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Jeffrey G. Lundin
Chemistry Division, United States Naval Research Laboratory, Washington, DC 20375, United States

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Research article
Published: 14 July 2021 in ACS ES&T Water
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The removal of oil from bilgewater is necessary for compliance with national and international maritime regulations; however, the formation of stable oil-in-water emulsions makes oil separation difficult. Therefore, it is necessary to understand the physical and chemical properties of emulsions created in bilgewater. Recent experiments have demonstrated that synthetic bilgewater emulsions can be stabilized in the absence of surfactants or cleaners. Consequently, the objective of this study was to determine if compounds found in fuels and lubricating oils can significantly contribute to bilgewater emulsion stability. Surface tension, conductivity, emulsion stability, and GC-MS measurements were conducted to determine transportation of oil additives into the aqueous phase. Results revealed that small polar compounds in common shipboard fuels and lubricants were capable of migrating from the oil phase to the aqueous phase. In particular, it was found that oxygenated alkanes and monoaromatic compounds are likely responsible for the stabilization of bilgewater emulsions. These compounds were found in the highest concentrations in diesel fuel and were found to stabilize simulated bilgewater emulsions more than lubricating oils. Overall, this work shows shipboard oils can contribute to the stabilization of bilgewater emulsions, and further research is needed to determine the full impact of these additives.

ACS Style

Jared Church; Grant C. Daniels; Jeffrey G. Lundin; Woo Hyoung Lee; Danielle Paynter. Stabilization of Bilgewater Emulsions by Shipboard Oils. ACS ES&T Water 2021, 1 .

AMA Style

Jared Church, Grant C. Daniels, Jeffrey G. Lundin, Woo Hyoung Lee, Danielle Paynter. Stabilization of Bilgewater Emulsions by Shipboard Oils. ACS ES&T Water. 2021; ():1.

Chicago/Turabian Style

Jared Church; Grant C. Daniels; Jeffrey G. Lundin; Woo Hyoung Lee; Danielle Paynter. 2021. "Stabilization of Bilgewater Emulsions by Shipboard Oils." ACS ES&T Water , no. : 1.

Research article
Published: 30 December 2020 in Industrial & Engineering Chemistry Research
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This study presents a systematic investigation of bilgewater emulsion characteristics using various in situ analytical methods, while assessing the effect of environmental parameters [e.g., ionic strength, suspended solids (SS), and temperature] on emulsion destabilization. The stabilizing properties of three emulsifiers [Triton X-100, B&B 3100, and sodium dodecyl sulfate (SDS)] were evaluated under various conditions over 5 days. Time-course visual observation, relative oil separation, droplet size distribution, and grayscale intensity profiles were used for the physical characterization of the emulsion samples. In particular, the grayscale intensity was found to be a useful technique for the rapid detection of emulsion separation using simple image analysis. Major findings on bilgewater emulsion stability in this study are as follows: (1) emulsion stability decreased with NaCl (ionic strength) addition and temperature increase, resulting in higher oil separation, (2) emulsions stabilized with B&B 3100 (commercial cleaner) were more stable than Triton X-100 and SDS (neat surfactants) at the equivalent critical micelle concentration, and (3) SSs particle size larger than the initial droplet size could promote the formation of larger emulsion droplets, thus increasing oil coalescence as corroborated by visual observation. Overall, this study highlighted a defined set of easy and rapid emulsion analytical methods, which provided significant information regarding bilgewater emulsion stability. These techniques demonstrated to be a rapid solution for the in situ characterization of bilgewater emulsions primarily in offshore locations lacking sophisticated equipment. These methods can be used for further investigation of other cleaning products found on ships and actual bilgewater samples to assist in the appropriate bilgewater treatment and management.

ACS Style

Daniela Diaz; Jared Church; Marjorie R. Willner; Stephen Sarnyai; Jeffrey G. Lundin; Danielle M. Paynter; Woo Hyoung Lee. Evaluation of Bilgewater Emulsion Stability Using Nondestructive Analytical Methods. Industrial & Engineering Chemistry Research 2020, 60, 1014 -1025.

AMA Style

Daniela Diaz, Jared Church, Marjorie R. Willner, Stephen Sarnyai, Jeffrey G. Lundin, Danielle M. Paynter, Woo Hyoung Lee. Evaluation of Bilgewater Emulsion Stability Using Nondestructive Analytical Methods. Industrial & Engineering Chemistry Research. 2020; 60 (2):1014-1025.

Chicago/Turabian Style

Daniela Diaz; Jared Church; Marjorie R. Willner; Stephen Sarnyai; Jeffrey G. Lundin; Danielle M. Paynter; Woo Hyoung Lee. 2020. "Evaluation of Bilgewater Emulsion Stability Using Nondestructive Analytical Methods." Industrial & Engineering Chemistry Research 60, no. 2: 1014-1025.

