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At least 235 records · Page 13

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DOE OSTI2022

Control over emergence and alignment of transient blisters in thermo-responsive gels using hierarchically patterned substrates

Surfaces with tunable microscale textures are vital in a large variety of technological applications, including heat transfer, antifouling and adhesion. To facilitate such broad-scale use, there is a need to create surfaces that undergo reconfigurable changes in topology and thus, enable switchable functionality. To date, there is a relative dearth of methods for engineering surfaces that can be actuated to change topography over a range of length scales, and hence, form tunable hierarchically structured layers. Combining modeling and experiments, we design a geometrically patterned, thermo-responsive poly (N-isopropylacrylamide) gel film that undergoes controllable hierarchical changes in topology with changes in temperature. At the bottom, the film is covalently bound to a solid, curved substrate; at the top, the film encompasses longitudinal rectangular ridges that are oriented perpendicular to the underlying cylindrical curves. At temperatures below lower critical solution temperature (LCST), the swollen gel exhibits 3D variations in polymer density and thickness defined by the gel's top and bottom topography. As the temperature rises above LCST, the interplay between the upper ridges and lower curves in the gel drives non-uniform, directional solvent transport, the nucleation and propagation of a phase-separated higher-density skin layer, and the resulting pressure buildup within the film. These different, interacting kinetic processes lead to an instability, which produces transient microscopic blisters in the film. Through simulations, we show how tuning the width of the ridges modifies the propagation of a skin layer and creates localized pressure build-up points, which enables control over the emergence, distribution, and alignment of the microscopic blisters. Futhermore, we provide a simple argument to predict the size of such microscopic features. Experiments confirm our predictions and further highlight how our computational model enables the rational design of topographical transitions in these tunable films. The development of actuatable, hierarchically structured films provides new routes for achieving switchable functionality in actuators, drug release systems and adhesives.

42 ENGINEERING↗

DOE OSTI2015

Nanoporous silica-based protocells at multiple scales for designs of life and nanomedicine

In this study, various protocell models have been constructed de novo with the bottom-up approach. Here we describe a silica-based protocell composed of a nanoporous amorphous silica core encapsulated within a lipid bilayer built by self-assembly that provides for independent definition of cell interior and the surface membrane. In this review, we will first describe the essential features of this architecture and then summarize the current development of silica-based protocells at both micro- and nanoscale with diverse functionalities. As the structure of the silica is relatively static, silica-core protocells do not have the ability to change shape, but their interior structure provides a highly crowded and, in some cases, authentic scaffold upon which biomolecular components and systems could be reconstituted. In basic research, the larger protocells based on precise silica replicas of cells could be developed into geometrically realistic bioreactor platforms to enable cellular functions like coupled biochemical reactions, while in translational research smaller protocells based on mesoporous silica nanoparticles are being developed for targeted nanomedicine. Ultimately we see two different motivations for protocell research and development: (1) to emulate life in order to understand it; and (2) to use biomimicry to engineer desired cellular interactions.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Smart Meters Enabling Voltage Monitoring and Control Functionalities: The Last-Mile Voltage Stability Issue

It is a demanding yet challenging task to design the next generation of smart meters. This work investigates the new voltage monitoring and control function for the next-generation smart meters, and identifies its added values for power system voltage stability issues. In terms of voltage monitoring, the risk benefit analysis for adding voltage magnitudes to smart meter measurements is presented, and the risk mitigation strategies along with the co-simulation validation via GridLAB-D and NS-3 are proposed, all providing insight into the new function evaluation. In terms of voltage control, a new voltage stability control scheme is developed, which uses voltage measurements from smart meters and utilizes the observability and controllability of distributed energy resources and controllable loads. Different from traditional voltage control schemes focusing on voltage regulation and power quality monitoring from the utility perspective, the proposed control scheme can achieve the maximum real power transfer margin at the end user side, enabling the voltage stability issues being solved at the grid edge, i.e. the last-mile segment. It is the first work that considers voltage monitoring and control collectively for smart meter investment. It can help power engineering community supplement smart meter applications and shape the next-generation smart meters.

