Robust Chemiresistive Behavior in Conductive Polymer/MOF Composites
Name
Advanced Materials - 2024 - Roh - Robust Chemiresistive Behavior in Conductive Polymer MOF Composites.pdf
Description
Published version
Size
4.28 MB
Format
Adobe PDF
Checksum (MD5)
eea3cf4ec2ef3670f00a2d535fde8ec3
Author(s)
Roh, Heejung
Kim, Dong‐Ha
Cho, Yeongsu
Jo, Young‐Moo
del Alamo, Jesús A
Kulik, Heather J
Dincă, Mircea
Gumyusenge, Aristide
Date Issued
April 17, 2024
Journal
Advanced Materials
Publisher
Wiley
Citation
H. Roh, D.-H. Kim, Y. Cho, Y.-M. Jo, J. A. del Alamo, H. J. Kulik, M. Dincă, A. Gumyusenge, Robust Chemiresistive Behavior in Conductive Polymer/MOF Composites. Adv. Mater. 2024, 36, 2312382.
Version
Final published version
Abstract
Metal-organic frameworks (MOFs) are promising materials for gas sensing but are often limited to single-use detection. A hybridization strategy is demonstrated synergistically deploying conductive MOFs (cMOFs) and conductive polymers (cPs) as two complementary mixed ionic-electronic conductors in high-performing stand-alone chemiresistors. This work presents significant improvement in i) sensor recovery kinetics, ii) cycling stability, and iii) dynamic range at room temperature. The effect of hybridization across well-studied cMOFs is demonstrated based on 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and 2,3,6,7,10,11-hexaiminotriphenylene (HITP) ligands with varied metal nodes (Co, Cu, Ni). A comprehensive mechanistic study is conducted to relate energy band alignments at the heterojunctions between the MOFs and the polymer with sensing thermodynamics and binding kinetics. The findings reveal that hole enrichment of the cMOF component upon hybridization leads to selective enhancement in desorption kinetics, enabling significantly improved sensor recovery at room temperature, and thus long-term response retention. This mechanism is further supported by density functional theory calculations on sorbate–analyte interactions. It is also found that alloying cPs and cMOFs enables facile thin film co-processing and device integration, potentially unlocking the use of these hybrid conductors in diverse electronic applications.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
MIT-IBM Watson AI Lab
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Creative Commons Attribution-NonCommercial-NoDerivatives
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DOI of Published Version
https://doi.org/10.1002/adma.202312382
