La3+取代的纳米尺寸砷钨氧簇的合成、晶体结构及光催化性质研究

摘要/Abstract

摘要： 本文基于自组装原理,以Na₂WO₄·2H₂O、亚砷酸钠和LaCl₃·6H₂O为主要原料,采用一锅法将稀土金属La^Ⅲ与缺位结构的多钨氧簇构筑单元结合得到了一例新型稀土基砷钨氧簇合物,并借助单晶X射线衍射、X射线粉末衍射(PXRD)、傅里叶红外光谱(IR)等手段确认了其结构和组成。单晶X射线衍射结果表明:该配合物属于单斜晶系,C2/c空间群,晶胞参数为a=3.595 56(14) nm,b=1.222 48(4) nm,c=2.247 34(9) nm,β=117.117 0(10)°,V=8.792 3(6) nm³,Z=4,其分子式为[(CH₃)₂NH₂]₈H_3.56[{LaO(H₂O)₂}{WO(H₂O)}{W_0.24(H₂O)₂}{AsW₉O₃₃}₂]。在该化合物中,聚阴离子簇[{LaO(H₂O)₂}{WO(H₂O)}{W_0.24(H₂O)₂}{AsW₉O₃₃}₂]^11.56-具有三明治结构,可以看作是由两个{AsW₉O₃₃}单元夹心1个{LaO(H₂O)₂}片段、1个{WO(H₂O)}组分和1个{W_0.24(H₂O)₂}片段组成。本文进一步探究了该化合物对于罗丹明-B的催化降解性质,结果表明,在300 W的汞灯照射条件下,该化合物表现出了良好的光催化活性,降解效率为74%。

关键词: 多金属氧酸盐, 砷钨氧酸盐, 一锅法, 镧配合物, 晶体结构, 有机染料, 光催化降解

Abstract: Based on the principle of molecular design and self-assembly, a novel rare earth based arsenotungstate was obtained by introducing rare earth La^Ⅲ ions into the lacunary polyoxotungstates clusters with vacancy structure by one-pot method with Na₂WO₄·2H₂O, NaAsO₂ and LaCl₃·6H₂O as the main materials. The structure and composition of this complex was confirmed by single-crystal X-ray diffraction, X-ray powder diffraction (PXRD), infrared spectroscopy (IR) and so on. The single crystal X-ray diffraction results show that the complex is in the monoclinic system, C2/c space group, and with the cell parameters of a=3.595 56(14) nm, b=1.222 48(4) nm, c=2.247 34(9) nm, β = 117.117 0(10)°, V=8.792 3(6) nm³, Z=4. The molecular formula of this compound is [(CH₃)₂NH₂]₈H_3.56[{LaO(H₂O)₂}{WO(H₂O)}{W_0.24(H₂O)₂}{AsW₉O₃₃}₂]. And the polyoxoanion [{LaO(H₂O)₂}{WO(H₂O)}{W_0.24(H₂O)₂}{AsW₉O₃₃}₂]^11.56- shows a novel sandwich type structure, which can be simply described as two trilacunary Keggin type{AsW₉O₃₃} units are linked by a {LaO(H₂O)₂} segment, a {WO(H₂O)} segment and a {W_0.24(H₂O)₂} segment. Catalytic degradation property of this compound for Rhodamine-B was further inverstigated. The results demonstrate that the compound shows good photocatalytic activity under the condition of 300 W Hg lamp irradiation, and the degradation efficiency reaches to 74%.

Key words: polyoxometalate, arsenotungstate, one-pot method, lanthanum complex, crystal structure, organic dye, photocatalytic degradation

中图分类号:

杨玲, 苏斌斌, 王宏胜, 李金钊, 李叶盛, 陈睿. La³⁺取代的纳米尺寸砷钨氧簇的合成、晶体结构及光催化性质研究[J]. 人工晶体学报, 2024, 53(9): 1591-1598.

YANG Ling, SU Binbin, WANG Hongsheng, LI Jinzhao, LI Yesheng, CHEN Rui. Synthesis, Crystal Structure and Photocatalytic Properties of Nanosized La³⁺-Substituted Arsenotungstate Cluster[J]. JOURNAL OF SYNTHETIC CRYSTALS, 2024, 53(9): 1591-1598.

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La³⁺取代的纳米尺寸砷钨氧簇的合成、晶体结构及光催化性质研究

Synthesis, Crystal Structure and Photocatalytic Properties of Nanosized La³⁺-Substituted Arsenotungstate Cluster

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