Onset of long-range order in a critical solution of macromolecules
Diffusion broadening in inelastic scattering of monochromatic light off cyclohexane polystyrene, near critical point for mixing
CYCLOHEXANE↗
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Onset of long-range order in a critical solution of macromolecules.
Diffusion broadening in inelastic light scattering of cyclohexane-polystyrene near critical point for mixing
CYCLOHEXANE↗
Advancements in Validation of TSLs through Inelastic Neutron Scattering and Transmission Measurements [Abstract]
Historically, the free gas approximation has been used to treat the thermal scattering of neutrons with energies below a few electron-volts (eV) in unevaluated materials. However, this method inadequately reproduces neutron scattering at these energies. Until recently, only a limited number of materials had available thermal scattering law (TSL) files/libraries in the ENDF nuclear data libraries in this energy range. With advancements in atomistic modeling techniques, such as molecular dynamics, ab-initio molecular dynamics, and density functional theory, TSL libraries have become available for many more materials. This is particularly relevant due to the rising interest in several advanced reactor systems that require novel moderator and reflector materials. While quasi-integral and integral benchmarks have been designed to validate historically important moderator materials (such as light water and polyethylene), there is currently a lack of standard validation methods for TSLs, especially when multiple conflicting TSLs exist. To address this issue, the Oak Ridge National Lab Nuclear Data group has been working on utilizing inelastic neutron scattering (INS) measurements combined with transmission (i.e., total cross section) measurements to evaluate and validate TSLs for different materials. We plan to demonstrate how this method has worked on materials such as polyethylene, lucite, and polystyrene. In addition, we will compare the newly created libraries to ENDF libraries for these materials and explain why integral benchmarks should not be used for validation when multiple TSLs exist.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
High-Performance Mesostructured Organic Hybrid Pseudocapacitor Electrodes
The electrodes of a hybrid electrochemical capacitor which utilize the quinone (Q)-hydroquinone (QH 2 ) couple, a prototypical organic redox system known to provide fast and reversible proton-coupled electron-transfer reactions, are deterministically mesostructured via a colloidal templating strategy to provide good ion and electron transport pathways, enabling a high rate performance. Specifically, a conducting polymer, polypyrrole (PPy), is functionalized with a pseudocapacitive material, a Q/QH 2 -containing catechol derivative, by noncovalent interactions. The mesostructure of this hybrid material is formed into an ordered 3D porous structure by a polystyrene colloidal crystal template-assisted electrosynthesis. The catechol derivative is sufficiently bound to the PPy through noncovalent interactions to provide a volumetric capacitance as high as ≈130 F cm –3 and a capacitance retention of ≈75% over 10 000 charging/discharging cycles. Furthermore, when compared with a randomly structured electrode, the deterministically structured electrode exhibits an improved rate performance due to the mesostructure facilitated electron and ion transport.
36 MATERIALS SCIENCE↗
Cold Sintering Process of Composites: Bridging the Processing Temperature Gap of Ceramic and Polymer Materials
Co-sintering ceramic and thermoplastic polymer composites in a single step with very high volume fractions of ceramics seems unlikely, given the vast differences in the typical sintering temperatures of ceramics versus polymers. These processing limitations are overcome with the introduction of a new sintering approach, namely “cold sintering process” (CSP). CSP utilizes a transient low temperature solvent, such as water or water with dissolved solutes in stoichiometric ratios consistent with the ceramic composition, to control the dissolution and precipitation of ceramics and effect densification between room temperature and ≈200 °C. Under these conditions, thermoplastic polymers and ceramic materials can be jointly formed into dense composites. Three diphasic composite examples are demonstrated to show the overall diversity of composite material design between organic and inorganic oxides, including the microwave dielectric Li 2 MoO 4 –(-C 2 F 4 -) n , electrolyte Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 –(-CH 2 CF 2 -) x [-CF2CF(CF3)-] y, and semiconductor V 2 O 5 –poly(3,4-ethylenedioxythiophene) polystyrene sulfonate composites. Cold sintering is more general and shall have a major impact on the processing of composite materials for many different applications, mechanical, thermal, and electronic, to mention a few possibilities. CSP concepts open up new composite material design and device integration schemes, impacting a wide variety of applications.
