Unprecedented Ultralow Detection Limit of Amines using a Thiadiazole-Functionalized Zr(IV)-Based Metal–Organic Framework
Author(s) -
Arijit Mallick,
Ahmed M. ElZohry,
Osama Shekhah,
Jun Yin,
Jiangtao Jia,
Himanshu Aggarwal,
AbdulHamid Emwas,
Omar F. Mohammed,
Mohamed Eddaoudi
Publication year - 2019
Publication title -
journal of the american chemical society
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 7.115
H-Index - 612
eISSN - 1520-5126
pISSN - 0002-7863
DOI - 10.1021/jacs.9b01839
Subject(s) - chemistry , detection limit , metal organic framework , limit (mathematics) , zirconium , metal , combinatorial chemistry , nanotechnology , inorganic chemistry , nuclear chemistry , organic chemistry , chromatography , adsorption , mathematics , mathematical analysis , materials science
A luminescent Zr(IV)-based metal-organic framework (MOF), with the underlying fcu topology, encompassing a π-conjugated organic ligand with a thiadiazole functionality, exhibits an unprecedented low detection limit of 66 nM for amines in aqueous solution. Markedly, this ultralow detection is driven by hydrogen-bonding interactions between the linker and the hosted amines. This observation is supported by density functional theory (DFT) calculations, which clearly corroborate the suppression of the twisting motion of thiadiazole core in the presence of amine, reducing significantly the nonradiative recombination pathways and subsequently enhancing the emission intensity. Credibly, nicotine regarded as a harmful chemical and bearing an amine pending group is also detected with high sensitivity, positioning this MOF as a potential sensor for practical environmental applications. This finding serves also as a benchmark to understand the sensing mechanism in MOFs.
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