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At least 829 records · Page 46

A New Method for Creating Structured High-Performance Current Collectors for Electrochemical Applications

A significant challenge in many electrochemical systems is finding a stable, high-performing current collector material that is mechanically robust, adaptable in form factor, and free of precious metals. Titanium electrodes are robust in many of these regards but exhibit poor charge transfer performance due to self-passivation. Herein, a new materials processing paradigm based on the titanium/titanium nitride (Ti/TiN) system which allows for robust, stable, and low-resistance current collectors of arbitrary form factor is presented. Specifically, a gas-nitriding process for 3D-printed titanium electrodes that results in a 20-fold improvement of charge transfer characteristics relative to the untreated material is outlined. The ability to utilize 3D-structured current collectors with a net 40-fold improvement in performance over nonstructured electrodes is further demonstrated. This novel approach to creating electrochemical current collectors requires minimal laboratory resources and can be widely adapted for a variety of applications, including desalination, electrolysis, energy storage, and basic research. In conclusion, the work described herein provides both a means for accelerating research and opens the door to hierarchical tuneability for enhanced performance.

36 MATERIALS SCIENCE↗

DNA-assembled superconducting 3D nanoscale architectures

Studies of nanoscale superconducting structures have revealed various physical phenomena and led to the development of a wide range of applications. Most of these studies concentrated on one- and two-dimensional structures due to the lack of approaches for creation of fully engineered three-dimensional (3D) nanostructures. Here, we present a ‘bottom-up’ method to create 3D superconducting nanostructures with prescribed multiscale organization using DNA-based self-assembly methods. We assemble 3D DNA superlattices from octahedral DNA frames with incorporated nanoparticles, through connecting frames at their vertices, which result in cubic superlattices with a 48 nm unit cell. The superconductive superlattice is formed by converting a DNA superlattice first into highly-structured 3D silica scaffold, to turn it from a soft and liquid-environment dependent macromolecular construction into a solid structure, following by its coating with superconducting niobium (Nb). Through low-temperature electrical characterization we demonstrate that this process creates 3D arrays of Josephson junctions. This approach may be utilized in development of a variety of applications such as 3D Superconducting Quantum interference Devices (SQUIDs) for measurement of the magnetic field vector, highly sensitive Superconducting Quantum Interference Filters (SQIFs), and parametric amplifiers for quantum information systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Biomimetic tissue phantoms for neurosurgical near-infrared fluorescence imaging

Neurosurgical fluorescence imaging is a well-established clinical approach with a growing range of indications for use. However, this technology lacks effective phantom-based tools for development, performance testing, and clinician training. Our primary aim was to develop and evaluate 3D-printed phantoms capable of optically and morphologically simulating neurovasculature under fluorescence angiography. Volumetric digital maps of the circle of Willis with basilar and posterior communicator artery aneurysms, along with surrounding cerebral tissue, were generated. Phantoms were fabricated with a stereolithography printer using custom photopolymer composites, then visualized under white light and near-infrared fluorescence imaging. Feature sizes of printed components were found to be within 13% of digital models. Phantoms exhibited realistic optical properties and convincingly recapitulated fluorescence angiography scenes. Methods identified in this study can facilitate the development of realistic phantoms as powerful new tools for fluorescence imaging.

3D modeling↗

Cooperative Education

Los Alamos National Laboratory (LANL) is a multidisciplinary national laboratory that conducts research and development in national security, engineering, materials science, computational modeling, and advanced manufacturing. The laboratory develops innovative technologies to address complex scientific and engineering challenges. This project focuses on the development and evaluation of high-performance absorbing structures through computational design, simulation, and engineering analysis. Absorbing structures are used in applications where damage mitigation, structural protection, and material efficiency are critical performance requirements. The increasing demand for lightweight, high-strength, and highly efficient structural systems has created a need for improved design methodologies capable of maximizing absorption while minimizing weight and material usage. The project utilizes advanced engineering software, including 3D CAD software and FEA, to generate and optimize structural concepts. Computational simulations are performed to evaluate structural behavior under loading conditions, while mathematical analyses are conducted using Python-based tools as well as established analytical equations from material and structural mechanics. The project benefits LANL by supporting the development of advanced design methodologies and improving the understanding of material and structural performance. During the internship term, a significant portion of the design development, simulation, and data analysis activities will be completed. Success of the project depends on collaboration among engineering mentors and technical staff members. Work will be conducted at Los Alamos National Laboratory using laboratory computing resources and engineering software.

