Co-reporter:Sneh K. Sinha, Yeonsik Noh, Natasa Reljin, Gregory M. Treich, Shirin Hajeb-Mohammadalipour, Yang Guo, Ki H. Chon, and Gregory A. Sotzing
ACS Applied Materials & Interfaces November 1, 2017 Volume 9(Issue 43) pp:37524-37524
Publication Date(Web):October 12, 2017
DOI:10.1021/acsami.7b09954
Electrocardiography (ECG) is an essential technique for analyzing and monitoring cardiovascular physiological conditions such as arrhythmia. This article demonstrates the integration of screen-printed ECG circuitry from a commercially available conducting polymer, PEDOT:PSS, onto commercially available finished textiles. ECG signals were recorded in dry skin conditions due to the ability of PEDOT:PSS to function as both ionic and electronic conductors. The signal amplifies when the skin transpires water vapor or by applying a common lotion on the skin. Finally, PEDOT:PSS wires connected to PEDOT:PSS electrodes have been shown to record ECG signals comparable to Ag/AgCl connected to copper wires.Keywords: electrocardiogram; mixed conduction; PEDOT:PSS; screen printing; wearable electronics;
Co-reporter:Gregory M. Treich, Shamima Nasreen, Arun Mannodi Kanakkithodi, Rui Ma, Mattewos Tefferi, James Flynn, Yang Cao, Rampi Ramprasad, and Gregory A. Sotzing
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 33) pp:21270
Publication Date(Web):July 28, 2016
DOI:10.1021/acsami.6b04091
Recently, there has been a growing interest in developing wide band gap dielectric materials as the next generation insulators for capacitors, photovoltaic devices, and transistors. Organotin polyesters have shown promise as high dielectric constant, low loss, and high band gap materials. Guided by first-principles calculations from density functional theory (DFT), in line with the emerging codesign concept, the polymer poly(dimethyltin 3,3-dimethylglutarate), p(DMTDMG), was identified as a promising candidate for dielectric applications. Blends and copolymers of poly(dimethyltin suberate), p(DMTSub), and p(DMTDMG) were compared using increasing amounts of p(DMTSub) from 10% to 50% to find a balance between electronic properties and film morphology. DFT calculations were used to gain further insight into the structural and electronic differences between p(DMTSub) and p(DMTDMG). Both blend and copolymer systems showed improved results over the homopolymers with the films having dielectric constants of 6.8 and 6.7 at 10 kHz with losses of 1% and 2% for the blend and copolymer systems, respectively. The energy density of the film measured as a D–E hysteresis loop was 6 J/cc for the copolymer, showing an improvement compared to 4 J/cc for the blend. This improvement is hypothesized to come from a more uniform distribution of diacid repeat units in the copolymer compared to the blend, leading toward improved film quality and subsequently higher energy density.Keywords: breakdown; DFT calculation; dielectric properties; polyester; structure; thermal properties; tin; tin ester
Co-reporter:Yang Guo, Michael T. Otley, Mengfang Li, Xiaozheng Zhang, Sneh K. Sinha, Gregory M. Treich, and Gregory A. Sotzing
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 40) pp:26998
Publication Date(Web):September 15, 2016
DOI:10.1021/acsami.6b08036
Herein, the fabrication of all-organic conductive wires is demonstrated by utilizing patterning techniques such as inkjet printing and sponge stencil to apply poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) onto nonwoven polyethylene terephthalate (PET) fabric. The coating of the conducting polymer is only present on the surface of the substrate (penetration depth ∼ 200 μm) to retain the functionality and wearability of the textile. The wires fabricated by different patterning techniques provide a wide range of resistance, i.e., tens of kΩ/□ to less than 2 Ω/□ that allows the resistance to be tailored to a specific application. The sheet resistance is measured to be as low as 1.6 Ω/□, and the breakdown current is as high as 0.37 A for a 1 mm wide line. The specific breakdown current exceeds the previously reported values of macroscopic carbon nanotube based materials. Simple circuits composed of the printed wires are demonstrated, and resistance of the circuit from the measurement agrees with the calculated value based on Kirchhoff’s rules. Additionally, the printed PEDOT:PSS wires show less than 6.2% change in sheet resistance after three washing and drying cycles using detergent.Keywords: conducting polymer; electronic textile; patterning; PEDOT:PSS; wearable electronics
