Mechanistic Understanding of Water Oxidation in the Presence of a Copper Complex by In Situ Electrochemical Liquid Transmission Electron Microscopy
文献类型：期刊论文
| 作者 | Balaghi, S. Esmael; Mehrabani, Somayeh; Mousazade, Younes; Bagheri, Robabeh; Sologubenko, Alla S.; Song, Zhenlun; Patzke, Greta R.; Najafpour, Mohammad Mahdi |
| 刊名 | ACS APPLIED MATERIALS & INTERFACES
 |
| 出版日期 | 2021 |
| 卷号 | 13期号:17页码:19927-19937 |
| 关键词 | HYDROGEN EVOLUTION REACTION MOLECULAR CATALYSTS HOMOGENEOUS CATALYSTS DIOXYGEN EVOLUTION MANGANESE OXIDE CUO NI TRISBIPYRIDYLRUTHENIUM(III) VISUALIZATION BATTERIES |
| 英文摘要 | The design of molecular oxygen-evolution reaction (OER) catalysts requires fundamental mechanistic studies on their widely unknown mechanisms of action. To this end, copper complexes keep attracting interest as good catalysts for the OER, and metal complexes with TMC (TMC = 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane) stand out as active OER catalysts. A mononuclear copper complex, [Cu(TMC)(H2O)](NO3)(2) (TMC = 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane), combined both key features and was previously reported to be one of the most active copper-complex-based catalysts for electrocatalytic OER in neutral aqueous solutions. However, the functionalities and mechanisms of the catalyst are still not fully understood and need to be clarified with advanced analytical studies to enable further informed molecular catalyst design on a larger scale. Herein, the role of nanosized Cu oxide particles, ions, or clusters in the electrochemical OER with a mononuclear copper(II) complex with TMC was investigated by operando methods, including in situ vis-spectroelectrochemistry, in situ electrochemical liquid transmission electron microscopy (EC-LTEM), and extended X-ray absorption fine structure (EXAFS) analysis. These combined experiments showed that Cu oxide-based nanoparticles, rather than a molecular structure, are formed at a significantly lower potential than required for OER and are candidates for being the true OER catalysts. Our results indicate that for the OER in the presence of a homogeneous metal complex-based (pre)catalyst, careful analyses and new in situ protocols for ruling out the participation of metal oxides or clusters are critical for catalyst development. This approach could be a roadmap for progress in the field of sustainable catalysis via informed molecular catalyst design. Our combined approach of in situ TEM monitoring and a wide range of complementary spectroscopic techniques will open up new perspectives to track the transformation pathways and true active species for a wide range of molecular catalysts. |
| 源URL | [http://ir.nimte.ac.cn/handle/174433/21937]  |
| 专题 | 中国科学院宁波材料技术与工程研究所 2021专题_期刊论文 |
| 作者单位 | 1.Najafpour, MM (corresponding author), Inst Adv Studies Basic Sci IASBS, Res Ctr Basic Sci & Modern Technol RBST, Zanjan 4513766731, Iran. 2.Patzke, GR (corresponding author), Univ Zurich, Dept Chem, CH-8057 Zurich, Switzerland. 3.Najafpour, MM (corresponding author), Inst Adv Studies Basic Sci IASBS, Dept Chem, Zanjan 4513766731, Iran. 4.Najafpour, MM (corresponding author), Inst Adv Studies Basic Sci IASBS, Ctr Climate Change & Global Warming, Zanjan 4513766731, Iran. |
| 推荐引用方式 GB/T 7714 | Balaghi, S. Esmael,Mehrabani, Somayeh,Mousazade, Younes,et al. Mechanistic Understanding of Water Oxidation in the Presence of a Copper Complex by In Situ Electrochemical Liquid Transmission Electron Microscopy[J]. ACS APPLIED MATERIALS & INTERFACES,2021,13(17):19927-19937. |
| APA | Balaghi, S. Esmael.,Mehrabani, Somayeh.,Mousazade, Younes.,Bagheri, Robabeh.,Sologubenko, Alla S..,...&Najafpour, Mohammad Mahdi.(2021).Mechanistic Understanding of Water Oxidation in the Presence of a Copper Complex by In Situ Electrochemical Liquid Transmission Electron Microscopy.ACS APPLIED MATERIALS & INTERFACES,13(17),19927-19937. |
| MLA | Balaghi, S. Esmael,et al."Mechanistic Understanding of Water Oxidation in the Presence of a Copper Complex by In Situ Electrochemical Liquid Transmission Electron Microscopy".ACS APPLIED MATERIALS & INTERFACES 13.17(2021):19927-19937. |
入库方式： OAI收割
来源：宁波材料技术与工程研究所
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