42 ENGINEERING↗

DOE OSTI2020

Enzyme-Directed Functionalization of Designed, Two-Dimensional Protein Lattices

The design and construction of crystalline protein arrays to selectively assemble ordered nanoscale materials has potential applications in sensing, catalysis and medicine. Whereas numerous designs have been implemented for the bottom-up construction of novel protein assemblies, the generation of artificial functional materials has been relatively unexplored. Enzyme-directed post-translational modifications are responsible for the functional diversity of the proteome and thus, could be harnessed to selectively modify artificial protein assemblies. In this study, we describe the use of phosphopantetheinyl transferases (PPTases), a class of enzymes that covalently modify proteins using coenzyme A (CoA), to site-selectively tailor the surface of designed, two-dimensional (2D) protein crystals. We demonstrate that a short peptide (ybbR) or a molecular tag (CoA) can be covalently tethered to 2D arrays to enable enzymatic functionalization using Sfp PPTase. Here, the site-specific modification of two different protein array platforms is facilitated by PPTases to afford both small-molecule- and protein-functionalized surfaces with no loss in crystalline order. This work highlights the potential for chemoenzymatic modification of large protein surfaces towards the generation of sophisticated protein platforms reminiscent of the complex landscape of cell surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2022

All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating

Li 7 La 3 Zr 2 O 12 (LLZO) garnet-type lithium-ion conductors are being investigated as a promising solid electrolyte for solid-state lithium batteries. To enable a functional all-solid-state configuration intensive investigations are needed to reduce the cathode/electrolyte interfacial resistance which contributes the most to cell performance loss. Among the commercial cathode materials investigated so far, LiCoO 2 (LCO) is one of the most stable with garnet electrolytes as only a superficial reaction has been detected between the two materials. However, even this minor reaction would block the Li-ion transport through the interface, resulting in deteriorated cell performance. In this work, we demonstrate that a thin aluminum oxide layer (5 nm) can be an effective interlayer to impede the formation of a harmful interphase and enable facile Li-ion transfer between LCO and the LLZO garnet. Room-temperature-sputtered LCO thin films were employed to form an interface with the garnet electrolyte and annealed at 800 °C to reveal the effect of the interfacial reaction on the Li-ion transfer across the interface. An aluminum oxide layer was then introduced between LCO and the garnet electrolyte by sputtering a metallic aluminum layer which is then annealed together with the upper LCO layer in oxygen, or by direct atomic layer deposition of the oxide. Compared to the LCO/LLZO/Li cells without an aluminum oxide interlayer, those with the interlayer exhibited improved performance, i.e., a stable discharge capacity of up to 90 mAh/(g LCO) at a C/10 rate, a rate capability up to 1.68C and a stable galvanostatic cycling at 0.1C for over 100 cycles with a discharge capacity fade rate of 0.15% per cycle. It was determined that aluminum diffused into the LCO layer after preventing the initial detrimental reaction between LCO and the LLZO garnet from happening during high temperature annealing, suggesting that the coating does not have to remain a physically blocking layer during cycling to function.

Electrochemistry↗

DOE OSTI2016

Transient expression in Nicotiana benthamiana for rapid functional analysis of genes involved in non‐photochemical quenching and carotenoid biosynthesis

Summary Plants must switch rapidly between light harvesting and photoprotection in response to environmental fluctuations in light intensity. This switch can lead to losses in absorbed energy usage, as photoprotective energy dissipation mechanisms can take minutes to hours to fully relax. One possible way to improve photosynthesis is to engineer these energy dissipation mechanisms (measured as non‐photochemical quenching of chlorophyll a fluorescence, NPQ ) to induce and relax more quickly, resulting in smaller losses under dynamic light conditions. Previous studies aimed at understanding the enzymes involved in the regulation of NPQ have relied primarily on labor‐intensive and time‐consuming generation of stable transgenic lines and mutant populations – approaches limited to organisms amenable to genetic manipulation and mapping. To enable rapid functional testing of NPQ ‐related genes from diverse organisms, we performed Agrobacterium tumefaciens ‐mediated transient expression assays in Nicotiana benthamiana to test if NPQ kinetics could be modified in fully expanded leaves. By expressing Arabidopsis thaliana genes known to be involved in NPQ , we confirmed the viability of this method for studying dynamic photosynthetic processes. Subsequently, we used naturally occurring variation in photosystem II subunit S, a modulator of NPQ in plants, to explore how differences in amino acid sequence affect NPQ capacity and kinetics. Finally, we functionally characterized four predicted carotenoid biosynthesis genes from the marine algae Nannochloropsis oceanica and Thalassiosira pseudonana and examined the effect of their expression on NPQ in N. benthamiana . This method offers a powerful alternative to traditional gene characterization methods by providing a fast and easy platform for assessing gene function in planta .

