https://scholars.lib.ntu.edu.tw/handle/123456789/631327
標題: | Molecular Engineering of Metal–Organic Frameworks as Efficient Electrochemical Catalysts for Water Oxidation | 作者: | Liu, Yizhe Li, Xintong Zhang, Shoufeng Wang, Zilong Wang, Qi He, Yonghe WEI-HSIANG HUANG Sun, Qidi Zhong, Xiaoyan Hu, Jue Guo, Xuyun Lin, Qing Li, Zhuo Zhu, Ye CHU-CHEN CHUEH Chen, Chi Liang Xu, Zhengtao Zhu, Zonglong |
關鍵字: | metal–organic frameworks | nickel–mercaptan links | oxygen evolution | thiol functionalization | 公開日期: | 1-一月-2023 | 出版社: | WILEY-V C H VERLAG GMBH | 來源出版物: | Advanced Materials | 摘要: | Metal–organic framework (MOF) solids with their variable functionalities are relevant for energy conversion technologies. However, the development of electroactive and stable MOFs for electrocatalysis still faces challenges. Here, a molecularly engineered MOF system featuring a 2D coordination network based on mercaptan–metal links (e.g., nickel, as for Ni(DMBD)-MOF) is designed. The crystal structure is solved from microcrystals by a continuous-rotation electron diffraction (cRED) technique. Computational results indicate a metallic electronic structure of Ni(DMBD)-MOF due to the Ni–S coordination, highlighting the effective design of the thiol ligand for enhancing electroconductivity. Additionally, both experimental and theoretical studies indicate that (DMBD)-MOF offers advantages in the electrocatalytic oxygen evolution reaction (OER) over non-thiol (e.g., 1,4-benzene dicarboxylic acid) analog (BDC)-MOF, because it poses fewer energy barriers during the rate-limiting *O intermediate formation step. Iron-substituted NiFe(DMBD)-MOF achieves a current density of 100 mA cm−2 at a small overpotential of 280 mV, indicating a new MOF platform for efficient OER catalysis. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/631327 | ISSN: | 09359648 | DOI: | 10.1002/adma.202300945 |
顯示於: | 化學工程學系 |
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