6-苯基吡啶-2-羧酸- 4,4′-联吡啶配体新型Gd(III)配位聚合物的合成、结构表征及光催化CO2还原活性

Xi-Shi Tai, Yuan-Fang Wang, Li-Hua Wang, Xi-Hai Yan
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摘要

以6-苯基吡啶-2-羧酸、4,4 ' -联吡啶、NaOH和GdCl3∙6H2O为原料合成了新型Gd(III)配位聚合物{[Gd(L1)3(H2O)2]∙L2}n (1) (HL1 = 6-苯基吡啶-2-羧酸,L2 = 4,4 ' -联吡啶)。用红外光谱和x射线单晶衍射对Gd(III)配位聚合物的结构进行了表征。单晶分析结果表明,Gd(III)配位聚合物的基本单元包含1个Gd(III)离子、3个L1配体、2个配位水分子和1个不配位的4,4′-联吡啶。在1中,Gd(III)离子是8配位的,分别被来自3个L1配体的6个O原子和来自2个配位水分子的2个O原子包围。配合物1通过两个羧基氧原子的桥接相互作用和O−H∙∙N氢键相互作用呈现出1D链式结构。一维链通过叠加相互作用进一步连接,形成三维网络结构。研究了配合物1的光催化CO2还原活性。配合物1具有良好的CO2还原活性。随着时间的增加,CO的产率从第1 h的18.2 mmol/g提高到第3 h的60.3 mmol/g。CO选择性达到100%。版权所有©2023作者,BCREC集团出版。这是一篇基于CC BY-SA许可(https://creativecommons.org/licenses/by-sa/4.0)的开放获取文章。
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Synthesis, Structural Characterization and Photocatalytic CO2 Reduction Activity of a New Gd(III) Coordination Polymer with 6-Phenylpyridine-2-carboxylic acid and 4,4’-Bipyridine Ligands
A new Gd(III) coordination polymer, {[Gd(L1)3(H2O)2]∙L2}n (1) (HL1 = 6-phenylpyridine-2-carboxylic acid, L2 = 4,4’-bipyridine) was synthesized using 6-phenylpyridine-2-carboxylic acid, 4,4’-bipyridine, NaOH and GdCl3∙6H2O. The structure of Gd(III) coordination polymer has been characterized by IR and X-ray single crystal diffraction. The result of single crystal analysis indicates that fundamental unit of Gd(III) coordination polymer contains one Gd(III) ion, three L1 ligands, two coordinated water molecules and one uncoordinated 4,4’-bipyridine. In 1, the Gd(III) ion is eight-coordinated and surrounded by six O atoms from three L1 ligands and two O atoms from two coordinated water molecules, respectively. The complex 1 exhibits 1D chained structure by the bridging interactions of two carboxyl-oxygen atoms and O−H∙∙∙N hydrogen bonds interactions. The 1D chains are further connected by - stacking interactions to form 3D network architecture. The photocatalytic CO2 reduction activity of complex 1 has also been investigated. The complex 1 exhibits good CO2 reduction activity. With the increase of time, the yield of CO from 18.2 mmol/g in the first hour to 60.3 mmol/g in the third hour. And the CO selectivity has reached 100%. Copyright © 2023 by Authors, Published by BCREC Group. This is an open access article under the CC BY-SA License (https://creativecommons.org/licenses/by-sa/4.0).
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