42 ENGINEERING↗

MATBOX, an Open-Source Microstructure Analysis Toolbox for Meshing, Generation, Segmentation, and Characterization of 3D Heterogenous Volumes

Battery performance is strongly correlated with electrode microstructural properties. To account for its impact, lithium-ion battery (LIB) models either abstract the microstructural heterogeneity of composite electrodes using effective macroscopic properties (macro- or meso- scale models) or directly solve the system of equations on the microstructure geometry or mesh (microstructure-scale models). Therefore, to be adequate, both families of models require information from the microstructure geometry, which can be provided by the numerical tool presented in this work. MATBOX is a MATLAB open-source application [1] developed by NREL for performing various microstructure-related tasks including microstructure numerical generation, image filtering and microstructure segmentation, microstructure characterization and correlation, visualization, and microstructure meshing. MATBOX was originally developed for the analysis of LIB electrode microstructures; however, the algorithms provided by the toolbox are widely applicable to other heterogeneous materials. The toolbox provides a user-friendly experience thanks to a Graphical-User Interface, requires no coding by the user, and is well documented. This presentation will illustrate various MATBOX features for the characterization of a LIB electrode, including a fully automated Representative Volume Element (RVE) analysis, the numerical generation of complex 'virtual' microstructure, including dual-layer electrodes and carbon-binder additive phase, and the meshing of a complex NMC/graphite full cell microstructure suitable for 3D finite-element modeling. Other modules (segmentation, visualization, and correlation) will be briefly presented. Thanks to its modular, open-source approach, MATBOX can easily incorporate third-party algorithms to eventually build a standard in the field that will benefit the whole scientific community. Effective diffusion coefficient [2], additive phase numerical generation [3], and meshing [4] third-party algorithms have been already integrated in the toolbox with more to come.

DIRECT ENERGY CONVERSION,MATHEMATICS AND COMPUTING↗

3D modeling of deep borehole electromagnetic measurements with energized casing source for fracture mapping at the Utah Frontier Observatory for Research in Geothermal Energy