Research article
Published: 16 December 2020 in ACS Applied Nano Materials
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The encapsulation of liquid crystals (LCs) within semiflexible, nanoscale media has potential use for developing flexible photodisplays, electronic devices, and sensors. Here, coaxial electrospinning is used to fabricate mats of nanofibers consisting of a polyvinylpyrrolidine polymer sheath and an azobenzene-doped, low-molecular-weight LC core. The addition of the azobenzene chromophore into the LC core allows for the nematic to isotropic phase transition to be initiated photochemically. Fiber morphology was investigated by polarized optical microscopy (POM), differential scanning calorimetry (DSC), and scanning electron microscopy (SEM). Nanofibrous mats were analyzed using differential scanning calorimetry and polarized optical microscopy. Irradiation with UV light triggers the photoisomerization of the azobenzene dopant and the subsequent nematic to isotropic phase transition in the LC core. This was directly observed by the birefringence in the fibrous mats being turned “off” with UV light. Subsequently, the cis–trans isomerization triggered by visible light allows for the reformation of the nematic state and the birefringence being turned “on”. Encapsulation of the liquid crystal within the nanofibers results in precise spatial control over the optical properties of the nanofibers, which is used to photochemically generate detailed images patterned into nanofibrous mats.

ACS Style

Matthew D. Thum; Daniel C. Ratchford; Riccardo Casalini; James H. Wynne; Jeffrey G. Lundin. Azobenzene-Doped Liquid Crystals in Electrospun Nanofibrous Mats for Photochemical Phase Control. ACS Applied Nano Materials 2020, 4, 297 -304.

AMA Style

Matthew D. Thum, Daniel C. Ratchford, Riccardo Casalini, James H. Wynne, Jeffrey G. Lundin. Azobenzene-Doped Liquid Crystals in Electrospun Nanofibrous Mats for Photochemical Phase Control. ACS Applied Nano Materials. 2020; 4 (1):297-304.

Chicago/Turabian Style

Matthew D. Thum; Daniel C. Ratchford; Riccardo Casalini; James H. Wynne; Jeffrey G. Lundin. 2020. "Azobenzene-Doped Liquid Crystals in Electrospun Nanofibrous Mats for Photochemical Phase Control." ACS Applied Nano Materials 4, no. 1: 297-304.

Research article
Published: 06 August 2020 in Polymers for Advanced Technologies
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Conventional insect repellent treatments for fibers, fabrics, and garments suffer from limited durability to repeated laundering and, depending on the insecticide, potential irritation, or toxicity. In this work, electrospinning was employed to control the composition of hierarchically structured functional microscale to nanoscale fibers for tunable insect repellent release by physically incorporating picaridin into nylon‐6,6 nanofibers. The size and morphology of nylon fibers were unaffected by picaridin incorporation, even at loading concentrations up to 50 wt%. Picaridin release kinetics were largely dependent on loading concentration and temperature, as picaridin‐nylon intermolecular interactions were minimal affording diffusion based release. Coaxial nanofibers, in which the sheath component has potential to protect additives in the core for more durable fabrics and act as a diffusion barrier for extended release applications, were also developed and demonstrated altered release kinetics compared to monofilament analogues, indicating the capability to further tune release behavior.

ACS Style

Justin J. Ryan; Riccardo Casalini; Joshua A. Orlicki; Jeffrey G. Lundin. Controlled release of the insect repellent picaridin from electrospun nylon‐6,6 nanofibers. Polymers for Advanced Technologies 2020, 31, 3039 -3047.

AMA Style

Justin J. Ryan, Riccardo Casalini, Joshua A. Orlicki, Jeffrey G. Lundin. Controlled release of the insect repellent picaridin from electrospun nylon‐6,6 nanofibers. Polymers for Advanced Technologies. 2020; 31 (12):3039-3047.

Chicago/Turabian Style

Justin J. Ryan; Riccardo Casalini; Joshua A. Orlicki; Jeffrey G. Lundin. 2020. "Controlled release of the insect repellent picaridin from electrospun nylon‐6,6 nanofibers." Polymers for Advanced Technologies 31, no. 12: 3039-3047.

Research article
Published: 17 June 2020 in Langmuir
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Confinement of liquid crystals (LCs) in polymeric fibers offers a promising strategy to control liquid crystal response to external stimuli. Here, the confinement of 4-cyano-4′-pentylbiphenyl (5CB), a nematic liquid crystal, within the core of coaxially electrospun fibers composed of poly(vinylpyrrolidone) (PVP) containing different surfactants is discussed. The effects of surfactant type, surfactant concentration, and core flow rate (confinement) on the LC behavior were demonstrated using polarized optical microscopy, scanning electron microscopy, differential scanning calorimetry, Raman, and dielectric spectroscopy. Introduction of surfactant dopants of varying hydrophilic and hydrophobic components into the sheath altered the interfacial interaction between the PVP sheath and the 5CB core of the fibers. Significant effects on the LC nematic to isotropic phase transition were attributed to changes in surface anchoring between the sheath and core. Confinement of nematic LCs in surfactant doped polymeric fibers demonstrates a facile method for tuning LC phase behavior.

ACS Style

Kevin T. Dicker; Daniel C Ratchford; Riccardo Casalini; Matthew D. Thum; James H. Wynne; Jeffrey G. Lundin. Surfactant Modulated Phase Transitions of Liquid Crystals Confined in Electrospun Coaxial Fibers. Langmuir 2020, 36, 7916 -7924.