Plant Sciences↗

DOE OSTI2025

Programmable low-coherence wavefronts for enhanced localization

Engineering the properties of electromagnetic wavefronts has become essential to imaging, wireless security, sensing, and wireless communication. In particular, wavefronts that exhibit low spatial coherence can enable sensing functionalities with high accuracy and low latency. The typical use of such wavefronts cannot take advantage of these possibilities, as they require the ability to dynamically reconfigure the wavefront in a controllable and repeatable fashion, over a broad spectral bandwidth. Here, we propose a new approach for generating broadband reconfigurable wavefronts which not only exhibit low spatial coherence at a particular frequency, but are also decorrelated with the wavefronts simultaneously generated at other frequencies. We demonstrate that this frequency-domain decorrelation is a key feature that, in combination with dynamic reconfigurability, enables localization measurements with an order-of-magnitude improvement in accuracy compared to the state of the art.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Functionalized Polymersomes from a Polyisoprene-Activated Polyacrylamide Precursor

Self-assembled polymer nanoparticles have tremendous potential in biomedical and environmental applications. For all applications, tailored polymer chemistries are critical. In this study, we demonstrate a precursor approach in which an activated, organic solvent-soluble block polymer precursor is modified through mild postpolymerization modifications to access new polymer structures. We synthesized and characterized poly(isoprene)-block-poly(di-Boc acrylamide) diblock polymers. This activated-acrylamide-based polymer was then reacted with amines or reductants in the absence of catalysts to yield the hydrophilic blocks polyacrylamide, poly(hydroxypropylene), and poly(N-ethyl acrylamide). The resulting amphiphilic block polymers self-assembled in water to form polymersomes, as confirmed by cryo-electron microscopy and confocal microscopy. The approach also enables simple functionalization with specialized ligands, which we demonstrated by tagging polymers with an amino-fluorophore and imaging by confocal microscopy. Here, we expect that the methodologies established in this study will open doors to new and useful solution nanostructures with surface chemistries that can be optimized for various applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Reduced entropic model for studies of multidimensional nonlocal transport in high-energy-density plasmas

Hydrodynamic simulations of high-energy-density plasmas require a detailed description of energy fluxes. For low and intermediate atomic number materials, the leading mechanism is the electron transport, which may be a nonlocal phenomenon requiring a kinetic modeling. In this paper, we present and test the results of a nonlocal model based on the first angular moments of a simplified Fokker-Planck equation. This multidimensional model is closed thanks to an entropic relation (the Boltzman H-theorem). It provides a better description of the electron distribution function, thus enabling studies of small scale kinetic effects within the hydrodynamic framework. Examples of instabilities of electron plasma and ion-acoustic waves, driven by the heat flux, are presented and compared with the classical formula.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2010

Using digital imaging to assess spectral solar-optical properties of complex fenestration materials: A new approach in video-goniophotometry

A large variety of angularly selective fenestration systems have been developed in the past two decades and show great potential in improving visual comfort while reducing energy consumption, especially when combined with spectrally selective properties. Such systems include light-redirecting glazing, shading, film coatings, reflectors and others. To assess the potential of these systems accurately and reliably, one needs to be able to predict in detail how they modify the energy, direction and spectral make-up of solar radiation. For this assessment, spectral (wavelength-dependent) Bidirectional Transmission or Reflection Distribution Functions are used, usually referred to as BTDFs or BRDFs, or more generally BSDFs for Scattering Functions. To enable a faster, cheaper, and continuous investigation of these properties over most of the solar spectrum (400-1700 nm), an innovative goniospectrometric instrument has been created, relying on digital imaging, on light collection by an ellipsoidal half-transparent mirror, and on a filtering method in the visible range to generate spectral radiometric BSDFs. This so-called Heliodome instrument is described in this paper. It enables the performance of new fenestration technologies to be assessed in terms of lighting and solar gains management potential. The rotating table also serves as a heliodon, an architectural design tool for visualizing sunlight distribution inside a scale model and performing analyses on appropriate sun control strategies. The Heliodome's major innovations compared to other devices are to enable an analysis of both the visible and the near-infrared portions of the solar spectrum, to provide spectral as well as photometric light distribution data, and to ensure a continuous investigation of the transmitted or reflected light in a time-efficient way. (author)

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2017

Expression system for structural and functional studies of human glycosylation enzymes

