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材料导报  2020, Vol. 34 Issue (12): 12163-12168    https://doi.org/10.11896/cldb.19030276
  高分子与聚合物基复合材料 |
双核钴化合物分子催化剂光催化分解水析氢性能及机理研究
郑会勤
河南财政金融学院化学与环境学院,郑州 450046
Photocatalytic Hydrogen Production Performance and Mechanism Exploration of a Binuclear Cobalt Catalyst
ZHENG Huiqin
Department of Chemistry and Environment, Henan Finance University, Zhengzhou 450046, China
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摘要 通过[Co(dmgH)(dmgH2)Cl2]与4,4′-联吡啶反应合成了一种新的非贵金属双核钴化合物分子催化剂[Co2(dmgH)4(μ-4,4′-bpy)Cl2](1),并通过IR、1H NMR、CV、荧光等表征了其结构和性能。以1为光催化剂,曙红Y(EY2-)为光敏剂,三乙醇胺(TEOA)为牺牲剂,在可见光(λ>420 nm)照射下,构建了一种有效的均相光催化体系。在目标催化剂1的浓度为3.7×10-4 mol·L-1,EY2-为4×10-4 mol·L-1,TEOA为20%(v/v),pH为10的最佳析氢条件下,光照2 h后,该体系的最大H2产量为(1 488.3±34.5) μmol((160.0±3.7) TON vs.1),析氢速率为(744.2±17.3) μmol·h-1。此外,本工作还简要地讨论了当前体系的光解水析氢机理,在所构建的析氢体系中,从激发态的1*EY2-到Co催化中心的电子转移也被证实是热力学可行的过程。
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郑会勤
关键词:  合成  双核钴  分子催化剂  光催化  析氢    
Abstract: Anew binuclear cobalt molecular catalyst, namely [Co2(dmgH)4(μ-4,4′-bpy)Cl2](1), had been synthesized by the reaction of [Co-(dmgH)(dmgH2)Cl2] with 4,4′-bipyridine(μ-4,4′-bpy). Its structure and properties were characterized by IR,1H NMR, CV, fluorescence, etc. An efficient homogeneous photocatalytic system was constructed by combination of noble-metal-free cobalt complex as catalyst, Eosin Y (EY2-) dye as photosensitizer and TEOA as sacrificial reagent under visible-light irradiation (λ>420 nm). The maximum H2 yield of (1 488.3±34.5 μmol) ((160.0±3.7) TON vs. 1) and H2 evolution rate of (744.2±17.3) μmol·h-1 were recorded under the optimal conditions with 1 of 3.7×10-4 mol·L-1, EY2- of 4×10-4 mol·L-1, TEOA of 20% (v/v) and pH of 10 in 2 h irradiation. Furthermore, the mechanism of H2 evolution in the homogeneous photolysis system was also briefly discussed. The electron transfer from the excited 1*EY2- to Co catalytic center of complex 1 in the designed system was also confirmed to be thermodynamic feasible.
Key words:  synthesis    binuclear cobalt    molecular catalyst    photocatalysis    H2 evolution
               出版日期:  2020-06-25      发布日期:  2020-05-29
ZTFLH:  O641.4  
基金资助: :国家自然科学基金(21171147);河南省科技计划项目(182102210279 );河南省教师教育课程改革研究重点研究项目(2018-JSJYZD-035)
通讯作者:  zhenghuiqin2000@163.com   
作者简介:  郑会勤,2015年毕业于郑州大学,获得理学博士学位,现为河南财政金融学院化学与环境学院副教授,主要从事光催化析氢的研究工作。
引用本文:    
郑会勤. 双核钴化合物分子催化剂光催化分解水析氢性能及机理研究[J]. 材料导报, 2020, 34(12): 12163-12168.
ZHENG Huiqin. Photocatalytic Hydrogen Production Performance and Mechanism Exploration of a Binuclear Cobalt Catalyst. Materials Reports, 2020, 34(12): 12163-12168.
链接本文:  
http://www.mater-rep.com/CN/10.11896/cldb.19030276  或          http://www.mater-rep.com/CN/Y2020/V34/I12/12163
1 Lian Zichao, Masanori Sakamoto, Junie J M, et al. Journal of the American Chemical Society,2019,141(6),2446.
2 Tanmay Banerjee S, Frederik Haase, Gökcen Savasci, et al. Journal of the American Chemical Society,2017,139(45),16228.
3 Dong J, Wang M, Zhang P, et al. Journal of Physical Chemistry C,2011,115,15089.
4 Zhang P, Jacques P A, Murielle C K, et al. Inorganic Chemistry,2012,512,115.
5 Lv Hongjin, Guo Weiwei, Wu Kaifeng, et al. Journal of the American Chemical Society,2014,136(40),14015.
6 Xu Yuxing, Ye Yun, Liu Taifeng, et al. Journal of the American Chemical Society,2016,138(34),10726.
7 Manuela A Gross, Anna Reynal, James R Durrant, et al. Journal of the American Chemical Society,2014,136(1),356.
8 Lazarides T, Mccormick T M, Du P, et al. Journal of the American Chemical Society,2009,131,9192.
9 Shimidzu T, et al. Journal of the American Chemical Society,1985,107,35.
10 Abe R, Hara K, Sayama K, et al. Journal of Photochemistry and Photo-biology A,2000,137,63.
11 Probst B, et al. Inorganic Chemistry,2009,48,1836.
12 DeLaive P J, et al. Journal of the American Chemical Society,1980,102,5627.
13 Fleming G R, et al. Journal of the American Chemical Society,1977,99,4306.
14 Cline E D, Adamson S E, Bernhard S. Inorganic Chemistry,2008,47,10378.
15 Krishnan C V, Sutin N. Journal of the American Chemical Society,1981,103,2141.
16 Xie J F, Li C, Zhou Q, et al. Inorganic Chemistry,2012,51,6376.
17 Vincze L, Sandor F, Pem J, et al. Photochemistry and Photobiology,1999,120,11.
18 Cuilford J, et al. Journal of Physical Chemistry,1994,98,6906.
19 Rehm D, Weller A. Israel Journal of Chemistry,1970,8,259.
20 Sukanta M, Shinya S, Yusuke Y, et al. Journal of the American Chemical Society,2013,135,15294
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