AMA Style

Kevin T. Dicker, Daniel C Ratchford, Riccardo Casalini, Matthew D. Thum, James H. Wynne, Jeffrey G. Lundin. Surfactant Modulated Phase Transitions of Liquid Crystals Confined in Electrospun Coaxial Fibers. Langmuir. 2020; 36 (27):7916-7924.

Chicago/Turabian Style

Kevin T. Dicker; Daniel C Ratchford; Riccardo Casalini; Matthew D. Thum; James H. Wynne; Jeffrey G. Lundin. 2020. "Surfactant Modulated Phase Transitions of Liquid Crystals Confined in Electrospun Coaxial Fibers." Langmuir 36, no. 27: 7916-7924.

Research article
Published: 08 July 2019 in ACS Applied Polymer Materials
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Multi-compartmental ‘core-sheath’ fibers composed of a poly(caprolactone) (PCL) polymer sheath and poly(ethylene glycol) (PEG) fluids as the core materials were designed via coaxial electrospinning. Mechanical stretching of the fibers caused a discontinuous mechanical damping or stiffening behavior when the cores were composed of a PEG fluid as a known non-Newtonian shear-thickening fluid (PEG and SiO2 particles). Surprisingly, it is found that shear-thickening fluids are not a requirement for mechanical damping as is evidenced by similar behavior with Newtonian viscous PEG liquids. Data from optical microscopy, thermogravametric analysis, dynamic mechanical analysis, and rheology have been employed to gain insights into the interactions between the PCL sheath and the PEG cores. The degree of mechanical damping was found to correlate with the viscosity of the core PEGs and is discussed in terms of the interactions between the core and sheath during mechanical oscillation. Further, the non-woven fiber mats were tested for auditory sound attenuation (e.g., white noise, pink noise, frequency steps and chirps). The fiber mats effectively attenuate sound, especially in the low frequency regions where their ability to dissipate energy is most prevalent. It is also clear that the degree of sound attenuation is dependent upon the core liquid viscosity. To the best of our knowledge, the results presented here are the first report of mechanical damping behavior in electrospun core-sheath fibers that employ liquid cores to attenuate auditory sound.

ACS Style

Michael J. Bertocchi; Pearl Vang; Robert B. Balow; James H. Wynne; Jeffrey G. Lundin. Enhanced Mechanical Damping in Electrospun Polymer Fibers with Liquid Cores: Applications to Sound Damping. ACS Applied Polymer Materials 2019, 1, 2068 -2076.

AMA Style

Michael J. Bertocchi, Pearl Vang, Robert B. Balow, James H. Wynne, Jeffrey G. Lundin. Enhanced Mechanical Damping in Electrospun Polymer Fibers with Liquid Cores: Applications to Sound Damping. ACS Applied Polymer Materials. 2019; 1 (8):2068-2076.

Chicago/Turabian Style

Michael J. Bertocchi; Pearl Vang; Robert B. Balow; James H. Wynne; Jeffrey G. Lundin. 2019. "Enhanced Mechanical Damping in Electrospun Polymer Fibers with Liquid Cores: Applications to Sound Damping." ACS Applied Polymer Materials 1, no. 8: 2068-2076.

Full paper
Published: 25 June 2019 in Macromolecular Materials and Engineering
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Tough and elastic microfiber composites composed of an elastic polyurethane (Hydrothane) and a liquid crystalline polymer (Vectran) are fabricated via electrospinning. The composite fibers (HVC) are examined as a function of the mixing ratio of the polymers and evaluated on the bases of fiber formation, morphology, thermal properties, mechanical performance, and fiber alignment. The fiber diameters of the HVCs decrease as the content of Vectran increases. When the fibers are aligned via a rotating target, they have even smaller diameters and increased uniformity than when a static target is employed. Surprisingly, the aligned fibers’ mechanical properties are different than those of random orientation; the HVC fibers of random orientation display increases in strength, toughness, and elastic modulii when increasing amounts of Vectran are incorporated in the fibers. The aforementioned mechanical properties of the aligned fibers decrease somewhat as the content of Vectran is increased. Further, the durability of the aligned fibers is examined by extensional durability tests over ten cycles. The tests indicate that the HVC fibers are very durable and can function as tunable, tough, and elastic fibrous polymer scaffolds and have potential applications in high‐performance composites, polymeric filtration devices, and fibrous bioengineering materials.

ACS Style

Michael J. Bertocchi; Rachel A. Simbana; James H. Wynne; Jeffrey G. Lundin. Electrospinning of Tough and Elastic Liquid Crystalline Polymer–Polyurethane Composite Fibers: Mechanical Properties and Fiber Alignment. Macromolecular Materials and Engineering 2019, 304, 1 .

AMA Style

Michael J. Bertocchi, Rachel A. Simbana, James H. Wynne, Jeffrey G. Lundin. Electrospinning of Tough and Elastic Liquid Crystalline Polymer–Polyurethane Composite Fibers: Mechanical Properties and Fiber Alignment. Macromolecular Materials and Engineering. 2019; 304 (8):1.

Chicago/Turabian Style

Michael J. Bertocchi; Rachel A. Simbana; James H. Wynne; Jeffrey G. Lundin. 2019. "Electrospinning of Tough and Elastic Liquid Crystalline Polymer–Polyurethane Composite Fibers: Mechanical Properties and Fiber Alignment." Macromolecular Materials and Engineering 304, no. 8: 1.