Vertebrate glycoproteins and glycolipids are synthesized in complex biosynthetic pathways localized predominantly within membrane compartments of the secretory pathway. The enzymes that catalyze these reactions are exquisitely specific, yet few have been extensively characterized because of challenges associated with their recombinant expression as functional products. We used a modular approach to create an expression vector library encoding all known human glycosyltransferases, glycoside hydrolases, and sulfotransferases, as well as other glycan-modifying enzymes. We then expressed the enzymes as secreted catalytic domain fusion proteins in mammalian and insect cell hosts, purified and characterized a subset of the enzymes, and determined the structure of one enzyme, the sialyltransferase ST6GalNAcII. Many enzymes were produced at high yields and at similar levels in both hosts, but individual protein expression levels varied widely. Furthermore, this expression vector library will be a transformative resource for recombinant enzyme production, broadly enabling structure–function studies and expanding applications of these enzymes in glycochemistry and glycobiology.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

A Novel Design for Switchable Grid-Following and Grid-Forming Control

This paper presents the design of a novel grid- forming (GFM) control structure adapted from a typical grid- following (GFL) control structure with minimal edits, thereby enabling a switchable control structure for voltage sourced converters (VSCs) to operate in either GFL or GFM mode by simply switching a flag manually. The VSC is shown to be able to operate in the GFL control mode synchronizing to the main grid through a phase-locked-loop (PLL) and operate as a GFM controller with power-based synchronization for both grid-connected and islanded conditions. To guarantee smooth operation, the control schemes and the mode switching logic have been carefully designed and examined via a series of experiments. Here, the experiment results show that the switchable control structure can fulfill the desired control and operation functions and enable smooth transition between control modes.

14 SOLAR ENERGY↗

DOE OSTI2014

Velocity-space sensitivity of the time-of-flight neutron spectrometer at JET

The velocity-space sensitivities of fast-ion diagnostics are often described by so-called weight functions. Recently, we formulated weight functions showing the velocity-space sensitivity of the often dominant beam-target part of neutron energy spectra. These weight functions for neutron emission spectrometry (NES) are independent of the particular NES diagnostic. Here we apply these NES weight functions to the time-of-flight spectrometer TOFOR at JET. By taking the instrumental response function of TOFOR into account, we calculate time-of-flight NES weight functions that enable us to directly determine the velocity-space sensitivity of a given part of a measured time-of-flight spectrum from TOFOR.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2017

Ion-gel-gating-induced oxygen vacancy formation in epitaxial L a 0.5 S r 0.5 Co O 3 – δ films from in operando x-ray and neutron scattering

Ionic-liquid/gel-based transistors have emerged as a potentially ideal means to accumulate high charge-carrier densities at the surfaces of materials such as oxides, enabling control over electronic phase transitions. Substantial gaps remain in the understanding of gating mechanisms, however, particularly with respect to charge carrier vs oxygen defect creation, one contributing factor being the dearth of experimental probes beyond electronic transport. Here we demonstrate the use of synchrotron hard x-ray diffraction and polarized neutron reflectometry as in operando probes of ion-gel transistors based on ferromagnetic La 0.5 Sr 0.5 CoO 3-δ . An asymmetric gate-bias response is confirmed to derive from electrostatic hole accumulation at negative gate bias vs oxygen vacancy formation at positive bias. The latter is detected via a large gate-induced lattice expansion (up to 1%), complementary bulk measurements and density functional calculations enabling quantification of the bias-dependent oxygen vacancy density. Remarkably, the gate-induced oxygen vacancies proliferate through the entire thickness of 30-40-unit-cell-thick films, quantitatively accounting for changes in the magnetization depth profile. In conclusion, these results directly elucidate the issue of electrostatic vs redox-based response in electrolyte-gated oxides, also demonstrating powerful approaches to their in operando investigation.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Quantum dot coating of baculoviral vectors enables visualization of transduced cells and tissues

Highlights: •The use of quantum dot (QD)-labeled viral vectors for in vivo imaging is not well investigated. •A new method to label enveloped baculovirus with glutathione-capped CdTe QDs is developed. •The labeling enables the identification of transduced, cultured cells based on fluorescence. •The labeling also allows evaluation of viral transduction in a real-time manner in living mice. •The method has the potential to assess viral vector-based gene therapy protocols in future. -- Abstract: Imaging of transduced cells and tissues is valuable in developing gene transfer vectors and evaluating gene therapy efficacy. We report here a simple method to use bright and photostable quantum dots to label baculovirus, an emerging gene therapy vector. The labeling was achieved through the non-covalent interaction of glutathione-capped CdTe quantum dots with the virus envelope, without the use of chemical conjugation. The quantum dot labeling was nondestructive to viral transduction function and enabled the identification of baculoviral vector-transduced, living cells based on red fluorescence. When the labeled baculoviral vectors were injected intravenously or intraventricularly for in vivo delivery of a transgene into mice, quantum dot fluorescence signals allow us monitor whether or not the injected tissues were transduced. More importantly, using a dual-color whole-body imaging technology, we demonstrated that in vivo viral transduction could be evaluated in a real-time manner in living mice. Thus, our method of labeling a read-to-use gene delivery vector with quantum dots could be useful towards the improvement of vector design and will have the potential to assess baculovirus-based gene therapy protocols in future.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

