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Dual Pathways in Catalytic Ammonia Oxidation by a Ruthenium Complex Bearing a Tetradentate Bipyridine-Bipyrazole Ligand: Isolation of a Diruthenium Intermediate with a μ-Hexazene Derivative

文献类型：期刊论文

作者Feng, Sushan1,3,5; Chen, Jing3,4; Wang, Rui3; Li, Hui1,3,5; Xie, Jianhui4; Guo, Zhenguo4; Lau, Tai-Chu2; Liu, Yingying3
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2024-07-26
卷号146
ISSN号0002-7863
DOI10.1021/jacs.4c04326
通讯作者Lau, Tai-Chu(bhtclau@cityu.edu.hk) ; Liu, Yingying(yyliu@iim.ac.cn)
英文摘要We report herein chemical and electrochemical ammonia oxidation (AO) catalyzed by a Ru complex, [Ru-II(H2L)(pic)(2)](2+) [1, H2L = 6,6 '-di(1H-pyrazol-3-yl)-2,2 '-bipyridine, pic = 4-picoline], where H2L is a tetradentate ligand with a bipyridyl unit connected to two pyrazoles. 1 functions as an efficient electrocatalyst for the oxidation of NH3 to N-2, with a low overpotential of 0.51 V vs Fc(+/0) and a Faradaic efficiency of 96%. 1 also undergoes catalytic chemical AO using (4-BrPh)(3)N center dot+ as an oxidant, with a turnover number for N-2 reaching 41. A novel binuclear complex, [Ru-III(L)(pic)(2)(N-2)Ru-III(L)(pic)(2)](4+) (2), was isolated and structurally characterized in the catalytic chemical AO by 1. Complex 2 possesses a zigzag dianionic mu-hexazene unit where the N-2 derived from ammonia oxidation is bonded to the pyrazoles, with an N-N2-N-N2 bond length of 1.3091(70) & Aring;. 2 readily releases N-2 upon treating with NH3. Based on experimental and DFT studies, in chemical AO the formation of an N-N bond is proposed to occur via bimolecular coupling of a ruthenium pyrazole imido intermediate to give 2; while in electrochemical AO the N-N bond is formed by nucleophilic attack of NH3 on the intermediate.
WOS关键词WATER-OXIDATION ; CONVERSION ; HYDRAZINE
资助项目National Natural Science Foundation of China[22001253]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001279679700001
出版者AMER CHEMICAL SOC
资助机构National Natural Science Foundation of China
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/137353]  
专题中国科学院合肥物质科学研究院
通讯作者Lau, Tai-Chu; Liu, Yingying
作者单位1.Anhui Univ, Inst Informat Technol, Hefei 230601, Peoples R China
2.City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China
3.Chinese Acad Sci, Hefei Inst Phys Sci, Inst Intelligent Machines, Hefei 230031, Peoples R China
4.Hefei Univ Technol, Sch Chem & Chem Engn, Anhui Prov Key Lab Adv Catalyt Mat & React Engn, Hefei 230009, Peoples R China
5.Anhui Univ, Inst Phys Sci, Hefei 230601, Peoples R China
推荐引用方式
GB/T 7714		 Feng, Sushan,Chen, Jing,Wang, Rui,et al. Dual Pathways in Catalytic Ammonia Oxidation by a Ruthenium Complex Bearing a Tetradentate Bipyridine-Bipyrazole Ligand: Isolation of a Diruthenium Intermediate with a μ-Hexazene Derivative[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146.
APA Feng, Sushan.,Chen, Jing.,Wang, Rui.,Li, Hui.,Xie, Jianhui.,...&Liu, Yingying.(2024).Dual Pathways in Catalytic Ammonia Oxidation by a Ruthenium Complex Bearing a Tetradentate Bipyridine-Bipyrazole Ligand: Isolation of a Diruthenium Intermediate with a μ-Hexazene Derivative.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146.
MLA Feng, Sushan,et al."Dual Pathways in Catalytic Ammonia Oxidation by a Ruthenium Complex Bearing a Tetradentate Bipyridine-Bipyrazole Ligand: Isolation of a Diruthenium Intermediate with a μ-Hexazene Derivative".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146(2024).

入库方式： OAI收割

来源：合肥物质科学研究院

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