Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni3(hexaiminotriphenylene)2
| Autor: | Elise M. Miner, Ernest Pastor, Nathan D. Ricke, Sheraz Gul, Mircea Dincă, Troy Van Voorhis, Vittal K. Yachandra, Junko Yano |
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| Rok vydání: | 2017 |
| Předmět: |
biology
Chemistry Ligand Inorganic chemistry Active site 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Electrocatalyst 01 natural sciences Combinatorial chemistry Catalysis 0104 chemical sciences Metal visual_art biology.protein visual_art.visual_art_medium Metal-organic framework Reactivity (chemistry) 0210 nano-technology Selectivity |
| Zdroj: | Miner, EM; Gul, S; Ricke, ND; Pastor, E; Yano, J; Yachandra, VK; et al.(2017). Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni3(hexaiminotriphenylene)2. ACS Catalysis, 7(11), 7726-7731. doi: 10.1021/acscatal.7b02647. Lawrence Berkeley National Laboratory: Retrieved from: http://www.escholarship.org/uc/item/8fr4t6mt |
| ISSN: | 2155-5435 |
| DOI: | 10.1021/acscatal.7b02647 |
| Popis: | © 2017 American Chemical Society. Establishing catalytic structure-function relationships introduces the ability to optimize the catalyst structure for enhanced activity, selectivity, and durability against reaction conditions and prolonged catalysis. Here we present experimental and computational data elucidating the mechanism for the O2reduction reaction with a conductive nickel-based metal-organic framework (MOF). Elucidation of the O2reduction electrokinetics, understanding the role of the extended MOF structure in providing catalytic activity, observation of how the redox activity and pKaof the organic ligand influences catalysis, and identification of the catalyst active site yield a detailed O2reduction mechanism where the ligand, rather than the metal, plays a central role. More generally, familiarization with how the structural and electronic properties of the MOF influence reactivity may provide deeper insight into the mechanisms by which less structurally defined nonplatinum group metal electrocatalysts reduce O2. |
| Databáze: | OpenAIRE |
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