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At least 397 records · Page 22

X-ray fluorescence mapping: Insights into mesoscale structure impact on battery functional electrochemistry

Abstract Electron transfer and ion transport occurs over multiple-length scales ranging from the atomic to mesoscale within battery materials and electrodes. Micro-X-ray fluorescence (µ-XRF) is an important characterization tool as it can resolve structural, compositional, and redox information while providing insight into the spatial distribution of an electroactive material. In this work, µ-XRF mapping is used to probe the distribution of iron within thin planar slurry-based and thick porous carbon nanotube (CNT)-based magnetite (Fe 3 O 4 ) electrodes. Notably, the porous CNT-based electrode showed homogenous distribution of Fe within the electrode whereas the planar electrode demonstrated distinct Fe aggregates. This information was used to rationalize the electrochemistry observed by cyclic voltammetry and galvanostatic cycling. The thick porous electrode delivered 215% more capacity per gram of magnetite during the first discharge, consistent with increased electrode homogeneity enabling effective ion access and electron transfer. Graphical Abstract

Sadique, Nahian↗

The Science and Engineering of Durable Ultralow PGM Catalysts (2012 DOE-EERE-FCT Annual Progress Report)

Minimizing the quantity of Pt group metals used in polymer membrane fuel cells (PEMFCs) is one of the remaining grand challenges for fuel cell commercialization. Tremendous progress has been achieved over the last two decades in decreasing the Pt loading required for efficient fuel cell performance. Unfortunately, the fluctuations in the price of Pt represent a substantial barrier to the economics of widespread fuel cell use. Durability and impurity tolerance are also challenges that are tightly coupled to fuel cell Pt electrode loading. Traditional approaches to decreasing the amount of Pt required for good performance include: (1) Increasing mass activity by decreasing Pt particle size by supporting on carbon; (2) Alloy formulation Pt-Co, Pt-Cr alloys to improve mass activity; (3) Increasing Pt utilization by optimization of electronic and ionic contact of the Pt particles; (4) Improving conductivity of the electronic and ionic conducting constituents of the membrane electrode assembly; and (5) Improving reactant to and product mass transport away from the electroactive sites. Recent novel approaches include the nanoengineering of core shell catalysts and Pt particles of unusual geometries such as nanowires/whiskers. The success of the aforementioned approaches has been great; however further advances using such approaches have been hampered by a lack of underlining scientific understanding of the catalyst activity, particle growth mechanisms, and optimization strategies for designing composite electrodes The objectives of this report are: (1) Development of durable, high mass activity Platinum Group Metal (PGM) cathode catalysts-enabling lower cost fuel cells; (2) Elucidation of the fundamental relationships between PGM catalyst shape, particle size and activity to help design better catalysts; (3) Optimization of the cathode electrode layer to maximize the performance of PGM catalysts-improving fuel cell performance and lowering cost; (4) Understanding the performance degradation mechanisms of high mass activity cathode catalysts-provide insights to better catalyst design; and (5) Development and testing of fuel cells using ultra-low loading high activity PGM catalysts-validation of advanced concepts.

08 HYDROGEN↗

Exploring Charge Transport in Guest Molecule Infiltrated Cu 3 (BTC) 2 Metal Organic Framework

The goal of this Exploratory Express project was to expand the understanding of the physical properties of our recently discovered class of materials consisting of metal-organic frameworks with electroactive ‘guest’ molecules that together form an electrically conducting charge-transfer complex (molecule@MOF). Thin films of Cu 3 (BTC) 2 were grown on fused silica using solution step-by-step growth and were infiltrated with the molecule tetracyanoquinodimethane (TCNQ). The infiltrated MOF films were extensively characterized using optical microscopy, scanning electron microscopy, Raman spectroscopy, electrical conductivity, and thermoelectric properties. Thermopower measurements on TCNQ@Cu 3 (BTC) 2 revealed a positive Seebeck coefficient of ~400 μV/k, indicating that holes are the primary carriers in this material. The high value of the Seebeck coefficient and the expected low thermal conductivity suggest that molecule@MOF materials may be attractive for thermoelectric power conversion applications requiring low cost, solution-processable, and non-toxic active materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Organic Synthetic Advanced Materials for Optoelectronic and Energy Applications (at National Taipei University of Technology)

These slides cover Hung-Ju Yen's recent work in the synthesis and structural design of functional materials, which were further used for optoelectronic and energy applications, such as lithium ion battery, solar cell, LED, electrochromic, and fuel cells. This was for a job interview at National Taipei University of Technology. The following topics are detailed: current challenges for lithium-ion batteries; graphene, graphene oxide and nanographene; nanographenes with various functional groups; fine tune d-spacing through organic synthesis: varying functional group; schematic view of LIBs; nanographenes as LIB anode; rate performance (charging-discharging); electrochromic technology; electrochromic materials; advantages of triphenylamine; requirement of electrochromic materials for practical applications; low driving voltage and long cycle life; increasing the electroactive sites by multi-step synthetic procedures; synthetic route to starburst triarylamine-based polyamide; electrochromism ranging from visible to NIR region; transmissive to black electrochromism; RGB and CMY electrochromism.

