三嗪吡唑类配位超分子化合物的合成、 结构及光催化活性

doi:10.7503/cjcu20150099

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (8): 1478.doi: 10.7503/cjcu20150099

• 研究论文: 无机化学 • 上一篇下一篇

三嗪吡唑类配位超分子化合物的合成、结构及光催化活性

王志楠¹, 王继虓¹, 宋健¹, 高雪¹, 冯晓东¹, 孙立贤², 邢永恒¹()

1. 辽宁师范大学化学化工学院, 大连 116029
2. 桂林电子科技大学广西信息材料实验室, 桂林 541004

收稿日期:2015-01-27 出版日期:2015-08-10 发布日期:2015-07-17
作者简介:联系人简介: 邢永恒, 男, 博士, 教授, 主要从事生物无机化学和药物配位化学方面的研究. E-mail:xingyongheng2000@163.com
基金资助:
国家自然科学基金(批准号: 21371086)、辽宁省科学事业公益研究基金(批准号: 2014003019)和广西信息材料重点实验室开放基金(批准号: 1210908-06-K)资助

Syntheses, Structures and Photocatalytic Activities of Coordinated Supramolecular Complexes Containing Triazin-pyrazole Ligand^†

WANG Zhinan¹, WANG Jixiao¹, SONG Jian¹, GAO Xue¹, FENG Xiaodong¹, SUN Lixian², XING Yongheng^1,^*()

1. College of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, China
2. Guangxi Key Laboratory of Information Materials, Guilin University of Electronic Technology, Guilin 541004, China

Received:2015-01-27 Online:2015-08-10 Published:2015-07-17
Contact: XING Yongheng E-mail:xingyongheng2000@163.com
Supported by:
† Supported by the National Natural Science Foundation of China(No.21371086), the Commonweal Research Foundation of Liaoning Province, China(No.2014003019) and the Open Found of Guangxi Key Laboratory of Information Materials, China(No.1210908-06-K)

摘要/Abstract

摘要：

在水和乙醇的混合体系中合成了2个配位化合物[Co(Bpz*eaT)(H₂O)₃]·2H₂BTC·2H₂O(1)和[Cu(Bpz*eaT)(H₂O)₃]·2H₂BTC·CH₃CH₂OH·H₂O(2)[Bpz*eaT=2,4-二(3,5-二甲基吡唑)-6-二乙胺基-1,3,5-三嗪; H₃BTC=均苯三甲酸]. 通过元素分析、红外光谱、紫外光谱、热重分析、 X射线粉末衍射以及X射线单晶衍射方法对配合物进行了表征. 结构分析表明, 配合物1和2的中心金属均为六配位, 形成扭曲的八面体构型. 通过分子间氢键的作用, 配合物1和2分别被连接成三维和二维的超分子结构. 此外, 对2个配合物的光催化活性进行了研究.

关键词: 钴/铜配合物, 三嗪吡唑, 超分子, 晶体结构, 光催化活性

Abstract:

In the mixture of ethanol and water, two complexes [Co(Bpz*eaT)(H₂O)₃]·2H₂BTC·2H₂O(1) and [Cu(Bpz*eaT)(H₂O)₃]·2H₂BTC·CH₃CH₂OH·H₂O(2) were designed and synthesized via the reaction of metal salts and ligands H₃BTC(benzene-1,3,5-tricarboxylic acid) and Bpz*eaT[2,4-bis(3,5-dimethylpyrazol-1-yl)-6-diethylamino-1,3,5-triazine]. The complexes were characterized by elemental analysis, IR spectrometry, UV-Vis spectrometry, thermal gravimetric analysis, X-ray powder and X-ray single crystal diffraction analysis. Structural analysis reveals that both complexes 1 and 2 form distorted octahedral geometry, and complex 1 has a 3D network structure and complex 2 has a 2D layer structure via hydrogen bonding connection. Furthermore, the photocatalytic performances of complexes 1 and 2 were studied and the result revealed that the photocatalytic activity of complex 1 was better than that of complex 2.

Key words: Cobalt/Copper complex, Triazin-pyrazole Ligand, Supramolecule, Crystal structure, Photocatalytic activity

中图分类号:

O614

TrendMD:

王志楠, 王继虓, 宋健, 高雪, 冯晓东, 孙立贤, 邢永恒. 三嗪吡唑类配位超分子化合物的合成、结构及光催化活性. 高等学校化学学报, 2015, 36(8): 1478.

