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题名: Identification of homogeneous [Co4(H2O)4(HPMIDA)2(PMIDA)2]6−as an effective molecular-light-driven water oxidation catalyst
作者: Xu, Qian; Li, Hui; Chi, Le; Zhang, Liugen; Wan, Zheng; Ding, Y(丁勇); Wang, Jide
收录类别: SCIE ; EI
出版日期: 2017-03-01
刊名: APPLIED CATALYSIS B-ENVIRONMENTAL
卷号: 202, 页码:397-403
出版者: ELSEVIER
出版地: AMSTERDAM
英文摘要: Transition-metal complexes, especially cobalt complexes, are used as precatalysts in homogeneous water oxidation catalysis. However, a practical method of identifying the effective active species in cobalt complex homogeneous catalysts under highly oxidizing conditions have not yet been established. In this work, (H3O)(6).[Co-4(H2O)(4)(HPMIDA)(2)(PMIDA)(2)].2H(2)O (1) was introduced, and its photocatalytic performance was evaluated. The compound exhibited effective water oxidation catalysis, with a turnover number of 661.5 at pH 9.0 using [Ru(bpy)(3)](ClO4)(2) as photosensitizers and sodium persulfate as sacrificial electron acceptor. Accordingly, 1 was used as target catalysts, and the active species was thoroughly investigated under catalytic conditions. The stability of 1 was further tested and confirmed by a series of experiments (cyclic voltammetry (CV), ultraviolet-visible (UV-vis) spectrometry, dynamic light scattering (DLS), aging experiments, and extraction techniques). Results showed that 1 maintained its structural integrity under the given photocatalytic conditions. Furthermore, cathodic adsorptive stripping voltammetry and inductively coupled plasma-mass spectrometry were used to quantify the amount of Co2+ ions released from I into borate buffer after oxidation. The pH dependence of the oxygen-evolution performance of 1 and other cobalt species were then compared. Data collectively revealed that 1 was stable during water oxidation; it did not release free Co2+ ions and was not hydrolyzed to cobalt oxide or hydroxide, thereby confirming that 1 was the effective active species in water-oxidation catalysis. (C) 2016 Elsevier B.V. All rights reserved.
关键词: Precatalysts ; Photocatalytic ; WOCs ; Co complex ; Active species
作者部门: (1) Key Laboratory of Oil and Gas Fine Chemicals, Ministry of Education & Xinjiang Uygur Autonomous Region, College of Chemistry and Chemical Engineering of Xinjiang University, Urumqi ; 830046, China ; (2) College of Chemistry and Chemical Engineering of Lanzhou University, Lanzhou ; 730000, China
通讯作者: Wang, JD (reprint author), Xinjiang Univ, Coll Chem & Chem Engn, Minist Educ & Xinjiang Uygur Autonomous Reg, Key Lab Oil & Gas Fine Chem, Urumqi 830046, Peoples R China.
学科分类: Chemistry; Engineering
文章类型: Article
所属项目编号: National Nature Science Foundation of China (NSFC) [21261022, 21162027]
所属项目名称: 国家自然科学基金项目
项目资助者: NSFC
语种: 英语
DOI: 10.1016/j.apcatb.2016.09.056
ISSN号: 0926-3373
WOS记录号: WOS:000388052100040
EI记录号: 20164002861155
IR记录号: 20164002861155
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内容类型: 期刊论文
URI标识: http://ir.lzu.edu.cn/handle/262010/180614
Appears in Collections:化学化工学院_期刊论文

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Recommended Citation:
Xu, Qian,Li, Hui,Chi, Le,et al. Identification of homogeneous [Co4(H2O)4(HPMIDA)2(PMIDA)2]6−as an effective molecular-light-driven water oxidation catalyst[J]. Applied Catalysis B: Environmental,2017,202:397-403.
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