36 MATERIALS SCIENCE↗
Tuning Hole Transport Layer Using Urea for High-Performance Perovskite Solar Cells
Interface engineering is critical to the development of highly efficient perovskite solar cells. Here, urea treatment of hole transport layer (e.g., poly(3,4-ethylene dioxythiophene):polystyrene sulfonate (PEDOT:PSS)) is reported to effectively tune its morphology, conductivity, and work function for improving the efficiency and stability of inverted MAPbI 3 perovskite solar cells (PSCs). This treatment has significantly increased MAPbI 3 photovoltaic performance to 18.8% for the urea treated PEDOT:PSS PSCs from 14.4% for pristine PEDOT:PSS devices. The use of urea controls phase separation between PEDOT and PSS segments, leading to the formation of a unique fiber-shaped PEDOT:PSS film morphology with well-organized charge transport pathways for improved conductivity from 0.2 S cm -1 for pristine PEDOT:PSS to 12.75 S cm -1 for 5 wt% urea treated PEDOT:PSS. The urea-treatment also addresses a general challenge associated with the acidic nature of PEDOT:PSS, leading to a much improved ambient stability of PSCs. Additionally, the device hysteresis is significantly minimized by optimizing the urea content in the treatment.
14 SOLAR ENERGY↗
Detection and Signal Processing for Near-Field Nanoscale Fourier Transform Infrared Spectroscopy
Researchers from a broad spectrum of scientific and engineering disciplines are increasingly using scattering-type near-field infrared spectroscopic techniques to characterize materials non-destructively with nanoscale spatial resolution. However, a sub-optimal understanding of a technique's implementation can complicate data interpretation and act as a barrier to entering the field. Here the key detection and processing steps involved in producing scattering-type near-field nanoscale Fourier transform infrared spectra (nano-FTIR) are outlined. The self-contained mathematical and experimental work derives and explains: i) how normalized complex-valued nano-FTIR spectra are generated, ii) why the real and imaginary components of spectra qualitatively relate to dispersion and absorption respectively, iii) a new and generally valid equation for spectra which can be used as a springboard for additional modeling of the scattering processes, and iv) an algebraic expression that can be used to extract an approximation to the sample's local extinction coefficient from nano-FTIR. The algebraic model for weak oscillators is validated with nano-FTIR and attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectra on samples of polystyrene and Kapton and further provides a pedagogical pathway to cementing some of the technique's key qualitative attributes.
36 MATERIALS SCIENCE↗
Preventing Thin Film Dewetting via Graphene Capping
A monolayer 2D capping layer with high Young's modulus is shown to be able to effectively suppress the dewetting of underlying thin films of small organic semiconductor molecule, polymer, and polycrystalline metal, respectively. To verify the universality of this capping layer approach, the dewetting experiments are performed for single‐layer graphene transferred onto polystyrene (PS), semiconducting thienoazacoronene (EH‐TAC), gold, and also MoS 2 on PS. Thermodynamic modeling indicates that the exceptionally high Young's modulus and surface conformity of 2D capping layers such as graphene and MoS 2 substantially suppress surface fluctuations and thus dewetting. As long as the uncovered area is smaller than the fluctuation wavelength of the thin film in a dewetting process via spinodal decomposition, the dewetting should be suppressed. The 2D monolayer‐capping approach opens up exciting new possibilities to enhance the thermal stability and expands the processing parameters for thin film materials without significantly altering their physical properties.
