=83.441(1)°、V=1.282 89(8) nm3Z=1、R=0.034 0、wR2=0.079 9.The structure of the compounds was composed of four 1-imidazoleacetic acid and a classical Keggin[SiMo12O40]4- unit and the organic ligands and the polyoxo-metalate anion formed a one-dimensional chain along x axis through electrostatic interaction,proton transfer and hydrogen bonding.These chains were parallel to each other,forming a two-dimensional layers parallel to the xy plane,which were connected by hydrogen bonds to obtain a three-dimensional network structure.The catalyst exhibited excellent catalytic activity in the oxidation of iodide ion,and the reaction rate reached 2.641 6×10-5 mol/(L·s) at the condition of c(SiMo-12)=2.0×10-4 mol/L、c(H2O2)= 2.0×10-3 mol/L、pH=1.4、T=50 ℃,which was 1 565 times higher than that without catalyst.

Cite this article

Xiao Feng , Jun Guo , Dan Zhang . Study on synthesis,structure and catalytic iodide oxidation of (C5H7N2O24(SiMo12O40)[J]. Inorganic Chemicals Industry, 2021 , 53(9) : 109 -113 . DOI: 10.19964/j.issn.1006-4990.2020-0554

References

[1] 王恩波, 陈维林. 多酸化学[M].朱清时. 北京: 科学出版社, 2013.
[2] 陈发旺, 胡长文. 多金属氧簇催化研究进展[J]. 化学进展, 2011, 23(1):19-41.
[3] Yamase T. Photo- and electrochromism of polyoxometalates and related materials[J]. Chemical Reviews, 1998, 98(11):307-326.
[4] Wang S S, Yang G Y. Recent advances in polyoxometalate-catalyzed reactions[J]. Chemical Reviews, 2015, 115(11):4893-4962.
[5] Rhule J T, Hill C L, Judd D A, et al. Polyoxometalates in medicine[J]. Chemical Reviews, 1998, 98(11):327-358.
[6] Grinenval E, Basset J M, Lefebvre F. A novel approach to prepare well-defined silica-supported polyoxometalate species by reaction with a chlorinated support[J]. Journal of Inorganic Chemistry, 2013.Doi: 10.1155/2013/902192.
[7] Li H, Gong P, Jiang J, et al. Organic-inorganic hybrids assembled from plenary Keggin-type germanotungstate units and 3d-4f hetero-metal clusters[J]. Dalton Transactions, 2019, 48(11):3730-3742.
[8] 周欣, 叶晶, 王志花, 等. 两个基于多金属氧簇和咪唑类化合物的有机-无机杂化物的合成及性质[J]. 无机化学学报, 2019, 35(1):43-49.
[9] Li N, Mu B, Cao X, et al. The structures and properties of the new two-dimensional inorganic-organic hybrid materials based on the molybdate chains[J]. Journal of Solid State Chemistry, 2014, 127(1):180-186.
[10] Taleghani S, Mirzaei M, Eshtiagh-Hosseini H, et al. Tuning the topology of hybrid inorganic-organic materials based on the study of flexible ligands and negative charge of polyoxometalates:A crystal engineering perspective[J]. Coordination Chemistry Reviews, 2016, 309:84-106.
[11] 林宏艳, 曾凌, 王青林, 等. 一种双吡啶双酰胺配体修饰的Keggin型硅钼酸盐基配合物的合成、结构与催化性能[J]. 应用化学, 2016, 33(1):76-83.
[12] 史振雨, 冯小利, 郑玉国, 等. 2,6-二甲基-3,5-二(吡唑-3-基)吡啶构筑的新型八钼酸盐的合成及其电化学性质[J]. 合成化学, 2020, 28(1):30-35.
[13] Du X D, Li C H, Zhang Y, et al. Coordination polymers based on the octamolybdate and flexible bis(triazole) ligands with different spacer lengths[J]. Crystengcomm, 2011, 13(7):2350-2357.
[14] 郭军, 蔡丽丽, 解田, 等. 非均相多钼氧簇/硅藻土催化氧化碘离子研究[J]. 功能材料, 2019, 50(9):120-128.
[15] 宋锡高. 中国碘素产业发展现状[J]. 无机盐工业, 2014, 46(3):9-12.
[16] 周维珍, 郭军, 李文飞, 等. 膨润土负载磷钼酸催化碘离子氧化反应的研究[J]. 无机盐工业, 2017, 49(10):62-66.
[17] Gong Y, Hu C, Li H, et al. Synjournal,crystal structure and calcination of three novel complexes based on 2-aminopyridine and polyoxometalates[J]. Journal of Molecular Structure, 2006, 784(1/2/3):228-238.
[18] Cao Y, Lv J, Yu K, et al. Synjournal and photo-/electro-catalytic properties of Keggin polyoxometalate inorganic-organic hybrid layers based on d10 metal and rigid benzo-diazole/-triazole ligands[J]. New Journal of Chemistry, 2017, 41(21):12459-12469.
[19] 王晓波. 新型多金属氧酸盐催化剂的设计合成及催化过氧化氢氧化淀粉性能的研究[D]. 长春:东北师范大学, 2017.
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