Journal article
Published: 18 December 2018 in Reactive and Functional Polymers
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Hemostatic macroporous polymer foams synthesized via high internal phase emulsion (HIPE) templating were loaded with iodine to impart broad-spectrum antimicrobial activity. The effects of kaolin loading and iodine content on structure and antimicrobial activity were identified. ATR-FTIR, Raman, and XRD provided detailed insight into the complexation of iodine with the cross-linked PEG-NaAA-PEG macroporous polymer matrix. Iodine was found to incorporate into the foams exclusively as triiodide (I3−) ion coordinated to the various carbonyls throughout the polymer structure. Continued, sustained release kinetics of iodine over 48 h was achieved at high iodine loading, while low iodine yielded burst release kinetics. Broad spectrum antimicrobial activity dependent on iodine loading was demonstrated with significant zone of inhibition against E. coli, K. pneumoniae, P. aeruginosa, and S. aureus. This represents the first report of detailed complexation and sustained release of antimicrobial iodine into highly absorbent, hemostatic, and biocompatible polymeric wound dressing material with potential to combat bacterial resistance in infected wounds.

ACS Style

Jeffrey G. Lundin; Christopher L. McGann; Nickolaus K. Weise; Luis A. Estrella; Robert B. Balow; Benjamin C. Streifel; James H. Wynne. Iodine binding and release from antimicrobial hemostatic polymer foams. Reactive and Functional Polymers 2018, 135, 44 -51.

AMA Style

Jeffrey G. Lundin, Christopher L. McGann, Nickolaus K. Weise, Luis A. Estrella, Robert B. Balow, Benjamin C. Streifel, James H. Wynne. Iodine binding and release from antimicrobial hemostatic polymer foams. Reactive and Functional Polymers. 2018; 135 ():44-51.

Chicago/Turabian Style

Jeffrey G. Lundin; Christopher L. McGann; Nickolaus K. Weise; Luis A. Estrella; Robert B. Balow; Benjamin C. Streifel; James H. Wynne. 2018. "Iodine binding and release from antimicrobial hemostatic polymer foams." Reactive and Functional Polymers 135, no. : 44-51.

Research article
Published: 05 July 2018 in The Journal of Physical Chemistry C
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Encapsulation of the nematic liquid crystal N-(methoxybenzylidene)-4-butylaniline (MBBA) into the core of poly(vinylpyrrolidone) (PVP) microfibers has been accomplished via coaxial electrospinning for the first time. Data from optical microscopy, 2D Raman mapping, differential scanning calorimetry, and dielectric spectroscopy have been employed to gain detailed insights into the confinement effects on MBBA in a semi-flexible polymer sheath. The electrospun fiber diameters could be tuned easily by modifying the flow rate of MBBA and both the MBBA core and PVP sheath diameters were determined via Raman line cuts. The PVP sheath induced alignment of MBBA, where its long axis is parallel to the fiber axis. Further, the alignment of MBBA led to iridescence in the fibers, which was found to be temperature sensitive and reversible. Surprisingly, at temperatures below 0 °C, the phase transition temperatures of confined MBBA are different and one of its smectic phases is inhibited by the PVP sheath; however, the phases that occur above 0 °C appear to be unrestricted. Thus, electrospun core-sheath fibers with MBBA and PVP provide a useful platform for a semi-flexible material where it is especially necessary to control liquid crystal alignment and polymorphs or phases at low temperature. Overall, the results reported here provide new and important considerations for the effects of confinement on liquid crystals in semi-flexible media.

ACS Style

Michael J. Bertocchi; Daniel C. Ratchford; Riccardo Casalini; James H. Wynne; Jeffrey G. Lundin. Electrospun Polymer Fibers Containing a Liquid Crystal Core: Insights into Semiflexible Confinement. The Journal of Physical Chemistry C 2018, 122, 16964 -16973.

AMA Style

Michael J. Bertocchi, Daniel C. Ratchford, Riccardo Casalini, James H. Wynne, Jeffrey G. Lundin. Electrospun Polymer Fibers Containing a Liquid Crystal Core: Insights into Semiflexible Confinement. The Journal of Physical Chemistry C. 2018; 122 (29):16964-16973.

Chicago/Turabian Style

Michael J. Bertocchi; Daniel C. Ratchford; Riccardo Casalini; James H. Wynne; Jeffrey G. Lundin. 2018. "Electrospun Polymer Fibers Containing a Liquid Crystal Core: Insights into Semiflexible Confinement." The Journal of Physical Chemistry C 122, no. 29: 16964-16973.

Research article
Published: 14 June 2018 in Industrial & Engineering Chemistry Research
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Highly porous poly(dicyclopentadiene) (pDCPD) foam was synthesized via ring opening metathesis polymerization and high internal phase emulsion (HIPE) templating. Alkane and alkene moieties within the pDCPD foam oxidized slowly in air to form carbonyl, peroxy, and hydroxyl groups. Heating pDCPD to 85 °C in air accelerated the oxidation of pDCPD, producing reactive peroxy species at reduced timescales compared to oxidation at room temperature. The oxidized pDCPD foams rapidly sequestered and decontaminated the toxic chemical warfare agent simulant, demeton-S via oxidation to vinyl and sulfone oxidation products. Additionally, the porosity and high surface area of the pDCPD HIPE foams likely assists in the sequestration of demeton-S via capillary interaction. Collectively, these data demonstrate a new and highly tunable class of polymer materials capable of simultaneous sequestration and decontamination of toxic chemicals.