Here, we present a 3D numerical modelling analysis evaluating the deployment of a borehole electromagnetic measurement tool to detect and image a stimulated zone at the Utah Frontier Observatory for Research in Geothermal Energy geothermal site. As the depth to the geothermal reservoir is several kilometres and the size of the stimulated zone is limited to several 100 m, surface-based controlled-source electromagnetic measurements lack the sensitivity for detecting changes in electrical resistivity caused by the stimulation. To overcome the limitation, the study evaluates the feasibility of using a three-component borehole magnetic receiver system at the Frontier Observatory for Research in Geothermal Energy site. To provide sufficient currents inside and around the enhanced geothermal reservoir, we use an injection well as an energized casing source. To efficiently simulate energizing the injection well in a realistic 3D resistivity model, we introduce a novel modelling workflow that leverages the strengths of both 3D cylindrical-mesh-based electromagnetic modelling code and 3D tetrahedral-mesh-based electromagnetic modelling code. The former is particularly well-suited for modelling hollow cylindrical objects like casings, whereas the latter excels at representing more complex 3D geological structures. In this workflow, our initial step involves computing current densities along a vertical steel-cased well using a 3D cylindrical electromagnetic modelling code. Subsequently, we distribute a series of equivalent current sources along the well's trajectory within a complex 3D resistivity model. We then discretize this model using a tetrahedral mesh and simulate the borehole electromagnetic responses excited by the casing source using a 3D finite-element electromagnetic code. This multi-step approach enables us to simulate 3D casing source electromagnetic responses within a complex 3D resistivity model, without the need for explicit discretization of the well using an excessive number of fine cells. We discuss the applicability and limitations of this proposed workflow within an electromagnetic modelling scenario where an energized well is deviated, such as at the Frontier Observatory for Research in Geothermal Energy site. Using the workflow, we demonstrate that the combined use of the energized casing source and the borehole electromagnetic receiver system offer measurable magnetic field amplitudes and sensitivity to the deep localized stimulated zone. The measurements can also distinguish between parallel-fracture anisotropic reservoirs and isotropic cases, providing valuable insights into the fracture system of the stimulated zone. Besides the magnetic field measurements, vertical electric field measurements in the open well sections are also highly sensitive to the stimulated zone and can be used as additional data for detecting and imaging the target. We can also acquire additional multiple-source data by grounding the surface electrode at various locations and repeating borehole electromagnetic measurements. This approach can increase the number of monitoring data by several factors, providing a more comprehensive dataset for analysing the deep-localized stimulated zone. The numerical analysis indicates that it is feasible to use the combination of the energized casing and downhole electromagnetic measurements in monitoring localized stimulated zone at large depths.

58 GEOSCIENCES↗

HAM: Hotspot-Aware Manager for Improving Communications with 3D-Stacked Memory

merging High-Performance Computing (HPC) workloads, such as graph analytics, machine learning, and big data science, are data-intensive. Data-intensive workloads usually present fine-grained memory accesses with limited or no data locality, and thus incur frequent cache misses and low utilization of memory bandwidth. 3D-stacked memory devices such as Hybrid Memory Cube (HMC) and High Bandwidth Memory (HBM) can provide significantly higher bandwidth than conventional memory modules. However, the traditional interfaces and optimization methods for JEDEC DDR devices do not allow to fully exploit the potential performance of 3D-stacked memory with the massive amount of irregular memory accesses of data-intensive applications. In this paper, we propose a novel Hotspot-Aware Manager (HAM) infrastructure for 3D-stacked memory devices capable of optimizing memory access streams via request aggregation, hotspot detection, and in-memory prefetching. %and an associated hotspot-aware page policy. We present the HAM design and implementation, and simulate it on a system using RISC-V embedded cores with attached HMC devices. We extensively evaluate HAM with over 12 benchmarks and applications representing diverse irregular memory access patterns. The results show that, on average, HAM reduces redundant requests by 37.51\% and increases the prefetch buffer hit rate by 4.2 times, compared to a baseline streaming prefetcher. On the selected benchmark set, HAM provides performance gains of 21.81\% in average (up to 34.28\%) and power savings of 35.07\% over a standard 3D-stacked memory.

Wang, Xi↗

Learning diffractive optical communication around arbitrary opaque occlusions

Abstract Free-space optical communication becomes challenging when an occlusion blocks the light path. Here, we demonstrate a direct communication scheme, passing optical information around a fully opaque, arbitrarily shaped occlusion that partially or entirely occludes the transmitter’s field-of-view. In this scheme, an electronic neural network encoder and a passive, all-optical diffractive network-based decoder are jointly trained using deep learning to transfer the optical information of interest around the opaque occlusion of an arbitrary shape. Following its training, the encoder-decoder pair can communicate any arbitrary optical information around opaque occlusions, where the information decoding occurs at the speed of light propagation through passive light-matter interactions, with resilience against various unknown changes in the occlusion shape and size. We also validate this framework experimentally in the terahertz spectrum using a 3D-printed diffractive decoder. Scalable for operation in any wavelength regime, this scheme could be particularly useful in emerging high data-rate free-space communication systems.

