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人工晶体学报 ›› 2021, Vol. 50 ›› Issue (11): 2123-2128.

• 研究论文 • 上一篇    下一篇

Keggin型多酸基超分子化合物H3[{H(4-AP)}6(PMo6Mo6O40)]的结构和电催化性能

徐娜, 王金玲, 张众, 李晓慧, 常之晗   

  1. 渤海大学化学与材料工程学院,辽宁省全谱太阳能电池转光材料专业技术创新中心,锦州 121013
  • 出版日期:2021-11-15 发布日期:2021-12-13
  • 作者简介:徐 娜(1990—),辽宁省人,博士,讲师。E-mail:xun872@bhu.edu.cn
  • 基金资助:
    国家自然科学基金青年科学基金(21901018);渤海大学博士启动基金(0520bs022)

Structure and Electrocatalytic Performance of a Keggin-Type Polyoxometalate-Based Supramolecular Complex H3[{H(4-AP)}6(PMoV6MoVI6O40)]

XU Na, WANG Jinling, ZHANG Zhong, LI Xiaohui, CHANG Zhihan   

  1. Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell, College of Chemistry and Materials Engineering, Bohai University, Jinzhou 121013, China
  • Online:2021-11-15 Published:2021-12-13

摘要: 通过水热合成方法,以钼酸铵、氯化镍和4-氨基吡啶为原料成功合成了一个Keggin型多酸基超分子化合物H3[{H(4-AP)}6(PMoV6MoVI6O40)] (4-AP=4-氨基吡啶)。该化合物的结构单元包含一个[PMoV6MoVI6O40]9-阴离子和6个质子化的配体。而[PMoV6MoVI6O40]9-阴离子与配体之间通过N(1)—H(1)…O(3)、N(2)—H(2A)…O(5)和N(2)—H(2B)…O(1)三种氢键相互作用,进而形成二维超分子层。通过X射线单晶衍射、IR和粉末X射线衍射对其进行表征。晶体结构分析表明:该标题化合物属于三方晶系,R-3空间群,a=2.191 2 (10) nm, b=2.191 2 (10) nm, c=1.042 3(5) nm, α=β=90°, γ=120°, V=4.333 8(4) nm3, Z=3, R1=0.036 2, wR2=0.095 6, 电催化性质研究表明该标题化合物对H2O2和K2Cr2O7具有良好的电催化还原效果,以及对抗坏血酸具有良好的电催化氧化效果。

关键词: Keggin型多酸, 超分子化合物, 电催化性能, 水热法, 晶体结构

Abstract: A Keggin-type polyoxometalate-based supramolecular complex H3[{H(4-AP)}6(PMoV6MoVI6O40)] (4-AP=4-aminopyridine) was successfully synthesized from ammonium molybdate, nickel chloride, and 4-aminopyridine by hydrothermal method. The structural unit of the complex contains a [PMoV6MoVI6O40]9- anion and six protonated ligands. [PMoV6MoVI6O40]9- anion and ligands are connected to each other by N(1)—H(1)…O(3), N(2)—H(2A)…O(5), and N(2)—H(2B)…O(1) hydrogen bonds, which further form a two-dimensional supramolecular layer. It was characterized by X-ray single crystal diffraction, IR spectra, and powder X-ray diffraction. The crystal structure analysis shows that the complex belongs to the trigonal crystal system, R-3 space group, a=2.191 2 (10) nm, b=2.191 2 (10) nm, c=1.042 3 (5) nm, α=β=90°, γ=120°, V=4.333 8 (4) nm3, Z=3, R1=0.036 2, wR2=0.095 6. The electrocatalytic performance shows that the complex has a good electrocatalytic reduction effect on H2O2 and K2Cr2O7. It also has a good effect of electrocatalytic oxidation on ascorbic acid.

Key words: Keggin-type polyoxometalate, supramolecular complex, electrocatalytic performance, hydrothermal method, crystal structure

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