36 MATERIALS SCIENCE↗

Organic Synthetic Advanced Materials for Optoelectronic and Energy Applications (at National Sun Yat-sen University)

These slides cover Hung-Ju Yen's recent work in the synthesis and structural design of functional materials, which were further used for optoelectronic and energy applications, such as lithium ion battery, solar cell, LED, electrochromic, and fuel cells. This was for a job interview at National Sun Yat-sen University. The following topics are detailed: current challenges for lithium-ion batteries; graphene, graphene oxide and nanographene; nanographenes with various functional groups; fine tune d-spacing through organic synthesis: varying functional group; schematic view of LIBs; nanographenes as LIB anode; rate performance (charging-discharging); electrochromic technology; electrochromic materials; advantages of triphenylamine; requirement of electrochromic materials for practical applications; low driving voltage and long cycle life; increasing the electroactive sites by multi-step synthetic procedures; synthetic route to starburst triarylamine-based polyamide; electrochromism ranging from visible to NIR region; transmissive to black electrochromism; RGB and CMY electrochromism.

36 MATERIALS SCIENCE↗

Organic Synthetic Advanced Materials for Optoelectronic and Energy Applications (at Center for Condensed Matter Sciences)

These slides cover Hung-Ju Yen's recent work in the synthesis and structural design of functional materials, which were further used for optoelectronic and energy applications, such as lithium ion battery, solar cell, LED, electrochromic, and fuel cells. This was for a job interview at Center for Condensed Matter Sciences. The following topics are detailed: current challenges for lithium-ion batteries; graphene, graphene oxide and nanographene; nanographenes with various functional groups; fine tune d-spacing through organic synthesis: varying functional group; schematic view of LIBs; nanographenes as LIB anode; rate performance (charging-discharging); electrochromic technology; electrochromic materials; advantages of triphenylamine; requirement of electrochromic materials for practical applications; low driving voltage and long cycle life; increasing the electroactive sites by multi-step synthetic procedures; synthetic route to starburst triarylamine-based polyamide; electrochromism ranging from visible to NIR region; transmissive to black electrochromism; RGB and CMY electrochromism.

36 MATERIALS SCIENCE↗

Development of an All-Aqueous Thermally Regenerative Redox Flow Battery to Support Fossil Fuel Assets

Low-temperature thermal energy, a largely untapped resource, holds significant promise for large-scale electrical power generation globally. Various stationary sources, including industrial entities and thermal power plants, emit considerable low-temperature heat that currently remains unutilized. This energy is often overlooked because its low temperature renders it unsuitable for efficient power generation using conventional methods. However, current research is exploring diverse technologies capable of converting low-temperature heat into grid-scale power, aiming to enhance grid efficiency, further decarbonization initiatives, and facilitate a shift toward more decentralized power systems. One such innovative technology is the thermally regenerative battery (TRB), noted for its high power and energy densities compared to similar technologies, positioning it as a potential game-changer in power generation. TRBs integrate two scalable and well-established unit operations: a redox flow battery and a distillation column. This integration suggests that once an effective TRB chemistry is established, the pathway to commercialization could be expedited. The copper-based thermally regenerative ammonia battery (Cu aq -TRAB) stands out as the first TRB that circumvents electrodeposition/dissolution reactions, stabilizing Cu(I) and Cu(II) within the electrolyte and maintaining stability of all electroactive species in an aqueous phase. This stabilization has led to improvements in coulombic efficiency, open circuit potential, and copper solubility, thereby enhancing power density, energy density, and overall energy efficiency. Preliminary tests were conducted to determine the effects of various electrolyte species on the performance metrics of the battery, both theoretically and experimentally. These tests revealed that the solubility of copper in the Cu aq -TRAB electrolyte was constrained by the Cu(I)-NH 3 complex. Adjusting the background electrolyte to 5 M NH4Br and the ligand concentration to 4 M NH 3 enabled the copper concentration to reach a maximum of 0.6 M. This modification led to an estimated theoretical maximum energy density of 9.5 Wh L -1 for the Cu aq -TRAB. Additionally, full cell testing indicated a tradeoff between peak power and energy density with varying copper and ammonia concentrations. Increasing the applied current density during discharge linearly raised the average power output, with a minimal reduction in energy density due to a balance between higher ohmic overpotential and reduced time for undesirable ammonia crossover. Furthermore, a comprehensive numerical sensitivity analysis of the complete Cu aq -TRAB system was performed. This analysis aimed to assess how the battery and the distillation column responded to changes in system input parameters, providing insights into optimal research directions for enhancing system performance. The analysis revealed that at room temperature, battery power was significantly more sensitive to ohmic losses than to mass transfer, with reaction rates having minimal impact. This trend continued even at higher temperatures. Also, the thermal energy required for ammonia separation was studied, showing that increased temperatures generally reduced energy requirements, except in low-pressure scenarios above 65 °C. An investigation into membrane performance in the Cu aq -TRAB was undertaken, given the significant impact of ammonia transport control and ohmic losses on system performance. Various membranes were evaluated to identify key performance metrics. Among the tested membranes, Selemion CMVN exhibited the highest performance, with a peak power density of 84 mW cm -2 and average values of 26 ± 6.8 mW cm -2 for power density and 2.9 Wh L -1 for energy density at an applied current density of 50 mA cm -2 . An economic assessment indicated a levelized cost of storage at $410 per MWh under optimal conditions, highlighting the commercial potential of the Cu aq -TRAB when utilizing cost-effective, readily available materials.