36 MATERIALS SCIENCE↗

Design of metal-mediated protein assemblies via hydroxamic acid functionalities

The self-assembly of proteins into sophisticated multicomponent assemblies is a hallmark of all living systems and has spawned extensive efforts in the construction of novel synthetic protein architectures with emergent functional properties. Protein assemblies in nature are formed via selective association of multiple protein surfaces through intricate noncovalent protein-protein interactions, a challenging task to accurately replicate in the de novo design of multiprotein systems. In this protocol, we describe the application of metal-coordinating hydroxamate (HA) motifs to direct the metal-mediated assembly of polyhedral protein architectures and 3D crystalline protein frameworks (protein-MOFs). This strategy has been implemented using an asymmetric cytochrome cb562 monomer through selective, concurrent association of Fe 3+ and Zn 2+ ions to form polyhedral cages. Furthermore, the use of ditopic HA linkers as bridging ligands with metal-binding protein nodes has allowed the construction of crystalline 3D protein-MOF lattices. The protocol is divided into two major sections: (1) the development of a Cys-reactive HA molecule for protein derivatization and self-assembly of protein-HA conjugates into polyhedral cages and (2) the synthesis of ditopic HA bridging ligands for the construction of ferritin-based protein-MOFs using symmetric metal-binding protein nodes. Furthermore, protein cages can be analyzed using analytical ultracentrifugation (AUC), transmission electron microscopy (TEM) and single-crystal X-ray diffraction (sc-XRD) techniques. HA-mediated protein-MOFs are formed in sitting-drop vapor diffusion crystallization trays and are probed via sc-XRD and multi-crystal small-angle X-ray scattering (SAXS) measurements. Ligand synthesis, construction of HA-mediated assemblies, and post-assembly analysis as described in this protocol can be performed by a graduate-level researcher within six weeks.

36 MATERIALS SCIENCE↗

A WKB based preconditioner for the 1D Helmholtz wave equation

Frequency-domain full-wave solutions to the cold-plasma problem have become ubiquitous in the study of radio frequency power in fusion plasmas. However, recent efforts at extreme levels of geometric fidelity have revealed fundamental limits in the problem size that can be solved by typical sparse direct solver based methods. These limits are of particular importance in the 3D study of RF launchers, where the number of degrees of freedom required can exceed 100 million. In such cases, it would be advantageous to solve the system via iterative means, but due to the large null space of the curl-curl operator, the convergence properties of algorithms like GMRES are poor. Here we present a physics-based preconditioner in the form of a WKB solution and demonstrate the iterative solution to the frequency-domain Helmholtz problem in 1D for several cases ranging from satisfying the WKB approximation to strongly violating it.

Green, David↗

Rotation curves and scaling relations of extremely massive spiral galaxies

We study the kinematics and scaling relations of a sample of 43 giant spiral galaxies that have stellar masses exceeding $10^{11} \, {\rm M}_\odot$ and optical discs up to 80 kpc in radius. We use a hybrid 3D–1D approach to fit 3D kinematic models to long-slit observations of the H α-$\rm{[N\, \small {II}]}$ emission lines and we obtain robust rotation curves of these massive systems. We find that all galaxies in our sample seem to reach a flat part of the rotation curve within the outermost optical radius. We use the derived kinematics to study the high-mass end of the two most important scaling relations for spiral galaxies: the stellar/baryonic mass Tully–Fisher relation and the Fall (mass-angular momentum) relation. All galaxies in our sample, with the possible exception of the two fastest rotators, lie comfortably on both these scaling relations determined at lower masses, without any evident break or bend at the high-mass regime. When we combine our high-mass sample with low-mass data from the Spitzer Photometry & Accurate Rotation Curves catalogue, we find a slope of α = 4.25 ± 0.19 for the stellar Tully–Fisher relation and a slope of γ = 0.64 ± 0.11 for the Fall relation. Our results indicate that most, if not all, of these rare, giant spiral galaxies are scaled up versions of less massive discs and that spiral galaxies are a self-similar population of objects up to the very high-mass end.