ACS Style

Robert B. Balow; Spencer L. Giles; Christopher L. McGann; Grant C. Daniels; Jeffrey G. Lundin; Pehr E. Pehrsson; James H. Wynne. Rapid Decontamination of Chemical Warfare Agent Simulant with Thermally Activated Porous Polymer Foams. Industrial & Engineering Chemistry Research 2018, 57, 8630 -8634.

AMA Style

Robert B. Balow, Spencer L. Giles, Christopher L. McGann, Grant C. Daniels, Jeffrey G. Lundin, Pehr E. Pehrsson, James H. Wynne. Rapid Decontamination of Chemical Warfare Agent Simulant with Thermally Activated Porous Polymer Foams. Industrial & Engineering Chemistry Research. 2018; 57 (25):8630-8634.

Chicago/Turabian Style

Robert B. Balow; Spencer L. Giles; Christopher L. McGann; Grant C. Daniels; Jeffrey G. Lundin; Pehr E. Pehrsson; James H. Wynne. 2018. "Rapid Decontamination of Chemical Warfare Agent Simulant with Thermally Activated Porous Polymer Foams." Industrial & Engineering Chemistry Research 57, no. 25: 8630-8634.

Communication
Published: 22 May 2018 in Macromolecular Rapid Communications
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The threat of chemical warfare agents (CWA) compels research into novel self‐decontaminating materials (SDM) for the continued safety of first‐responders, civilians, and active service personnel. The capacity to actively detoxify, as opposed to merely sequester, offending agents under typical environmental conditions defines the added value of SDMs in comparison to traditional adsorptive materials. Porous polymers, synthesized via the high internal phase emulsion (HIPE) templating, provide a facile fabrication method for materials with permeable open cellular structures that may serve in air filtration applications. PolyHIPEs comprising polydicyclopentadiene (polyDCPD) networks form stable hydroperoxide species following activation in air under ambient conditions. The hydroperoxide‐containing polyDCPD materials react quickly with CWA simulants, Demeton‐S and 2‐chloroethyl ethyl sulfide, forming oxidation products as confirmed via gas chromatography mass spectrometry. The simplicity of the detoxification chemistry paired with the porous foam form factor presents an exciting opportunity for the development of self‐decontaminating filter media.

ACS Style

Christopher L. McGann; Grant C. Daniels; Spencer L. Giles; Robert B. Balow; Jorge L. Miranda‐Zayas; Jeffrey G. Lundin; James H. Wynne. Air Activated Self‐Decontaminating Polydicyclopentadiene PolyHIPE Foams for Rapid Decontamination of Chemical Warfare Agents. Macromolecular Rapid Communications 2018, 39, e1800194 .

AMA Style

Christopher L. McGann, Grant C. Daniels, Spencer L. Giles, Robert B. Balow, Jorge L. Miranda‐Zayas, Jeffrey G. Lundin, James H. Wynne. Air Activated Self‐Decontaminating Polydicyclopentadiene PolyHIPE Foams for Rapid Decontamination of Chemical Warfare Agents. Macromolecular Rapid Communications. 2018; 39 (12):e1800194.

Chicago/Turabian Style

Christopher L. McGann; Grant C. Daniels; Spencer L. Giles; Robert B. Balow; Jorge L. Miranda‐Zayas; Jeffrey G. Lundin; James H. Wynne. 2018. "Air Activated Self‐Decontaminating Polydicyclopentadiene PolyHIPE Foams for Rapid Decontamination of Chemical Warfare Agents." Macromolecular Rapid Communications 39, no. 12: e1800194.

Full paper
Published: 17 April 2018 in Macromolecular Bioscience
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A novel hemostatic and absorbent wound dressing material compatible with 3D printing is developed to address deficiencies in current wound dressing protocol. The design involves an open celled, microporous hydrogel foam via a high internal phase emulsion (HIPE) template with biocompatible components and tunable hemostatic character by kaolin loading, the viscosity and cure kinetics of which are tailored for 3D printing applications. The use of nontoxic mineral oil organic phase results in cytocompatability with human dermal fibroblasts. Kaolin distribution is shown by X‐ray diffraction and elemental dispersive spectroscopy to be exfoliated and dispersed in the hydrogel dressing. In addition to demonstrating high fluid absorption and noncytotoxicity of relevant cell lines, the high internal phase emulsion polymers (polyHIPEs) also match the hemostatic performance of commercial wound dressing materials. Furthermore, the polyHIPEs display the requisite rheological properties for 3D printing that result in the fabrication of a prototype dressing with hierarchical porosity and a large number of controllable form factors.

ACS Style

Benjamin C. Streifel; Jeffrey G. Lundin; Allix M. Sanders; Karli A. Gold; Thomas S. Wilems; Sierra J. Williams; Elizabeth Cosgriff‐Hernandez; James H. Wynne. Hemostatic and Absorbent PolyHIPE–Kaolin Composites for 3D Printable Wound Dressing Materials. Macromolecular Bioscience 2018, 18, e1700414 .