25 ENERGY STORAGE↗

Redox-Hopping-Based Charge Transport Mediated by Ru(II)-Polypyridyl Species Immobilized in a Mesoporous Metal-Organic Framework

Electronic charge transport through crystalline metal-organic frameworks (MOFs) can be accomplished by site-to-site electron (or hole) hopping, provided that redox-active sites, such as easily reducible or oxidizable MOF linkers, are present. If the framework itself is redox-inert, solvent-assisted ligand incorporation of redox-active moieties can serve to enable hopping-based charge transport. Here we have studied the redox hopping process within Ru-bpy@NU-1008, where Ru-bpy is a carboxylate-functionalized derivative, i . e ., a node-ligating derivative, of the well-known chromophore Ru(2,2′-bipyridine) 3 2+ , and NU-1008 is a redox-inert MOF featuring hierarchical porosity and csq topology. Chronoamperometry experiments with electrode-supported thin films of Ru-bpy@NU-1008 show that charge transport is feasible through portions of the MOF, with other portions being inaccessible. Possible confounding features are the undersized c- pores that cross-connect 1D mesoporous channels, as ingress and egress of charge-compensating anions is believed to accompany the net oxidation of Ru(II) to Ru(III) and the reduction of Ru(III) to Ru(II). Phenomenologically, transport through the electroactive portion of the films is diffusion-like, with the magnitude of the apparent diffusion coefficient being 6 × 10 −12 cm 2 /s.

Duan, Jiaxin↗

Extracellular electron uptake from a cathode by the lactic acid bacterium Lactiplantibacillus plantarum

A subset of microorganisms that perform respiration can endogenously utilize insoluble electron donors, such as Fe(II) or a cathode, in a process called extracellular electron transfer (EET). However, it is unknown whether similar endogenous EET can be performed by primarily fermentative species like lactic acid bacteria. We report for the first time electron uptake from a cathode by Lactiplantibacillus plantarum, a primarily fermentative bacteria found in the gut of mammals and in fermented foods. L. plantarum consumed electrons from a cathode and coupled this oxidation to the reduction of both an endogenous organic (pyruvate) and an exogenous inorganic electron acceptor (nitrate). This electron uptake from a cathode reroutes glucose fermentation toward lactate degradation and provides cells with a higher viability upon sugar exhaustion. Moreover, the associated genes and cofactors indicate that this activity is mechanistically different from that one employed by lactic acid bacteria to reduce an anode and to perform respiration. Our results expand our knowledge of the diversity of electroactive species and of the metabolic and bioenergetic strategies used by lactic acid bacteria.