Cao, Peigen↗
Critical Role of Interface and Crystallinity on the Performance and Photostability of Perovskite Solar Cell on Nickel Oxide
Abstract not provided
Nie, Wanyi↗
Solvent-Induced Self-Assembly Strategy to Synthesize Well-Defined Hierarchically Porous Polymers
Porous polymers with well-orchestrated nanomorphologies are useful in many fields, but high surface area, hierarchical structure, and ordered pores are difficult to be satisfied in one polymer simultaneously. A solvent-induced self-assembly strategy to synthesize hierarchical porous polymers with tunable morphology, mesoporous structure, and microporous pore wall is reported. The poly(ethylene oxide)-b-polystyrene (PEO-b-PS) diblock copolymer micelles are cross-linked via Friedel–Crafts reaction, which is a new way to anchor micelles into porous polymers with well-defined structure. Varying the polarity of the solvent has a dramatic effect upon the oleophobic/oleophylic interaction, and the self-assembly structure of PEO-b-PS can be tailored from aggregated nanoparticles to hollow spheres even mesoporous bulk. A morphological phase diagram is accomplished to systematically evaluate the influence of the composition of PEO-b-PS and the mixed solvent component on the pore structure and morphology of products. The hypercrosslinked hollow polymer spheres provide a confined microenvironment for the in situ reduction of K 2 PdCl 4 to ultrasmall Pd nanoparticles, which exhibit excellent catalytic performance in solvent-free catalytic oxidation of hydrocarbons and alcohols.
36 MATERIALS SCIENCE↗
Time-Resolved Structural Kinetics of an Organic Mixed Ionic–Electronic Conductor
The structure and packing of organic mixed ionic–electronic conductors have an especially significant effect on transport properties. In operating devices, this structure is not fixed but is responsive to changes in electrochemical potential, ion intercalation, and solvent swelling. Toward this end, the steady-state and transient structure of the model organic mixed conductor, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), is characterized using multimodal time-resolved operando techniques. Steady-state operando X-ray scattering reveals a doping-induced lamellar expansion of 1.6 Å followed by 0.4 Å relaxation at high doping levels. Time-resolved operando X-ray scattering reveals asymmetric rates of lamellar structural change during doping and dedoping that do not directly depend on potential or charging transients. Further, time-resolved spectroscopy establishes a link between structural transients and the complex kinetics of electronic charge carrier subpopulations, in particular the polaron–bipolaron equilibrium. These findings provide insight into the factors limiting the response time of organic mixed-conductor-based devices, and present the first real-time observation of the structural changes during doping and dedoping of a conjugated polymer system via X-ray scattering.
36 MATERIALS SCIENCE↗
A Low-Swelling Polymeric Mixed Conductor Operating in Aqueous Electrolytes
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99 GENERAL AND MISCELLANEOUS↗
Macroscale Fabrication of Lightweight and Strong Porous Carbon Foams through Template-Coating Pair Design
Manufacturing of low-density-high-strength carbon foams can benefit the construction, transportation, and packaging industries. One successful route to lightweight and mechanically strong carbon foams involves pyrolysis of polymeric architectures, which is inevitably accompanied by drastic volumetric shrinkage (usually >98%). As such, a challenge of these materials lies in maintaining bulk dimensions of building struts that span orders of magnitude difference in length scale from centimeters to nanometers. Here, this work demonstrates fabrication of macroscale low-density-high-strength carbon foams that feature exceptional dimensional stability through pyrolysis of robust template-coating pairs. The template serves as the architectural blueprint and contains strength-imparting properties (e.g., high node density and small strut dimensions); it is composed of a low char-yielding porous polystyrene backbone with a high carbonization-onset temperature. The coating serves to imprint and transcribe the template architecture into pyrolytic carbon; it is composed of a high char-yielding conjugated polymer with a relatively low carbonization-onset temperature. The designed carbonization mismatch enables structural inheritance, while the decomposition mismatch affords hollow struts, minimizing density. The carbons synthesized through this new framework exhibit remarkable dimensional stability (≈80% dimension retention; ≈50% volume retention) and some of the highest specific strengths (≈0.13 GPa g -1 cm 3 ) among reported carbon foams derived from porous polymer templates.