AMA Style

Benjamin C. Streifel, Jeffrey G. Lundin, Allix M. Sanders, Karli A. Gold, Thomas S. Wilems, Sierra J. Williams, Elizabeth Cosgriff‐Hernandez, James H. Wynne. Hemostatic and Absorbent PolyHIPE–Kaolin Composites for 3D Printable Wound Dressing Materials. Macromolecular Bioscience. 2018; 18 (5):e1700414.

Chicago/Turabian Style

Benjamin C. Streifel; Jeffrey G. Lundin; Allix M. Sanders; Karli A. Gold; Thomas S. Wilems; Sierra J. Williams; Elizabeth Cosgriff‐Hernandez; James H. Wynne. 2018. "Hemostatic and Absorbent PolyHIPE–Kaolin Composites for 3D Printable Wound Dressing Materials." Macromolecular Bioscience 18, no. 5: e1700414.

Research article
Published: 31 October 2017 in ACS Applied Materials & Interfaces
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Zirconium hydroxide (Zr(OH)4) has excellent sorption properties and wide-ranging reactivity toward numerous types of chemical warfare agents (CWAs) and toxic industrial chemicals. Under pristine laboratory conditions, the effectiveness of Zr(OH)4 has been attributed to a combination of diverse surface hydroxyl species and defects; however, atmospheric components (e.g., CO2, H2O, etc.) and trace contaminants can form adsorbates with potentially detrimental impact to the chemical reactivity of Zr(OH)4. Here, we report the hydrolysis of a CWA simulant, dimethyl methylphosphonate (DMMP) on Zr(OH)4 determined by gas chromatography–mass spectrometry and in situ attenuated total reflectance Fourier transform infrared spectroscopy under ambient conditions. DMMP dosing on Zr(OH)4 formed methyl methylphosphonate and methoxy degradation products on free bridging and terminal hydroxyl sites of Zr(OH)4 under all evaluated environmental conditions. CO2 dosing on Zr(OH)4 formed adsorbed (bi)carbonates and interfacial carbonate complexes with relative stability dependent on CO2 and H2O partial pressures. High concentrations of CO2 reduced DMMP decomposition kinetics by occupying Zr(OH)4 active sites with carbonaceous adsorbates. Elevated humidity promoted hydrolysis of adsorbed DMMP on Zr(OH)4 to produce methanol and regenerated free hydroxyl species. Hydrolysis of DMMP by Zr(OH)4 occurred under all conditions evaluated, demonstrating promise for chemical decontamination under diverse, real-world conditions.

ACS Style

Robert B. Balow; Jeffrey G. Lundin; Grant C. Daniels; Wesley Gordon; Monica McEntee; Gregory W. Peterson; James H. Wynne; Pehr E. Pehrsson. Environmental Effects on Zirconium Hydroxide Nanoparticles and Chemical Warfare Agent Decomposition: Implications of Atmospheric Water and Carbon Dioxide. ACS Applied Materials & Interfaces 2017, 9, 39747 -39757.

AMA Style

Robert B. Balow, Jeffrey G. Lundin, Grant C. Daniels, Wesley Gordon, Monica McEntee, Gregory W. Peterson, James H. Wynne, Pehr E. Pehrsson. Environmental Effects on Zirconium Hydroxide Nanoparticles and Chemical Warfare Agent Decomposition: Implications of Atmospheric Water and Carbon Dioxide. ACS Applied Materials & Interfaces. 2017; 9 (45):39747-39757.

Chicago/Turabian Style

Robert B. Balow; Jeffrey G. Lundin; Grant C. Daniels; Wesley Gordon; Monica McEntee; Gregory W. Peterson; James H. Wynne; Pehr E. Pehrsson. 2017. "Environmental Effects on Zirconium Hydroxide Nanoparticles and Chemical Warfare Agent Decomposition: Implications of Atmospheric Water and Carbon Dioxide." ACS Applied Materials & Interfaces 9, no. 45: 39747-39757.

Journal article
Published: 01 October 2017 in Materials Science and Engineering: C
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There are numerous challenges associated with the acute care of traumatic limb injuries in forward military settings. A lack of immediate medical facilities necessitates that the wound dressing perform multiple tasks including exudate control, infection prevention, and physical protection of the wound for extended periods of time. Here, kaolin was incorporated into recently developed robust polyurethane (PU) hydrogel foams at 1-10wt% in an effort to impart hemostatic character. ATR-IR and gel fraction analysis demonstrated that the facile, one-pot synthesis of the PU hydrogel was unaffected by kaolin loading, as well as the use of a non-toxic catalyst, which significantly improved cytocompatibility of the materials. Kaolin was generally well dispersed throughout the PU matrix, though higher loadings exhibited minor evidence of aggregation. Kaolin-PU composites exhibited burst release of ciprofloxacin over 2h, the initial release rates of which increased with kaolin loading. Kaolin loading imparted excellent hemostatic character to the PU foams at relatively low loading levels (5wt%). This work demonstrates the simple and inexpensive synthesis of robust, hemostatic, and absorptive kaolin-PU foams that have promising potential as multifunctional wound dressing materials.

