Metal Centers and Organic Ligands Determine Electrochemistry of Metal–Organic Frameworks

金属有机骨架 电化学 吸附 材料科学 金属 无机化学 微分脉冲伏安法 循环伏安法 电极 化学 物理化学 冶金
作者
Caoling Li,Jian Shen,Kangbing Wu,Nianjun Yang
出处
期刊:Small [Wiley]
卷期号:18 (11) 被引量:37
标识
DOI:10.1002/smll.202106607
摘要

Abstract The properties and applications of metal‐organic frameworks (MOFs) can be tuned by their metal centers and organic ligands. To reveal experimentally and theoretically the influence of metal centers and ligands on electrochemical performance of MOFs, three MOFs with copper or zinc centers and organic ligands of 2‐methylimidazole (2MI) or 1,3,5‐benzenetricarboxylic acid (H 3 BTC) are synthesized and characterized in this study. 2D and porous Cu‐2MI exhibits a larger active area, faster electron transfer capability, and stronger adsorption capacity than bulk Cu‐BTC and dodecahedron Zn‐2MI. Density functional theory calculations of adsorption ability of three MOFs toward xanthine (XA), hypoxanthine (HXA), and malachite green (MG) prove that 2D Cu‐2MI has the strongest adsorption energies to three targets. Rotating disk electrode measurements reveal that 2D Cu‐2MI features the biggest intrinsic heterogeneous rate constant toward three analytes. On 2D Cu‐2MI sensitive and selective monitoring of XA, HXA, and MG is then achieved using differential pulse voltammetry. Their monitoring in real samples on 2D Cu‐2MI is accurate and comparable with that using high‐performance liquid chromatography. In summary, regulation of electrochemical sensing features of MOFs is realized through defining selected metal centers and organic ligands.
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