Co-reporter:Aaron F. Baldwin;Rui Ma;Arun Mannodi-Kanakkithodi;Tran Doan Huan;Chenchen Wang;Mattewos Tefferi;Jolanta E. Marszalek;Mukerrem Cakmak;Yang Cao;Rampi Ramprasad
Advanced Materials 2015 Volume 27( Issue 2) pp:346-351
Publication Date(Web):
DOI:10.1002/adma.201404162
Co-reporter:Fahad Alhashmi Alamer, Michael T. Otley, Yumin Zhu, Amrita Kumar, Gregory A. Sotzing
Solar Energy Materials and Solar Cells 2015 Volume 132() pp:131-135
Publication Date(Web):January 2015
DOI:10.1016/j.solmat.2014.08.033
•Photopic contrast was increased by 14% over the control.•The maximum photopic contrast is related to the ionic conductivity maximum.•Experimental results are supported by theory.•Over 50% photopic contrast in electrochromic devices is demonstrated.Herein, we present a versatile way to increase the photopic contrast of electrochromic devices (ECDs), approximately 14%, through the use of binary mixtures of propylene carbonate, diethyl carbonate, and ethylene carbonate that serve the role as plasticizers in the gel electrolyte. The binary plasticizer mixture changed the physical properties of the gel electrolyte medium, including the viscosity and dielectric constant, and also facilitates the diffusion of ions and monomer in the medium leading to an increase in ionic conductivity and the photopic contrast. ECDs were fabricated using a one-step lamination procedure, based on poly(2,2-dimethyl-3,4-propylenedioxythiophene) (PProDOT-Me2) with different polymer gel electrolyte compositions where the electrochromic polymer was electrochemically obtained in situ. Gel electrolytes based on unary or binary plasticizer systems and poly(ethylene glycol) diacrylate (PEG-DA) with varying lithium trifluoromethanesulfonate (LiTrif) loading were investigated for the effect of solvent on ionic conductivity and the resulting photopic contrast of the ECD. This study demonstrates a relationship between photopic contrast and ionic conductivity, where the system reaches a maximum in photopic contrast the system is also at the maximum ionic conductivity.
Co-reporter:Michael T. Otley;Yumin Zhu;Xiaozheng Zhang;Mengfang Li
Advanced Materials 2014 Volume 26( Issue 47) pp:8004-8009
Publication Date(Web):
DOI:10.1002/adma.201403370
Co-reporter:Yumin Zhu, Michael T. Otley, Xiaozheng Zhang, Mengfang Li, Chris Asemota, Geng Li, Michael A. Invernale and Gregory A. Sotzing
Journal of Materials Chemistry A 2014 vol. 2(Issue 46) pp:9874-9881
Publication Date(Web):15 Oct 2014
DOI:10.1039/C4TC01855A
Utilizing the in situ method, we report the fabrication of flexible electrochromic (EC) devices in a one-step lamination procedure. In this study, electrochromic device performance was enhanced via the use of new gel polymer electrolyte (GPE) materials based on poly(ethylene glycol) (PEG) derivatives. PEG serves as the polymer matrix in electrochromic devices (ECDs) that provides not only mechanical stability, but also a wide potential window and compatibility with a variety of salts. Poly(ethylene glycol) dimethacrylate (PEGDMA) in conjunction with poly(ethylene glycol) methyl ether acrylate (PEGMA), containing lithium trifluoromethanesulfonate (LiTRIF) as the salt and propylene carbonate (PC) as a plasticizer; we investigated various electrolyte parameters, including salt loading, the mono/di-functional PEG ratio, and the plasticizer to PEG ratio. Optimized gel systems exceed the mechanical flexibility of indium tin oxide (ITO) coated polyethylene terephthalate (PET) substrates in their sustainable minimum bending radius of curvature, exhibit an ionic conductivity up to 1.36 × 10−3 S cm−1, and yield electrochromic devices (ECDs) with photopic contrasts as high as 53% (without background correction) using poly(2,2-dimethyl-3,4-propylenedioxythiophene) (PProDOT-Me2) as the standard electrochromic material. In addition to ionic conductivity, the crosslink density of the GPEs was found to have an important effect on the photopic contrast of the resultant ECDs. Using these results, 110 cm2 flexible patterned EC displays were assembled as a demonstration of their potential in real world applications.