ACS Style

Jeffrey G. Lundin; Christopher L. McGann; Grant C. Daniels; Benjamin C. Streifel; James H. Wynne. Hemostatic kaolin-polyurethane foam composites for multifunctional wound dressing applications. Materials Science and Engineering: C 2017, 79, 702 -709.

AMA Style

Jeffrey G. Lundin, Christopher L. McGann, Grant C. Daniels, Benjamin C. Streifel, James H. Wynne. Hemostatic kaolin-polyurethane foam composites for multifunctional wound dressing applications. Materials Science and Engineering: C. 2017; 79 ():702-709.

Chicago/Turabian Style

Jeffrey G. Lundin; Christopher L. McGann; Grant C. Daniels; Benjamin C. Streifel; James H. Wynne. 2017. "Hemostatic kaolin-polyurethane foam composites for multifunctional wound dressing applications." Materials Science and Engineering: C 79, no. : 702-709.

Journal article
Published: 01 September 2017 in Polymer
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ACS Style

Christopher L. McGann; Benjamin C. Streifel; Jeffrey G. Lundin; James H. Wynne. Multifunctional polyHIPE wound dressings for the treatment of severe limb trauma. Polymer 2017, 126, 408 -418.

AMA Style

Christopher L. McGann, Benjamin C. Streifel, Jeffrey G. Lundin, James H. Wynne. Multifunctional polyHIPE wound dressings for the treatment of severe limb trauma. Polymer. 2017; 126 ():408-418.

Chicago/Turabian Style

Christopher L. McGann; Benjamin C. Streifel; Jeffrey G. Lundin; James H. Wynne. 2017. "Multifunctional polyHIPE wound dressings for the treatment of severe limb trauma." Polymer 126, no. : 408-418.

Journal article
Published: 01 July 2017 in Applied Catalysis A: General
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ACS Style

Spencer L. Giles; Jeffrey G. Lundin; Bobby Balow; Pehr E. Pehrsson; James H. Wynne. Comparative roles of Zr4+ and Ni2+ Wells-Dawson hetero-metal substituted polyoxometalates on oxidation of chemical contaminants. Applied Catalysis A: General 2017, 542, 306 -310.

AMA Style

Spencer L. Giles, Jeffrey G. Lundin, Bobby Balow, Pehr E. Pehrsson, James H. Wynne. Comparative roles of Zr4+ and Ni2+ Wells-Dawson hetero-metal substituted polyoxometalates on oxidation of chemical contaminants. Applied Catalysis A: General. 2017; 542 ():306-310.

Chicago/Turabian Style

Spencer L. Giles; Jeffrey G. Lundin; Bobby Balow; Pehr E. Pehrsson; James H. Wynne. 2017. "Comparative roles of Zr4+ and Ni2+ Wells-Dawson hetero-metal substituted polyoxometalates on oxidation of chemical contaminants." Applied Catalysis A: General 542, no. : 306-310.

Journal article
Published: 01 April 2017 in Progress in Organic Coatings
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Jeffrey G. Lundin; Spencer L. Giles; Preston A. Fulmer; James H. Wynne. Distribution of quaternary ammonium salt encapsulated polyoxometalates in polyurethane films. Progress in Organic Coatings 2017, 105, 320 -329.

AMA Style

Jeffrey G. Lundin, Spencer L. Giles, Preston A. Fulmer, James H. Wynne. Distribution of quaternary ammonium salt encapsulated polyoxometalates in polyurethane films. Progress in Organic Coatings. 2017; 105 ():320-329.

Chicago/Turabian Style

Jeffrey G. Lundin; Spencer L. Giles; Preston A. Fulmer; James H. Wynne. 2017. "Distribution of quaternary ammonium salt encapsulated polyoxometalates in polyurethane films." Progress in Organic Coatings 105, no. : 320-329.

Article
Published: 05 December 2016 in Macromolecular Materials and Engineering
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Jeffrey G. Lundin; Grant C. Daniels; Christopher L. McGann; Joshua Stanbro; Chaselynn Watters; Michael Stockelman; James H. Wynne. Multi‐Functional Polyurethane Hydrogel Foams with Tunable Mechanical Properties for Wound Dressing Applications. Macromolecular Materials and Engineering 2016, 302, 1 .

AMA Style

Jeffrey G. Lundin, Grant C. Daniels, Christopher L. McGann, Joshua Stanbro, Chaselynn Watters, Michael Stockelman, James H. Wynne. Multi‐Functional Polyurethane Hydrogel Foams with Tunable Mechanical Properties for Wound Dressing Applications. Macromolecular Materials and Engineering. 2016; 302 (3):1.

Chicago/Turabian Style

Jeffrey G. Lundin; Grant C. Daniels; Christopher L. McGann; Joshua Stanbro; Chaselynn Watters; Michael Stockelman; James H. Wynne. 2016. "Multi‐Functional Polyurethane Hydrogel Foams with Tunable Mechanical Properties for Wound Dressing Applications." Macromolecular Materials and Engineering 302, no. 3: 1.