79 ASTRONOMY AND ASTROPHYSICS↗

Improved Gamma-Ray Point Source Quantification in Three Dimensions by Modeling Attenuation in the Scene

We discuss using a series of detector measurements taken at different locations to localize a source of radiation as a well-studied problem. The source of radiation is sometimes constrained to a single point-like source, in which case the location of the point source can be found using techniques such as maximum likelihood. Recent advancements have shown the ability to locate point sources in 2D and even 3D, but few have studied the effect of intervening material on the problem. In this work we examine gamma-ray data taken from a freely moving system and develop voxelized 3-D models of the scene using data from the onboard LiDAR. Ray casting is used to compute the distance each gamma ray travels through the scene material, which is then used to calculate attenuation assuming a single attenuation coefficient for solids within the geometry. Parameter estimation using maximum likelihood is performed to simultaneously find the attenuation coefficient, source activity, and source position that best match the data. Using a simulation, we validate the ability of this method to reconstruct the true location and activity of a source, along with the true attenuation coefficient of the structure it is inside, and then we apply the method to measured data with sources and find good agreement.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Accelerating Large-Format Metal Additive Manufacturing: How Controls R&D is Driving Speed, Scale, and Efficiency

This article highlights work at Oak Ridge National Laboratory’s Manufacturing Demonstration Facility to develop closed-loop, feedback control for laser-wire based Directed Energy Deposition, a form of metal Big Area Additive Manufacturing (m-BAAM), a process being developed in partnership with GKN Aerospace specifically for the production of Ti-6Al-4V pre-forms for aerospace components. A large-scale structural demonstrator component is presented as a case-study in which not just control, but the entire 3D printing workflow for m-BAAM is discussed in detail, including design principles for large-format metal AM, toolpath generation, parameter development, process control, and system operation, as well as post-print net-shape geometric analysis and finish machining. In terms of control, a multi-sensor approach has been utilized to measure both layer height and melt pool size, and multiple modes of closed-loop control have been developed to manipulate process parameters (laser power, print speed, deposition rate) to control these variables. Layer height control and melt pool size control have yielded excellent local (intralayer) and global (component-level) geometry control, and the impact of melt pool size control in particular on thermal gradients and material properties is the subject of continuing research. Further, these modes of control have allowed the process to advance to higher deposition rates (exceeding 7.5 lb/hr), larger parts (1-meter scale), shorter build times, and higher overall efficiency. The control modes are examined individually, highlighting their development, demonstration, and lessons learned, and it is shown how they operate concurrently to enable the printing of a large-scale, near net shape Ti-6Al-4V component.

Gibson, Brian↗

Disorder, interactions, and their interplay in novel narrow-gap Dirac materials and Weyl semimetals

