Aerosol-Jet-Printable Covalent Organic Framework Colloidal Inks and Temperature-Sensitive Nanocomposite Films

Nathan P. Bradshaw, Zoheb Hirani, Lidia Kuo, Siyang Li, Nicholas X. Williams, Vinod K. Sangwan, Lindsay E. Chaney, Austin M. Evans, William R. Dichtel*, Mark C. Hersam*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

With molecularly well-defined and tailorable 2D structures, covalent organic frameworks (COFs) have emerged as leading material candidates for chemical sensing, storage, separation, and catalysis. In these contexts, the ability to directly and deterministically print COFs into arbitrary geometries will enable rapid optimization and deployment. However, previous attempts to print COFs have been restricted by low spatial resolution and/or post-deposition polymerization that limits the range of compatible COFs. Here, these limitations are overcome with a pre-synthesized, solution-processable colloidal ink that enables aerosol jet printing of COFs with micron-scale resolution. The ink formulation utilizes the low-volatility solvent benzonitrile, which is critical to obtaining homogeneous printed COF film morphologies. This ink formulation is also compatible with other colloidal nanomaterials, thus facilitating the integration of COFs into printable nanocomposite films. As a proof-of-concept, boronate-ester COFs are integrated with carbon nanotubes (CNTs) to form printable COF-CNT nanocomposite films, in which the CNTs enhance charge transport and temperature sensing performance, ultimately resulting in high-sensitivity temperature sensors that show electrical conductivity variation by 4 orders of magnitude between room temperature and 300 °C. Overall, this work establishes a flexible platform for COF additive manufacturing that will accelerate the incorporation of COFs into technologically significant applications.

Original languageEnglish (US)
Article number2303673
JournalAdvanced Materials
Volume35
Issue number38
DOIs
StatePublished - Sep 21 2023

Funding

N.P.B., Z.H., and L.K. contributed equally to this work. This work was primarily supported by the Department of Energy (Grant DE‐SC0019356). Additional support was provided for the COF synthesis by the Army Research Office Multidisciplinary University Research Initiative (Grant W911NF‐15‐1‐0447), for the charge transport measurements by the Nationals Science Foundation Materials Research Science and Engineering Center (MRSEC) at Northwestern University (Grant DMR‐1720139), and for the screen‐printed graphene electrodes by the U.S. Department of Commerce, National Institute of Standards and Technology (Award 70NANB19H005) as part of the Center for Hierarchical Materials. Z.H., L.K., and N.P.B. also acknowledge support from the National Science Foundation Graduate Research Fellowship Program (Grants DGE‐1842165 and DGE‐1324585, respectively). Portions of this research were performed at Sector 8‐ID‐E of the Advanced Photon Source (APS) a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. Dr. Joseph Strzalka is acknowledged for assistance in collecting synchrotron X‐ray data at high voltages and temperatures. This research also utilized resources available at Beamline 11‐BM (Complex Materials Scattering) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. Dr. Zhang Jiang and Dr. Ruipeng Li are acknowledged for their assistance in collecting synchrotron X‐ray scattering data. This work also made use of the IMSERC Facility at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐2025633). In addition, this work utilized the NUANCE Facility at Northwestern University, which has received support from the SHyNE Resource (NSF ECCS‐2025633) and the Northwestern University MRSEC Program (NSF DMR‐1720139).

Keywords

  • 2D materials
  • additive manufacturing
  • carbon nanotubes
  • covalent organic frameworks
  • temperature sensors

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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