Co-reporter:Yumin Zhu, Michael T. Otley, Amrita Kumar, Mengfang Li, Xiaozheng Zhang, Chris Asemota and Gregory A. Sotzing
Chemical Communications 2014 vol. 50(Issue 60) pp:8167-8170
Publication Date(Web):19 May 2014
DOI:10.1039/C4CC02289K
Herein, we present a facile, one-step method to color tune electrochromic devices (ECDs) that switch between two neutral colors via in situ electrochemical polymerization of electroactive monomers in the presence of a small molecule organic yellow dye using all commercially available materials. These devices exhibited photopic contrasts of ca. 30% without background correction when assembled on flexible PET-ITO substrates. In addition, devices exhibited switching speeds as low as 1 second, color uniformity, and stability. Large defect free ECDs of 100 cm2 were fabricated exceeding the active switch area required for goggles, lenses, and small display applications.
Co-reporter:Aaron F. Baldwin;Rui Ma;Tran Doan Huan;Yang Cao;Ramamurthy Ramprasad
Macromolecular Rapid Communications 2014 Volume 35( Issue 24) pp:2082-2088
Publication Date(Web):
DOI:10.1002/marc.201400507
Co-reporter:Yumin Zhu, Michael T. Otley, Fahad Alhashmi Alamer, Amrita Kumar, Xiaozheng Zhang, Donna M.D. Mamangun, Mengfang Li, Blaise G. Arden, Gregory A. Sotzing
Organic Electronics 2014 Volume 15(Issue 7) pp:1378-1386
Publication Date(Web):July 2014
DOI:10.1016/j.orgel.2014.03.038
•Photopic contrast was increased to 48%.•Switch speeds were as low as 1%.•Optical memory was as long as 27 h with a photopic transmittance loss of only 2%.•A defect free device of 171 cm2 was constructed using the optimized parameters.Herein, a study on varying salts and their composition used in the gel electrolyte for a one-step lamination assembly procedure for electrochromic devices was carried out to explore their effects on various electrochromic performance parameters, such as color uniformity, photopic contrast, switching speed, and optical memory. Electrochromic polymers formed in different gel electrolyte compositions are highly dependent on the type, amount, and composition of salt used. The following groups of salts were investigated: ionic liquids, ammonium salts, and lithium salts. The lithium salts yielded devices with the best color uniformity, photopic contrast as high as 48%, and switching response speeds as low as 1 s for 5.5 cm2 devices using the electroactive monomer 2,2-dimethyl-3,4-propylenedioxythiophene (ProDOT-Me2) to generate the electrochromic polymer. Hermetically sealed electrochromic devices exhibited optical memory of 27 h for a 2% photopic transmittance loss under normal laboratory conditions, and a 171 cm2 electrochromic device was demonstrated.Graphical abstract
Co-reporter:Robert G. Lorenzini
Journal of Applied Polymer Science 2014 Volume 131( Issue 24) pp:
Publication Date(Web):
DOI:10.1002/app.40179
ABSTRACT
Herein, the synthesis and characterization of a series of Diels–Alder (DA) polymers made with various bis-furans and 1,3-bis(maleimide)propane are described. Due to the fact that these syntheses produce no byproducts inherent to their mechanism, as well as the relative ease at which highly functionalized monomers can be made, these polymers are identified as candidates for dielectric materials with high dielectric constants. The dielectric spectra of these polymers are reported, with an emphasis placed on describing observed structure–property trends. Dielectric constants for these materials range from 4.31 to 6.75 at room temperature, with dielectric losses in the 1–2% regime. These polymers are thermally stable to ∼130°C, where the retro DA reaction was confirmed with multiple analytical methods, including thermogravimetric analysis, differential scanning calorimetry, and gas chromatography/mass spectrometry thermal desorption spectroscopy. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40179.