biocathode↗

2D Graphene Sheets as a Sensing Material for the Electroanalysis of Zileuton

Zileuton (ZLT) is an active oral inhibitor of enzyme 5-lipoxygenase, and long-term intake and overdose of ZLT cause adverse effects, leading to critical conditions in patients. This is a well-recognized issue that necessitates a better approach for ZLT sensing. Given the increasing interest in ZLT sensing and the limitations of previous techniques, there is a need for a highly sensitive, robust, and fast operation method that is inexpensive and easy to use. Thus, for the sensitive detection and determination of ZLT, an electrochemical sensor based on graphene was fabricated. Graphene has excellent properties, such as high surface area, low toxicity, conductivity, and electroactive conjugation with biomolecules, making it suitable for sensing. The electrocatalytic property of graphene promotes the redox-coupled reaction of ZLT. Electrochemical investigation of the modifier was carried out by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). An optimization and analysis of the influence of different parameters on the electrochemical behavior of ZLT were carried out using the CV approach. The scan rate study aided in exploring the physicochemical properties of the electrode process, and two electrons with two protons were found to be involved in the electrooxidation of ZLT. The fabricated sensor showed a wide range of linearity with ZLT, from 0.3 µM to 100.0 µM, and the detection limit was evaluated as 0.03 µM under optimized conditions. The analysis of spiked urine samples, with good recovery values for percent RSD, provided support for the efficiency and applicability of the developed electrode.

2D Material↗

Direct Measurement of Crossover and Interfacial Resistance of Ion-Exchange Membranes in All-Vanadium Redox Flow Batteries

Among various components commonly used in redox flow batteries (RFBs), the separator plays a significant role, influencing resistance to current as well as capacity decay via unintended crossover. It is well-established that the ohmic overpotential is dominated by the membrane and interfacial resistance in most aqueous RFBs. The ultimate goal of engineering membranes is to improve the ionic conductivity while keeping crossover at a minimum. One of the major issues yet to be addressed is the contribution of interfacial phenomena in the influence of ionic and water transport through the membrane. In this work, we have utilized a novel experimental system capable of measuring the ionic crossover in real-time to quantify the permeability of ionic species. Specifically, we have focused on quantifying the contributions from the interfacial resistance to ionic crossover. The trade-off between the mass and ionic transport impedance caused by the interface of the membranes has been addressed. The MacMullin number has been quantified for a series of electrolyte configurations and a correlation between the ionic conductivity of the contacting electrolyte and the Nafion® membrane has been established. The performance of individual ion-exchange membranes along with a stack of various separators have been explored. We have found that utilizing a stack of membranes is significantly beneficial in reducing the electroactive species crossover in redox flow batteries compared to a single membrane of the same fold thickness. For example, we have demonstrated that the utilization of five layers of Nafion ® 211 membrane reduces the crossover by 37% while only increasing the area-specific resistance (ASR) by 15% compared to a single layer Nafion ® 115 membrane. Therefore, the influence of interfacial impedance in reducing the vanadium ion crossover is substantially higher compared to a corresponding increase in ASR, indicating that mass and ohmic interfacial resistances are dissimilar. We have expanded our analysis to a combination of commercially available ion-exchange membranes and provided a design chart for membrane selection based on the application of interest (short duration/high-performance vs. long-term durability). The results of this study provide a deeper insight into the optimization of all-vanadium redox flow batteries (VRFBs).

UV/Vis spectroscopy↗

Applying Dynamic Strain on Thin Oxide Films Immobilized on a Pseudoelastic Nickel-Titanium Alloy

Direct alteration of materials structure/function through strain is a burgeoning area of research that has allowed for novel properties of materials to emerge. Tuning materials structure can be achieved by controlling an external force imposed on materials and inducing stress-strain responses (i.e., applying dynamic strain). Electroactive thin films are typically deposited on shape or volume tunable elastic substrates, where mechanical loading (i.e. compression or tension) can affect films structure and function through imposed strain. Here we summarize methods for straining n-type doped titanium dioxide (TiO2) films prepared by a thermal treatment of a pseudo-elastic nickel-titanium alloy. The main purpose of the described methods is to study how strain affects electrocatalytic activities of metal oxide, specifically hydrogen evolution and oxygen evolution reactions. The same system can be adapted to study the effect of strain more broadly. Strain engineering can be applied for optimization of a material function, as well as for design of adjustable, multifunctional (photo)electrocatalytic materials under external stress control.

92 SC - Basic Energy Sciences (BES) (SC-22)↗

Photoelectrochemical electrodes

The surface of a moderate band gap semiconductor such as p-type molybdenum sulfide is modified to contain an adherent film of charge mediating ionene polymer containing an electroactive unit such as bipyridimium. Electron transport between the electrode and the mediator film is favorable and photocorrosion and recombination processes are suppressed. Incorporation of particles of catalyst such as platinum within the film provides a reduction in overvoltage. The polymer film is readily deposited on the electrode surface and can be rendered stable by ionic or addition crosslinking. Catalyst can be predispersed in the polymer film or a salt can be impregnated into the film and reduced therein.