Research article
Published: 26 July 2016 in The Journal of Physical Chemistry C
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Polyoxometalates (POMs) exhibit catalytic activity toward a variety of harmful chemicals such as chemical warfare agents, qualifying them as promising candidates as additives to create self-decontaminating surfaces and materials. However, POMs exhibit poor solubility and dispersion behavior in organic matrices, including polymeric coatings. In an effort to improve compatibility with polymer coatings and impart surface segregating behavior, we describe the encapsulation of a Ni(II)-containing POM, α2-K8P2W17O61(Ni2+∙OH2)∙17 H2O (Ni-POM), with a series of amphiphilic alkyl ethoxy dimethyl quaternary ammonium salts (QASs) and elucidate their structural coordination. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA) were utilized to confirm that QASs are coordinated to the Ni-POM and that the average number of QAS coordinated to each Ni-POM increases with increasing alkyl moiety length. The 1H NMR spectra of the QAS(Ni-POM) complexes show marked site-specific broadening and reduced spin-lattice relaxation times T1 compared to either a non-paramagnetic QAS(POM) complex or the neat QAS ligand. These paramagnetic relaxation enhancement (PRE) effects were used to obtain structural and dynamical information about the binding of QASs to the Ni-POM. The single-exponential saturation recovery behavior observed in all cases indicated that all bound QAS molecules are rapidly moving about the entire (Ni-POM) surface on a time scale less than tens of milliseconds. Motionally-averaged distances of the QAS protons to the paramagnetic Ni2+ center were estimated using a modified Solomon-Bloembergen equation. Comparisons of relative distances for protons at different sites on the QAS molecule provide key insights into the structural nature of the bonding. Surprisingly, the ethylene oxide moiety of the amphiphilic QAS was found to coordinate more closely with the surface of the Ni-POM than the quaternary ammonium nitrogen cation, and the alkyl moieties extended outwards from the Ni-POM center. These results suggest that QAS(Ni-POM) complexes should behave effectively as a hydrophobic non-polar complexes in their desired roles as catalytic centers in coatings.

ACS Style

Jeffrey G. Lundin; Spencer L. Giles; James P. Yesinowski; Brian T. Rasley; James H. Wynne. Nature of Polyoxometalate Intramolecular Coordination to Quaternary Ammonium Salts from Paramagnetic Relaxation Enhancement. The Journal of Physical Chemistry C 2016, 120, 17767 -17776.

AMA Style

Jeffrey G. Lundin, Spencer L. Giles, James P. Yesinowski, Brian T. Rasley, James H. Wynne. Nature of Polyoxometalate Intramolecular Coordination to Quaternary Ammonium Salts from Paramagnetic Relaxation Enhancement. The Journal of Physical Chemistry C. 2016; 120 (31):17767-17776.

Chicago/Turabian Style

Jeffrey G. Lundin; Spencer L. Giles; James P. Yesinowski; Brian T. Rasley; James H. Wynne. 2016. "Nature of Polyoxometalate Intramolecular Coordination to Quaternary Ammonium Salts from Paramagnetic Relaxation Enhancement." The Journal of Physical Chemistry C 120, no. 31: 17767-17776.

Journal article
Published: 13 August 2014 in Coatings
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Surfaces are often coated with paint for improved aesthetics and protection; however, additional functionalities that impart continuous self-decontaminating and self-cleaning properties would be extremely advantageous. In this report, photochemical additives based on C60 fullerene were incorporated into polyurethane coatings to investigate their coating compatibility and ability to impart chemical decontaminating capability to the coating surface. C60 exhibits unique photophysical properties, including the capability to generate singlet oxygen upon exposure to visible light; however, C60 fullerene exhibits poor solubility in solvents commonly employed in coating applications. A modified C60 containing a hydrophilic moiety was synthesized to improve polyurethane compatibility and facilitate segregation to the polymer–air interface. Bulk properties of the polyurethane films were analyzed to investigate additive–coating compatibility. Coatings containing photoactive additives were subjected to self-decontamination challenges against representative chemical contaminants and the effects of additive loading concentration, light exposure, and time on chemical decontamination are reported. Covalent attachment of an ethylene glycol tail to C60 improved its solubility and dispersion in a hydrophobic polyurethane matrix. Decomposition products resulting from oxidation were observed in addition to a direct correlation between additive loading concentration and decomposition of surface-residing contaminants. The degradation pathways deduced from contaminant challenge byproduct analyses are detailed.

ACS Style

Jeffrey G. Lundin; Spencer L. Giles; Robert F. Cozzens; James H. Wynne. Self-Cleaning Photocatalytic Polyurethane Coatings Containing Modified C60 Fullerene Additives. Coatings 2014, 4, 614 -629.

AMA Style

Jeffrey G. Lundin, Spencer L. Giles, Robert F. Cozzens, James H. Wynne. Self-Cleaning Photocatalytic Polyurethane Coatings Containing Modified C60 Fullerene Additives. Coatings. 2014; 4 (3):614-629.

Chicago/Turabian Style

Jeffrey G. Lundin; Spencer L. Giles; Robert F. Cozzens; James H. Wynne. 2014. "Self-Cleaning Photocatalytic Polyurethane Coatings Containing Modified C60 Fullerene Additives." Coatings 4, no. 3: 614-629.