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Title: Robust Chemiresistive Behavior in Conductive Polymer/MOF Composites

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [2];  [4];  [3];  [2]; ORCiD logo [5]
  1. Massachusetts Institute of Technology Department of Materials Science &, Engineering 77 Massachusetts Ave Cambridge MA 02139 USA, Massachusetts Institute of Technology Department of Chemistry 77 Massachusetts Ave Cambridge MA 02139 USA
  2. Massachusetts Institute of Technology Department of Chemistry 77 Massachusetts Ave Cambridge MA 02139 USA
  3. Massachusetts Institute of Technology Department of Chemistry 77 Massachusetts Ave Cambridge MA 02139 USA, Massachusetts Institute of Technology Department of Chemical Engineering 77 Massachusetts Ave Cambridge MA 02139 USA
  4. Massachusetts Institute of Technology Department of Electrical Engineering and Computer Science 77 Massachusetts Ave Cambridge MA 02139 USA, MIT‐IBM Watson AI Lab 75 Binney St Cambridge MA 02139 USA
  5. Massachusetts Institute of Technology Department of Materials Science &, Engineering 77 Massachusetts Ave Cambridge MA 02139 USA
+ Show Author Affiliations

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 ( c MOFs) and conductive polymers ( c Ps) 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 c MOFs 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 c MOF 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 c Ps and c MOFs enables facile thin film co‐processing and device integration, potentially unlocking the use of these hybrid conductors in diverse electronic applications.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0023288; NA0003965
OSTI ID:
2341652
Alternate ID(s):
OSTI ID: 2391015
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 27 Vol. 36; ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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