Revealing the working mechanism of a multi-functional block copolymer binder for lithium-sulfur batteries

The lithium-sulfur (Li-S) battery is one of the most promising substitutes for current energy storage systems because of its low cost, high theoretical capacity, and high energy density. However, the high solubility of intermediate products (i.e., lithium polysulfides) and the resultant shuttle effect lead to rapidly fading capacity and a low coulombic efficiency, which hinder the practical application of Li-S batteries. In this study, block copolymers are constructed with both an ethylene oxide unit and a styrene unit and then used as binders for Li-S batteries. Electrochemical performance improvements are attributed to the synergistic effects contributed by the different units of the block copolymer. Here, the ethylene oxide unit traps polysulfide, which bonds strongly with the intermediate lithium polysulfide, and enhances the transport of lithium ions to reach high capacity. Meanwhile, the styrene unit maintains cathode integrity by improving the mechanical properties and elasticity of the constructed block copolymer to accommodate the large volume changes. By enabling multiple functions via different units in the polymer chain, high sulfur utilization is achieved, polysulfide diffusion is confined, and the shuttle effect is suppressed during the cycle life of Li-S batteries, as revealed by operando ultraviolet–visible spectroscopy and S K-edge X-ray absorption spectroscopy.

25 ENERGY STORAGE↗

DOE OSTI2026

Finding the missing pieces: filling gaps that impede the translation of omics data into models

High-throughput omics technologies such as DNA sequencing have made the sequencing and computational assembly of microbial genomes recovered from the environment relatively routine. Computational inference of the protein products encoded by these genomes, and the associated biochemical functions, should enable the accurate prediction and modeling of microbial metabolism, organismal interactions, and ecosystem processes. However, a lack of scalable, probabilistic protein annotation tools limits the full potential of modeling for understanding the metabolism and biogeochemical cycles of microbial communities. Our approach to improve inference of protein annotations and metabolic models relied on learning from and emulating expert manual curation, leveraging software engineering and data science best practices to scale up the throughput and accuracy of annotations and metabolic model construction, building software to objectively evaluate different annotation strategies, and more closely linking the protein annotation and metabolic model inference process. Outcomes of this research include several improved or new computational tools, including DRAM (Distilled and Refined Annotation of Metabolism) for annotating microbial genomes with protein function and metabolic traits, CAMPER (Curated Annotations for Microbial Polyphenol Enzymes and Reactions) for annotating key polyphenol metabolisms, EC-Bench for comprehensive and unbiased benchmarking of annotation tools, and several apps available via the DOE Systems Biology Knowledgebase (KBase) for building genome-scale metabolic models. We demonstrate that these tools allow us to scalably annotate and understand thousands of genomes for microbial communities from a variety of systems and test cases, including rivers, thawing permafrost, and gut microbiomes. All of these computational tools are available as open-source software, with most broadly and easily accessible to the scientific community via KBase apps.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2014

When a single hole aligns several spins: Double exchange in organic systems

The double exchange is a well-known and technically important phenomenon in solid state physics. Ionizing a system composed of two antiferromagnetically coupled high-spin units, the ground state of which is a singlet state, may actually produce a high-spin ground state. This work illustrates the possible occurrence of such a phenomenon in organic chemistry. The here-considered high-spin units are triangulenes, the ground state of which is a triplet. Bridging two of them through a benzene ring produces a molecular architecture of singlet ground state. A careful exploitation of a series of unrestricted density functional calculations enables one to avoid spin contamination in the treatment of the doublet states and shows that under ionization the system becomes of quartet multiplicity in its ground state. The possibility to align more than three spins from conjugated hydrocarbon polyradicals is explored, considering partially hydrogenated triangulenes. A dramatic example shows that ionization of a singlet ground state molecule may generate a decuplet.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