WANG Zhinan, WANG Jixiao, SONG Jian, GAO Xue, FENG Xiaodong, SUN Lixian, XING Yongheng. Syntheses, Structures and Photocatalytic Activities of Coordinated Supramolecular Complexes Containing Triazin-pyrazole Ligand^†. Chem. J. Chinese Universities, 2015, 36(8): 1478.

图/表 7

Table 1 Crystal data and structure refinements for complexes 1 and 2

Complex	1	2
Formula	C₃₅H₄₄N₈O₁₇Co	C₃₇H₄₈N₈O₁₇Cu
Molecular weight	907.71	940.37
Crystal system	Orthorhombic	Orthorhombic
Space group	P2₁2₁2₁	P2₁2₁2₁
a/nm	1.3575(1)	1.3549(8)
b/nm	1.7271(1)	1.7182(9)
c/nm	1.8297(1)	1.8201(10)
α/(°)	90	90
β/(°)	90	90
γ/(°)	90	90
V/nm³	4.2897(5)	4.237(4)
Z	4	4
D_calc/(g·cm^-3)	1.406	1.474
F(000)	1892	1964
μ(Mo Kα)/mm^-1	0.480	0.599
θ range/(°)	1.62—28.45	1.87—28.25
Reflections collected	36042	26235
Independent reflections[I>2σ(I)]	6578	7551
Parameters	560	573
Goodness of fit	1.015	1.028
R^a	0.0688(0.1207)^b	0.0674(0.0935)^b
w $R 2 a$	0.1849(0.2187)^b	0.1709(0.1895)^b

Table 1 Crystal data and structure refinements for complexes 1 and 2

Complex	1	2
Formula	C₃₅H₄₄N₈O₁₇Co	C₃₇H₄₈N₈O₁₇Cu
Molecular weight	907.71	940.37
Crystal system	Orthorhombic	Orthorhombic
Space group	P2₁2₁2₁	P2₁2₁2₁
a/nm	1.3575(1)	1.3549(8)
b/nm	1.7271(1)	1.7182(9)
c/nm	1.8297(1)	1.8201(10)
α/(°)	90	90
β/(°)	90	90
γ/(°)	90	90
V/nm³	4.2897(5)	4.237(4)
Z	4	4
D_calc/(g·cm^-3)	1.406	1.474
F(000)	1892	1964
μ(Mo Kα)/mm^-1	0.480	0.599
θ range/(°)	1.62—28.45	1.87—28.25
Reflections collected	36042	26235
Independent reflections[I>2σ(I)]	6578	7551
Parameters	560	573
Goodness of fit	1.015	1.028
R^a	0.0688(0.1207)^b	0.0674(0.0935)^b
w $R 2 a$	0.1849(0.2187)^b	0.1709(0.1895)^b

Fig.1 Molecular structure of complex 1(A) and views of two 1D chains(B), 2D sheet(C) and 3D network(D) in complex 1The atoms from Bpz*eaT except those coordinating with metal and the H atoms except those forming the hydrogen bonds are omitted for clarity.

Fig.2 Molecular structure of complex 2(A), view of connected method of two H2BTCs(B), 1D chain(C) and 2D sheet(D) of hydrogen bonding in complex 2 All atoms from Bpz*eaT except for coordinated with metal and all H atoms except for the hydrogen bonds are omitted for clarity.

Fig.3 (Ahν)2-hν plots of complexes 1 and 2

Fig.4 UV-Vis absorption spectra of RhB aqueous solutions using complex 1(A) and 2(B) as photocatalyst, respectively

Fig.5 Degradation curves of RhB using different photocatalystsa. Without photocatalyst; b. with complex 1; c. with complex 2.

Fig.6 Schematic illustration for the photocatalytic mechanism

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三嗪吡唑类配位超分子化合物的合成、结构及光催化活性

Syntheses, Structures and Photocatalytic Activities of Coordinated Supramolecular Complexes Containing Triazin-pyrazole Ligand^†

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三嗪吡唑类配位超分子化合物的合成、 结构及光催化活性

Syntheses, Structures and Photocatalytic Activities of Coordinated Supramolecular Complexes Containing Triazin-pyrazole Ligand†

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三嗪吡唑类配位超分子化合物的合成、结构及光催化活性

Syntheses, Structures and Photocatalytic Activities of Coordinated Supramolecular Complexes Containing Triazin-pyrazole Ligand^†