Centimeter-Scale Pillared-Layer Metal–Organic Framework Thin Films Mediated by Hydroxy Double Salt Intermediates for CO2 Sensor Applications

Kim, Ki-Joong; Ellis, James E.; Howard, Bret H.; Ohodnicki, Paul R.

doi:10.1021/acsami.0c19621

Centimeter-Scale Pillared-Layer Metal–Organic Framework Thin Films Mediated by Hydroxy Double Salt Intermediates for CO₂ Sensor Applications

Journal Article · Tue Dec 22 00:00:00 EST 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c19621· OSTI ID:1842985

^[1]; ^[2]; Howard, Bret H. ^[2]; Ohodnicki, Paul R. ^[2]

National Energy Technology Lab. (NETL), Pittsburgh, PA (United States); Leidos Research Support Team, Pittsburgh, PA (United States)
National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)

Fabrication of metal–organic framework (MOF) thin films over macroscopic surface areas is a subject of great interest for gas sensor application platforms such as optics and microelectronics. However, a direct synthesis of MOF films at ambient conditions, in particular pillared-layer MOF films due to their anisotropic structures, remains a significant challenge. Herein, we demonstrate for the first time a facile construction of dense and continuous pillared-layer MOF thin films on a centimeter scale via an aluminum-doped zinc oxide template and hydroxy double salt (HDS) intermediates at room temperature. A series of Cu(II)-based pillared MOFs with different 1,4-benzenedicarboxylic acid (bdc) ligands were explored for optimizing MOF film formation for CO₂ sensor applications. Nonpolar ligands with lower water solubility preferentially formed crystalline pillared MOF structures from HDS intermediates. A Cu₂(ndc)₂(dabco) (ndc = 1,4-naphthalene-bdc; dabco = 1,4-diazabicyclo[2.2.2]octane) MOF demonstrated the most dense and uniform film growth with micrometer thickness over one square centimeter area. This synthetic approach for growing Cu₂(ndc)₂(dabco) MOF thin films was successfully translated toward two sensing platforms: a quartz crystal microbalance and an optical fiber sensor. These Cu₂(ndc)₂(dabco) MOF-coated sensors displayed sensitivity toward CO₂ and response/recovery time on the scale of seconds, even at moderate humidity levels. Finally, this work provides a road map for producing continuous and anisotropic crystalline MOF thin films over a centimeter scale area on various substrates, which will greatly facilitate their utilization in MOF-based sensor devices, among other applications.

View Accepted Manuscript (DOE)

Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: 89243318CFE000003

OSTI ID:: 1842985

Report Number(s):: RSS371

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 1 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
carbon dioxide sensing in humid conditions
hydroxy double salts
large-scale pillared MOF thin films
layers
ligands
metal organic frameworks
optical fiber sensor
quartz crystal microbalance sensor
sensors
thin films

Centimeter-Scale Pillared-Layer Metal–Organic Framework Thin Films Mediated by Hydroxy Double Salt Intermediates for CO2 Sensor Applications

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Centimeter-Scale Pillared-Layer Metal–Organic Framework Thin Films Mediated by Hydroxy Double Salt Intermediates for CO₂ Sensor Applications