Co-reporter:Robert G. Lorenzini, Jordan A. Greco, Robert R. Birge, Gregory A. Sotzing
Polymer 2014 Volume 55(Issue 16) pp:3573-3578
Publication Date(Web):5 August 2014
DOI:10.1016/j.polymer.2014.06.041
•The synthesis and characterization of Diels–Alder polysulfones is described.•The syntheses were evaluated a priori using computational HOMO/LUMO data.•Dielectric constants range from 4.96 to 5.98, loss tangents range from 0.4 to 0.9% at 1 kHz.•Bandgaps were determined with UV/Vis spectroscopy, and range between 2.15 and 2.61 eV.•The retro Diels–Alder temperature was determined with 3 analytical methods.Herein, we describe the synthesis and characterization of polymers formed by the Diels–Alder (DA) reaction between various difurans and divinylsulfone, and evaluate their dielectric properties. These syntheses were planned with computational support a priori in the form of HOMO/LUMO calculations for the dienes and dienophiles, with the calculated ΔE for the DA reactions ranging between 9.33 and 9.42 eV. We describe the structure–property relationship observed when changing an atom in the linking unit between two furan rings (–CH2–, –O-, –S-, –NH–) with respect to the dielectric constant and loss tangent. Dielectric constants for the polymers range between 4.96 and 5.98, with dielectric loss tangents ranging from 0.4 to 0.9% at 1 kHz and room temperature. Bandgaps of the polymers are elucidated with UV/Visible spectroscopy, and range from 2.15 to 2.61 eV. The retro DA onset is determined using three analytical methods: thermogravimetric analysis, dynamic scanning calorimetry, and gas chromatography/mass spectrometry polymer desorption spectroscopy, and is determined to be over 125 °C in all cases.
Co-reporter:R.G. Lorenzini, W.M. Kline, C.C. Wang, R. Ramprasad, G.A. Sotzing
Polymer 2013 Volume 54(Issue 14) pp:3529-3533
Publication Date(Web):21 June 2013
DOI:10.1016/j.polymer.2013.05.003
When designing polymeric capacitors, it is important to understand the structure–property relationship between chemical functionalities and dielectric properties to tailor materials for specific applications in terms of dielectric constant, dielectric loss, band gap, breakdown strength, etc. Herein, we report a clear structure–property relationship with dielectric constant and dielectric loss in a series of polyurea and polyurethane thin films. We demonstrate that the dielectric constant systematically increases and the dielectric loss decreases as the number of carbons between polarizable functional groups decreases. Our syntheses are guided with data obtained from high-throughput density functional theory calculations. By modeling 382 polymer systems, we have determined that a dielectric constant >4 is achieved with at least one aromatic group and at least one of the following moieties: –NH–, –C(O)–, or –O–.
