bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Digital Presentation) Sol-Gel Based Synthesis Route for High Capacity Disordered Rocksalt (DRX) Oxyfluoride Cathodes
Authors: Patil Shripad , Self Ethan , Nanda Jagjit 
Published: July 2022

The cost and energy density of commercial Li-ion batteries (LIBs) are largely limited by the cathode. Currently, the LIB cathode market is dominated by intercalation type layered transition metal oxides of the general form LiNixMnyCo1-x-yO2 (NMC). As the LIB market continues to grow, there is an increasing risk of over-reliance on cobalt and nickel, which not only leads to increased cost and resource depletion, but also raises ethical concerns related to the cobalt mining industry. Hence, there is an urgent need to develop new cathodes based on earth abundant materials.
Disordered rocksalt (DRX) oxides and oxyfluorides have emerged as a promising candidate for next generation LIB cathodes due to their high energy density and ability to utilize low-cost, earth abundant elements such as Mn and Ti. Studies have shown that anionic substitution of oxygen with fluorine enhances electrochemical performance and cycling stability of DRX cathodes. DRX cathodes are traditionally synthesized using high temperature solid-state and high energy mechanochemical routes. While these methods have yielded promising cathodes, they face challenges with fluorine substitution and process scalability. Keeping this in mind, the goal of this research is to develop alternate synthesis routes to prepare DRX oxyfluoride cathodes and identify key structure – property correlations to optimize cathode performance. Our team recently developed a sol-gel based approach to synthesize Li1.2MnxTi0.8-xO2-yFy (y=0-0.2; x=0.4-0.6) DRX oxides and oxyfluorides. This presentation will discuss recent development related to the synthesis, structure, and performance of these cathodes

Acknowledgements

This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) through the Vehicle Technologies Office (VTO).
A Thermo-Electrochemical Model for Simulating Internal Short Circuits in a Li-Ion Battery Depending on Lithium Dendrites
Authors: Kim Suhwan , Song Jihun , Lee Hyobin , Jung Seungwon , Park Joonam , Lee Yong Min 
Published: July 2022

An internal short circuit (ISC) is known to be the main cause of fatal accidents in Li-ion batteries (LIBs). If two electrodes come into contact with each other because of any event, the inner temperature of LIBs increases rapidly within the very short time. If the temperature can increase over the threshold temperature, fire or explosion accidents can occur in the LIB, which is called thermal runaway (TR). Because the fire in the LIBs is not easily extinguished and can cause significant damage of life and property, we should understand the fundamental electrochemical and thermal behavior of ISC-TR in order to prevent or delay these severe accidents. For this purpose, there have been tremendous attempts to analyze different ISC cases with a variety of LIB cells experimentally through penetrating nails, pucks, shape memory alloys, etc. However, experimental methods have limitations in measuring internal temperatures and estimating current density and lithium-ion concentration within LIB cells. Also it is still challenging to control the types and locations of ISCs practically. To compensate these experimental limitations, many simulation studies have also been conducted. However, many simulation research have been considering a two-dimensional-based microscale domain, which may have relatively inaccurate simulation results or cannot consider three-dimensional placement, or a three-dimensional-based large domain, which calculates ISC only in mm units or more.
In this work, we developed an advanced thermo-electrical model to simulate the responses of LIB cells depending on the sizes, numbers, and locations of lithium dendrites or impurities. This model can calculate the current density, which causes joule heat flux, and simulate heat transfer. Thus, this model can provide us with information on what kinds or how many of lithium dendrites will lead to thermal runaway. Also, it is possible to analyze the thermal behavior of LIBs according to the various physical and temperature conditions of the lithium dendrites.
Atomistic Scale Analysis of Motion and Dynamics of Li-Ion in Li-Zn-Zr-S Compound Electrolyte
Authors: Kwon Eunji , Lim Hyun-kyu , Lee Sangheon 
Published: July 2022