Williams, R. M.↗

A lithium oxygen secondary battery

Some recent work on a lithium-oxygen secondary battery is reported in which stabilized zirconia oxygen vacancy conducting solid electrolytes were used for the effective separation of respective half-cell reactions. The electroactive material consisted of alloys possessing the general composition Li(x)FeSi2 immersed in a ternary molten salt comprising LiF, LiCl, and Li2O. The manufacture of the cell is described, and discharge-current voltage curves for partially charged cells are shown and discussed. A galvanostatic IR free-changing curve and an IR-free charge-discharge curve are also shown.

Semkow, Krystyna W.↗

New secondary batteries utilizing electronically conductive polymer cathodes

The objectives of this project are to optimize the transport rates in electronically conductive polypyrrole films by controlling the morphology of the film and to assess the utility of these films as cathodes in a lithium/polypyrrole secondary battery. During this research period, progress has been made in improving the charge transport rate of the supermolecular-engineered polypyrrole electrode by eliminating the polypyrrole baselayer that hampered earlier work. Also, the fibril density of the polypyrrole electrode was increased, providing more electroactive sites per unit area.

Martin, Charles R.↗

Nonlinear optical properties of organic materials: A theoretical study

Replacement of electronic switching circuits in computing and telecommunication systems with purely optical devices offers the potential for extremely high throughput and compact information processing systems. The potential application of organic materials containing molecules with large nonresonant nonlinear effects in this area have triggered intensive research during the last decade. Interest on this area was due to two facts: (1) that many organic materials show nonlinearities that are orders of magnitude larger than those of conventional inorganic materials such as lithium niobate and potassium dihydrogen phosphate; and (2) that organic materials show much flexibility in terms of molecular designs. Some of the desirable characteristics that these materials should have are that they be transparent to the frequency of the incident laser and its second or third harmonic, that they have a high damage threshold, and, in the case of second-order effects, that their crystal structure or molecular orientation be accentric. Since polymeric assemblages can enhance the nonlinear response of organic molecules severalfold, efforts have been directed toward the synthesis of thin films with interpenetrating lattices of electroactive molecules. The goal of this theoretical investigation is to predict the magnitude of the molecular polarizabilities of organic molecules that could be incorporated into films. These calculations are intended to become a powerful tool to assist material scientists in screening for the best candidates for optical applications. The procedure that was developed for the present calculations is based on the static-field approach, and is a modification to the method developed by Dewar and Stewart, 1984 for calculating molecular linear polarizabilities.

Cardelino, Beatriz H.↗

A coated-wire ion-selective electrode for ionic calcium measurements

A coated-wire ion-selective electrode for measuring ionic calcium was developed, in collaboration with Teknektron Sensor Development Corporation (TSDC). This coated wire electrode sensor makes use of advanced, ion-responsive polyvinyl chloride (PVC) membrane technology, whereby the electroactive agent is incorporated into a polymeric film. The technology greatly simplifies conventional ion-selective electrode measurement technology, and is envisioned to be used for real-time measurement of physiological and environment ionic constituents, initially calcium. A primary target biomedical application is the real-time measurement of urinary and blood calcium changes during extended exposure to microgravity, during prolonged hospital or fracture immobilization, and for osteoporosis research. Potential advanced life support applications include monitoring of calcium and other ions, heavy metals, and related parameters in closed-loop water processing and management systems. This technology provides a much simplified ionic calcium measurement capability, suitable for both automated in-vitro, in-vivo, and in-situ measurement applications, which should be of great interest to the medical, scientific, chemical, and space life sciences communities.

Hines, John W.↗

Measurements of the fundamental thermodynamic parameters of Li/BCX and Li/SOCl2 cells

Two experimental techniques - equilibrium or reversible cell discharge and measurement of open circuit potential as a function of temperature - are used to determine the thermodynamic data needed to estimate the heat generation characteristics of Li/BCX and Li/SOCl2 cells. The results obtained showed that the reversible cell potential, the temperature dependence of the reversible cell potential, and the thermoneutral potential of the BCX cell were 3.74 V, -0.857 +/- 0.198 mV/K, and 3.994 +/- 0.0603 V, respectively. The respective values obtained for the Li/SOCl2 cell were 3.67 V, -0.776 +/- 0.255 mV/K, and 3.893 +/- 0.0776 V. The difference between the thermoneutral potential of Li/BCX and Li/SCl2 cells is attributable to the difference in their electroactive components.

Kalu, E. E.↗