Co-reporter:Tanmoy Dey, Michael A. Invernale, Yujie Ding, Zeki Buyukmumcu, and Gregory A. Sotzing
Macromolecules 2011 Volume 44(Issue 8) pp:2415-2417
Publication Date(Web):March 22, 2011
DOI:10.1021/ma102580x
Co-reporter:Arvind Kumar;Michael A. Invernale;Sung-Yeon Jang
Journal of Polymer Science Part A: Polymer Chemistry 2010 Volume 48( Issue 4) pp:756-763
Publication Date(Web):
DOI:10.1002/pola.23819
Abstract
Herein, we report the synthesis of conducting poly (terthiophene)s using a side chain precursor polymer approach. Random copolymers were prepared by ring opening metathesis polymerization of two norbornylene monomers, one containing a pendant terthiophene group and the other containing a pendant acetate group. Solid-state oxidative conversion of the terthiophene units was used to produce conductive polymers. Oxidative solid-state conversion was successful for copolymers containing as little as 1 mol % of terthiophene comonomer. The electrical and optical properties of CPs were studied as a function of the amount of electroactive moiety, terthiophene (3T), present in the copolymer. The CPs were found to have conductivity varying between 10−1 and 10−4 S/cm depending on the precursor copolymer compositions. The CPs obtained from all precursors had no significant difference in their energy gaps and showed blue to orange color transitions when switching from the oxidized to the neutral states, respectively. The absorbance intensity at 426 nm for poly(3T) from the precursors fits the Beer–Lambert law corresponding to the range of initial 3T content in the precursor copolymer composition (from 1 to 100 mol %). © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 756–763, 2010
Co-reporter:Yumin Zhu, Michael T. Otley, Xiaozheng Zhang, Mengfang Li, Chris Asemota, Geng Li, Michael A. Invernale and Gregory A. Sotzing
Journal of Materials Chemistry A 2014 - vol. 2(Issue 46) pp:NaN9881-9881
Publication Date(Web):2014/10/15
DOI:10.1039/C4TC01855A
Utilizing the in situ method, we report the fabrication of flexible electrochromic (EC) devices in a one-step lamination procedure. In this study, electrochromic device performance was enhanced via the use of new gel polymer electrolyte (GPE) materials based on poly(ethylene glycol) (PEG) derivatives. PEG serves as the polymer matrix in electrochromic devices (ECDs) that provides not only mechanical stability, but also a wide potential window and compatibility with a variety of salts. Poly(ethylene glycol) dimethacrylate (PEGDMA) in conjunction with poly(ethylene glycol) methyl ether acrylate (PEGMA), containing lithium trifluoromethanesulfonate (LiTRIF) as the salt and propylene carbonate (PC) as a plasticizer; we investigated various electrolyte parameters, including salt loading, the mono/di-functional PEG ratio, and the plasticizer to PEG ratio. Optimized gel systems exceed the mechanical flexibility of indium tin oxide (ITO) coated polyethylene terephthalate (PET) substrates in their sustainable minimum bending radius of curvature, exhibit an ionic conductivity up to 1.36 × 10−3 S cm−1, and yield electrochromic devices (ECDs) with photopic contrasts as high as 53% (without background correction) using poly(2,2-dimethyl-3,4-propylenedioxythiophene) (PProDOT-Me2) as the standard electrochromic material. In addition to ionic conductivity, the crosslink density of the GPEs was found to have an important effect on the photopic contrast of the resultant ECDs. Using these results, 110 cm2 flexible patterned EC displays were assembled as a demonstration of their potential in real world applications.
Co-reporter:Yumin Zhu, Michael T. Otley, Amrita Kumar, Mengfang Li, Xiaozheng Zhang, Chris Asemota and Gregory A. Sotzing
Chemical Communications 2014 - vol. 50(Issue 60) pp:NaN8170-8170
Publication Date(Web):2014/05/19
DOI:10.1039/C4CC02289K
Herein, we present a facile, one-step method to color tune electrochromic devices (ECDs) that switch between two neutral colors via in situ electrochemical polymerization of electroactive monomers in the presence of a small molecule organic yellow dye using all commercially available materials. These devices exhibited photopic contrasts of ca. 30% without background correction when assembled on flexible PET-ITO substrates. In addition, devices exhibited switching speeds as low as 1 second, color uniformity, and stability. Large defect free ECDs of 100 cm2 were fabricated exceeding the active switch area required for goggles, lenses, and small display applications.