Progress of the modern day condensed matter physics is to a large extent driven by the synthesis of new materials, advances in their experimental characterization and theoretical description. Recent discoveries of novel gapless Weyl semimetals, such as NaBi,CdAs, and BiTe-based films, in which magnetic dopants essentially suppress the gap, have added to the family of graphene and topological insulators actively investigated over the past decade. With the field of novel semimetals rapidly maturing, its focus necessarily shifts from demonstrations of the feasibility of such materials to their quantitative characterization. While the transport and optical properties of graphene and topological insulators are well captured within the picture of free non-interacting electrons, gapless 3D Weyl semimetals and narrow-gap 2D semiconductors with Dirac spectrum are known to be extremely susceptible to disorder and electron-electron interactions. This susceptibility obscures the manifestations of nontrivial band structure -- like quantum anomalous Hall effect -- of the new topological materials. Among particular projects to be addressed are: 1) optical conductivity of 3D gapless Dirac fermions in the presence of smooth disorder, 2) interplay of disorder and Coulomb interactions in the spectral properties of such fermions, 3) formation and structure of the impurity band with Coulomb supercritical clusters, 4) Coulomb interaction-driven renormalization of the electron spectrum and of the transport response in the presence of strong magnetic field, 5) instanton approach to the disorder-induced fluctuation states in zero-gap 3D materials, and 6) the role of disorder in quantum anomalous Hall effect. The proposal relies upon the investigators' previous broad expertise in interacting and disordered electron systems. The methods to be employed include perturbative diagrammatic technique, non-perturbative instanton and self-consistent approximations, hydrodynamics of electron liquid. Both analytical as well as numerical approaches are to be employed. The anticipated broader outcome of the proposal includes gaining an in-depth understanding of the interplay of the disorder and interactions under the conditions when this interplay has the most dramatic impact on observables. Traditionally, interaction effects are among the most challenging and interesting problems of condensed matter physics. Similarly, disordered systems typically present very difficult but extremely rich problems in the description of various materials. Importantly, understanding the spectral and transport properties of such materials not only presents the fundamental objective, but is also of particular interest for many applications, such as computation, memory, optics, plasmonics. In particular realization of the quantum anomalous Hall effect may lead to the development of low-power-consumption electronics. Indeed, a major constraint for practical use of the quantum Hall effect is limited by the requirement of the quantizing magnetic field. At the same time, the quantum anomalous Hall effect samples exhibit non-dissipative edge quantum transport in a zero magnetic field.

36 MATERIALS SCIENCE↗

Temperature Controlled Glass Additive Manufacturing

Glass additive manufacturing (AM) is an emerging technology with a wide range of applications in chemistry, biology, optical science, and engineering. A custom laser-based glass 3D printer was developed by a group of engineers at Los Alamos National Laboratory (LANL) and is being optimized to produce hardware for chemical processing equipment, microfluidic systems, as well as optical elements. AM glass using a filament deposition modeling (FDM) approach allows for generation of parts with high optical quality. The quality of the glass can be affected by the generation of defects such as bubbles and vaporization which affect the optical quality of the glass. The defects can also affect the mechanical performance of the glass and lead to sample cracking.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flexible Fuel Electric Hybrid Glass Furnace Demonstration

The furnace contractor completed General Arrangement (GA) layouts and Piping and Instrumentation Diagrams (P&ID) for both furnaces during this reporting period. Preliminary equipment lists accompanied this work. Control system architecture in progress. Key furnace design elements and deliverables on track to be complete by end of phase. The facilities design and integration contractor completed a 3D scan and modeling of the facility. The work during this period focused on preliminary design with a focus on overall project scope and feasibility. This key work supports the overall project deliverables for 30% preliminary engineering and Preliminary Design Report (PDR) which are on track to be complete by the end of the phase. These deliverables are approximately 50% complete through the end of this reporting period. The batch house operations design contractor continues development of site plan and General Arrangement (GA) layout to support the 30% preliminary engineering and design package. This work is 60% complete by the end of this reporting period and is on track to be complete by the end of the phase.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Carbonate Management to Enable Energy- and Carbon-Efficient CO 2 Electrolysis (Final Technical Report)