36 MATERIALS SCIENCE↗
Manufacturing Over Many Scales: High Fidelity Macroscale Coverage of Nanoporous Metal Arrays via Lift-Off-Free Nanofabrication
A low-cost, high-throughput, lift-off-free nanolithographic method is developed for creating hexagonal arrays of sub-30-nm-sized pores on a metal film, achieving uniform coverage over an entire wafer of 10 cm in diameter. Additionally, spherical nanodomains of poly(methyl methacrylate) are demonstrated to be well-controlled and self-aligned within a polystyrene matrix layer on a metal thin film without any intermediary coating. After removal of PMMA, the porous PS thin film acts as an etch mask for defining nanoscale pores in the metal underlayer by Ar ion beam milling, resulting in wafer-scale patterning with great fidelity.
36 MATERIALS SCIENCE↗
Roles of Interfacial Tension in Regulating Internal Organization of Low Bandgap Polymer Bulk Heterojunction Solar Cells by Polymer Additives
The role of a tertiary polymer-based additive is investigated in increasing the efficiency of inverted low bandgap polymer:fullerene bulk heterojunction (BHJ) solar cells. Charge separation in polymer BHJ solar cells relies on the phase separation between electron accepting fullerene derivatives and photoactive polymers. Proper distribution of individual phases of suitable crystallinities within the active layer is a key factor for efficient charge transport/extraction and high photovoltaic performance. Here in this paper, it is demonstrated that the minor addition of a tertiary amorphous polymer, polystyrene (PS), with optimized molecular weights can increase the overall photovoltaic efficiency of poly[N-9-heptadecanyl-2,7-carbazole-alt-5,5-(4,7-di-2-thienyl-2,1,3-benzothiadiazole)]:phenyl-C 61 butyric acid methyl ester (PCDTBT:PCBM) inverted BHJ solar cells, through the interfacial-tension-driven increase in crystallinities of photoactive phases and redistribution of PCBM molecules away from the top hole-collecting anode interface. Complementary studies correlating polymer interfacial tension, blend internal structure, charge transport, and photovoltaic characteristics show that tertiary, high molecular-weight polymers can serve as effective additives for improving the performance of low bandgap polymer solar cells.
25 ENERGY STORAGE↗
Laser-Induced Graphene Composites for Printed, Stretchable, and Wearable Electronics
Not provided.
Materials Science↗
4D Printing of Stretchable Supercapacitors via Hybrid Composite Materials
Stretchable supercapacitors (SCs) have attracted significant attention in developing power-independent stretchable electronic systems due to their intrinsic energy storage function and unique mechanical properties. Most current SCs are generally limited by their low stretchability, complicated fabrication process, and insufficient performance and robustness. This study presents a facile method to fabricate arbitrary-shaped stretchable electrodes via 4D printing of conductive composite from reduced graphene oxide, carbon nanotube, and poly(3,4-ethylenedioxythiophene) polystyrene sulfonate. The electrode patterns of an arbitrary shape can be deposited onto prestretched substrates by aerosol-jet printing, then self-organized origami (ridge) patterns are generated after releasing the substrates from holding stretchers due to the mismatched strains. The stretchable electrodes demonstrate superior mechanical robustness and stretchability without sacrificing its outstanding electrochemical performance. The symmetric SC prototype possesses a gravimetric capacitance of ≈21.7 F g -1 at a current density of 0.5 A g -1 and a capacitance retention of ≈85.8% from 0.5 to 5 A g -1 . A SC array with arbitrary-shaped electrodes is also fabricated and connected in series to power light-emitting diode patterns for large-scale applications. Finally, the proposed method paves avenues for scalable manufacturing of future energy-storage devices with controlled extensibility and high electrochemical performance.
36 MATERIALS SCIENCE↗