在線閱讀 --自然科學版 2021年3期《Keggin型磷鉬酸鹽超分子配合物的合成及光催化還原Cr(Ⅵ)的應用》
Keggin型磷鉬酸鹽超分子配合物的合成及光催化還原Cr(Ⅵ)的應用--[在線閱讀]
畢昊學, 李穩, 張雅琪, 馬媛媛, 韓占剛
河北師范大學 化學與材料科學學院, 河北省功能有機分子重點實驗室, 國家實驗化學教育示范中心, 河北 石家莊 050024
起止頁碼: 283--289頁
DOI: 10.13763/j.cnki.jhebnu.nse.202103009
摘要
通過水熱法合成了一例Keggin型磷鉬酸鹽超分子配合物,化學式為(H2bpe)(Hbpe){PMo12O40}·6H2O(1)(bpe=反式-1,2-雙(4-吡啶基)-乙烯).通過使用單晶X射線衍射、紅外光譜、X射線粉末衍射、熱重、循環伏安、固體可見漫反射光譜等測試手段對其結構、氧化還原性能以及光學活性進行了表征,并將其用于光催化還原Cr(Ⅵ)反應體系中.結構分析表明,化合物1中的無機部分由離散的[PMo12O40]3-陰離子簇組成,該陰離子簇通過與有機抗衡陽離子之間的氫鍵作用連接形成三維超分子結構.化合物1具有寬的可見光吸收和合適的能帶結構,在光催化還原Cr(Ⅵ)反應中展現出良好的光催化活性.在80min內,Cr(Ⅵ)還原轉化率可達到72%.經過4次循環后,結構依然保持良好.該工作為設計和制備高效的多酸基Cr(Ⅵ)光催化劑提供了新的方法.

Synthesis of Keggin Type Molybdophosphate Supramolecular Complex and Its Application in Photocatalytic Reduction of Cr(Ⅵ)
BI Haoxue, LI Wen, ZHANG Yaqi, MA Yuanyuan, HAN Zhangang
Hebei Key Laboratory of Organic Functional Molecules, National Demonstration Center for Experimental Chemistry Education, College of Chemistry and Materials Science, Hebei Normal University, Hebei Shijiazhuang 050024, China
Abstract:
In this work,a Keggin-type supramolecular complex with formula of (H2bpe)(Hbpe)[PMo12O40]·6H2O (1) (bpe=trans-1,2-bi(4-pyridyl)-ethylene) was hydrothermally synthesized and characterized by single crystal X-ray diffraction,infrared spectrum,powder X-ray diffraction,thermogravimetry TG,cyclic voltammetry,UV-vis diffuse-reflectance spectroscopy.Compound 1 was constructed by[PMo12O40]3- polyoxoanions and protonated bpe cations,and the hydrogen bonding interactions between them extended the whole structure into three-dimensional supramolecular structure.The UV-vis DRS spectrum demonstrated that compound 1 has wide absorption range towards visible-light and suitable energy band structure.When using as photocatalyst,compound 1 showed excellent photocatalytic performance towards the reduction of Cr(Ⅵ).The reduction rate of Cr (Ⅵ) can reach to 72% within 80min.After 4 cycles,the structure is still ingood condition.This work provides a newguidance for the design and preparation of highly efficient Cr(Ⅵ) photocatalysts based on polyoxometalates.

收稿日期: 2020-11-08
基金項目: 國家自然科學基金(21871076,21901060);大學生課外學術科技創新基金(AE2020102203215)

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