The rapid growth and plummeting cost of solar energy have spurred growing interest in using CO 2 electrolysis to produce chemicals and fuels as an alternative to conventional petrochemical processes. High-temperature (>800 °C) solid oxide electrolyzers that convert CO 2 into CO and O 2 have recently become commercially available. Low-temperature electrolysis cells offer the prospect of more convenient and flexible operation, which is critical for utilizing intermittent solar energy, and provide access to more valuable C 2+ products such as ethylene, ethanol, and propanol. Over the past 10 years, research in this area has yielded substantial progress in both fundamental understanding of the requisite electrocatalytic reactions and design of prototype devices. Leveraging insights from fuel cells and membrane water electrolyzers, researchers have developed electrolysis cells with gas diffusion electrodes (GDE) that have demonstrated high CO 2 electrolysis current densities (>100 mA cm –2 ) as well as promising selectivity and stability. Despite these advances, the energy efficiency (electrical energy-to-product) and carbon efficiency (CO 2 -to-product) of low-temperature CO 2 electrolysis remain far too low for large-scale deployment. A preponderance of evidence indicates that the principal source of efficiency losses is the rapid and thermodynamically favorable reaction of CO 2 with hydroxide (OH – ) to form carbonate (CO 3 2– ). Carbonate formation imposes steady-state electrolysis conditions that result in large voltage and CO 2 losses for all known (photo)electrochemical CO 2 cells. While much current research remains focused on CO 2 reduction catalyst design, this largely overlooked CO 3 2– problem presents a fundamental scientific barrier to creating a viable electrochemical option for converting solar energy into chemicals and fuels. The project pursues an integrated, multi-PI research effort that establishes a fundamental science of CO 3 2– management. PI Kanan and Co-PI Mani’s contribution to the project is to evaluate strategies to mitigate the CO 3 2– problem by changing the properties of the electrolyte and the environment in which CO 2 reduction catalysis takes place. Experimental studies showed that electrolytes composed of a high concentration of both CO 3 2– and HCO 3 – , which serve as moderately alkaline buffers, improved the cell voltage by compared to all-HCO 3 – electrolytes, but these buffered systems still show substantial CO 2 uptake that reduces pH over time. Computational studies developed a homogenized model of a CO 2 reduction catalyst layer that permits a low-cost exploration of the high-dimensional parameter space associated with catalyst layers on gas diffusion electrodes. The model was validated by accurately reproducing experimental data for the related but simpler reaction of CO reduction and then used to probe the effects of catalyst layer architecture on CO 2 reduction. Minimizing the size of catalyst and hydrophobic domains in the catalyst layer is predicted to mitigate CO 3 2– formation and thereby enable prolonged operation at elevated pH. In support of the CO 2 electrolysis studies, a new method for rapidly prototyping electrochemical cells was developed and validated. The method uses a combination of 3D printing and electroless plating to generate conductive cell components for evaluating new cell designs. The carbonate problem encompasses mass transport processes and acid-base reactions that are relevant to many other electrochemical systems. Investigation of strategies to address the carbonate problem led to an additional line of inquiry into the physicochemical phenomena that determine the efficiency of electrochemical acid-base production, which has numerous applications in the broader field of carbon management. New strategies for using the supporting electrolyte to inhibit H + /OH – recombination in electrochemical acid-base production were evaluated, leading to the development of a novel acid-base producing system that eliminates the need for ion exchange membranes and exhibits promising efficiency and current densities for scalable applications.

25 ENERGY STORAGE↗

Interpenetrated Structures for Enhancing Ion Diffusion Kinetics in Electrochemical Energy Storage Devices

The architectural design of electrodes offers new opportunities for next-generation electrochemical energy storage devices (EESDs) by increasing surface area, thickness, and active materials mass loading while maintaining good ion diffusion through optimized electrode tortuosity. However, conventional thick electrodes increase ion diffusion length and cause larger ion concentration gradients, limiting reaction kinetics. We demonstrate a strategy for building interpenetrated structures that shortens ion diffusion length and reduces ion concentration inhomogeneity. This free-standing device structure also avoids short-circuiting without needing a separator. The feature size and number of interpenetrated units can be adjusted during printing to balance surface area and ion diffusion. Starting with a 3D-printed interpenetrated polymer substrate, we metallize it to make it conductive. This substrate has two individually addressable electrodes, allowing selective electrodeposition of energy storage materials. Using a Zn//MnO 2 battery as a model system, the interpenetrated device outperforms conventional separate electrode configurations, improving volumetric energy density by 221% and exhibiting a higher capacity retention rate of 49% compared to 35% at temperatures from 20 to 0 °C. Our study introduces a new EESD architecture applicable to Li-ion, Na-ion batteries, supercapacitors, etc.

25 ENERGY STORAGE↗