Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 50, Pages 60306-60318Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c14453
Keywords
bismuth; coordination network; chemiresistor; crystalline; gas sensor; microelectron diffraction; semiconductive
Funding
- Dartmouth College, Walter and Constance Burke Research Initiation Award
- Irving Institute for Energy and Society
- National Institutes of Health [R35GM138318]
- National Science Foundation CAREER Award [1945218]
- National Science Foundation EPSCoR award [1757371]
- Army Research Office [W911NF-17-1-0398]
- US Army Cold Regions Research & Engineering Lab [W913E519C0008]
- Sloan Research Fellowship [FG2018-10561]
- Cottrell Scholars Award from the Research Corporation for Science Advancement [26019]
- Camille Dreyfus Teacher-Scholar Award
- Packard Foundation
- National Science Foundation Graduate Research Fellowship Program [DGE1650604]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1945218] Funding Source: National Science Foundation
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This paper presents the design, synthesis, characterization, and performance of a novel semiconductive crystalline coordination network utilizing HHTP ligands interconnected with bismuth ions for chemiresistive gas sensing. Bi(HHTP) exhibits two distinct structures and good electrical conductivity, enabling detection of gases and volatile organic compounds, with unique responses to VOCs at ppm concentrations. Spectroscopic analysis suggests the sensing mechanisms involve a complex combination of steric, electronic, and protic properties of the targeted analytes.
This paper describes the design, synthesis, characterization, and performance of a novel semiconductive crystalline coordination network, synthesized using 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) ligands interconnected with bismuth ions, toward chemiresistive gas sensing. Bi(HHTP) exhibits two distinct structures upon hydration and dehydration of the pores within the network, Bi(HHTP)-alpha and Bi(HHTP)-beta, respectively, both with unprecedented network topology (2,3-c and 3,4,4,5-c nodal net stoichiometry, respectively) and unique corrugated coordination geometries of HHTP molecules held together by bismuth ions, as revealed by a crystal structure resolved via microelectron diffraction (MicroED) (1.00 angstrom resolution). Good electrical conductivity (5.3 x 10(-3) S.cm(-1)) promotes the utility of this material in the chemical sensing of gases (NH3 and NO) and volatile organic compounds (VOCs: acetone, ethanol, methanol, and isopropanol). The chemiresistive sensing of NO and NH3 using Bi(HHTP) exhibits limits of detection 0.15 and 0.29 parts per million (ppm), respectively, at low driving voltages (0.1-1.0 V) and operation at room temperature. This material is also capable of exhibiting unique and distinct responses to VOCs at ppm concentrations. Spectroscopic assessment via X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopic methods (i.e., attenuated total reflectance-infrared spectroscopy (ATR-IR) and diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS)), suggests that the sensing mechanisms of Bi(HHTP) to VOCs, NO, and NH3 comprise a complex combination of steric, electronic, and protic properties of the targeted analytes.
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