Solid-state electrolytes are considered as key materials for overcoming the limitations of the liquid-electrolyte-based Li-ion batteries in terms of energy capacity, cyclability, and safety. Among the many possible solid-state electrolyte materials, inorganic sulfides are of intensive research interest mainly because the larger and more polarizable sulfur anions substantially enhance the mobility of cationic Li species. In particular, Li-P-S electrolytes, such as Li10GeP2S12and Li7P3S11, have been reported to have room-temperature Li-ion conductivity of greater than 10-2 S/cm, which is comparable to that of conventional liquid electrolytes. Despite the facile Li-ion transport, the Li-P-S electrolytes tend to undergo irreversible structural degradation within typical operating conditions of the battery. This lack of electrochemical stability leads to the formation of high impedance intermediate transition layers at the electrode/electrolyte interfaces, hindering the practical application of the Li-P-S electrolytes. Partial replacement of the element P with other elements within a Li-P-S structural family can improve the lithium-ion conductivity, but notable improvement in their electrochemical stability has yet to be achieved. Li-M-S (M = transition metals, such as Cr, Zr, Nb, Mo, and Sn) families can be possible candidates for electrochemically stabile solid-state electrolytes, while having excellent Li-ion transport properties of the inorganic sulfides. Like the Li-P-S structure, numerous Li-M-S structural derivatives have already been synthesized by varying the element M or by replacing a portion of the element M with another element, and the Li-ion conductivity and electrochemical stability are expected to be heavily dependent on the element composition and crystalline structure.
In this study, we investigate the motion and dynamics of Li-ions in Li-Zr-S and Li-Zn-Zr-S compound electrolyte by performing a series of first-principles calculations. To this end, we generate multiple Li-Zn-Zr-S compound model structures with varying Zr-to-Zn ratios. Then, we evaluate Li-ion conductivities by using velocity auto correlation scheme combined ab initio molecular dynamics (AIMD) simulations. More specifically, we calculate the diffusivity and ionic conductivity of the stoichiometric structure and at a range of defect concentrations on Li2+2xZnxZr1-xS3, from x = 0 to x = 0.5. Our calculation results reveal how the introduction of Zn into the Li-Zr-S compound affects the Li-ion mobilities. The theoretical insight obtained in this study well corroborates with recently reported experimental results for varying ionic conductivities in Li-Zn-Zr-S electrolytes depending on the Zr-to-Zn ratio. This fundamental understanding can be an important theoretical basis for developing practically applicable Li-M-S electrolytes.

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(Digital Presentation) Effects of Cation Doping on the Stability and Charge Acceptance of Alpha Nickel Hydroxide for Energy Storage Applications
Authors: Ilhan Turan , Göynük Tansu , Karakaya Ishak 
Published: July 2022

Nickel hydroxide is used as active material in nickel based batteries and capacitors. It has two phases which are alpha and beta, since alpha nickel hydroxide has higher capacity it attracts scientists attention. Although it has promising performance, low utilization and poor stability hinder commercialization of alpha nickel hydroxide. The most common strategy to improve stability is to dope nickel hydroxide with cobalt or aluminum. Aluminum is more prominent due to its lower price and environmental concern. Besides the stability, it is well known that discharge capacity of nickel hydroxide decreases with increasing amount of both aluminum and cobalt. Although capacity is decrasing, number of electrons which is involved in the reaction does not change with increasing amount of dopant. At the same molar doping levels, although aluminum doped samples had higher active mass (nickel) content, they had lower gravimetric capacity than cobalt doped samples. Therefore, it is not convenient to explain capacity loss by only decreasing amount of active mass.
Since cobalt doping raises differences between oxygen evolution potential and oxidation potential of nickel hydroxide, it enhances chargeability of nickel hydroxide but the cyclic voltammetry results showed that higher cobalt doping causes decrease in cell voltage and energy density of battery. The results showed that higher amount of aluminum must be doped to improve stability and relatively small amount of cobalt must be used to improve chargeability of alpha nickel hydroxide. Therefore, both aluminum and cobalt are effective in improving stability but cobalt is advantageous at low doping level, as it is reported in the literature.
Investigation of Temperature-Triggered Collapse of Surface-Bound ELP
Authors: Feeney Stanley , Balog Eva Rose M , Halpern Jeffrey M 
Published: July 2022

The reversible Lower Critical Solution Temperature (LCST) response of Elastin-Like Polymers (ELP) has been investigated. It is well known that the coacervation versus solubility of ELPs in solution can be triggered by different factors including ionic strength and temperature. Recently our group studied the electrochemical impedance spectroscopy (EIS) response of ELP-modified surfaces associated with changes in ionic strength, and we observed intermediate states of ELP surface collapse.1

Within this work, we present our progress on monitoring the thermal response of surface-bound ELP. We will examine the localized temperature-triggered collapse for a (VPGIG)40 ELP (with a cysteine near the N terminus) with EIS to better understand the way charge transfer changes within a range of temperature and intermediate states. We studied two surfaces, (1) carboxyphenyl-modified glassy carbon electrode modified with ELP via EDC/NHS bioconjugation chemistry and (2) gold electrode thiol-bonded ELP surfaces. We will report on observed changes in charge transfer resistance from 5 to 40 degrees Celsius.
[1] Morales, M.A., Paiva, W.A., Marvin, L., Balog, E.R.M. and Halpern, J.M., 2019. Electrochemical characterization of the stimuli-response of surface-immobilized elastin-like polymers. Soft matter, 15(47), pp.9640-9646.
(Digital Presentation) Improved Nanocatalysts, Supported IrOx and IrRuOx, for Enhanced Oxygen Evolution Reaction
Authors: Bornet Aline , Berner Etienne , Quinson Jonathan , Schröder Johanna , Arenz Matthias 
Published: July 2022

The production of hydrogen via acidic electrochemical water splitting is an important pillar towards more sustainability. The overall water electrolysis is hindered by the slow kinetics of the oxygen evolution reaction (OER). Therefore, the catalyst material for the anode still requires optimization. Hereby, we present two highly active OER catalysts, IrOx and Ir0.4Ru0.6Ox nanoparticles (NPs), prepared by a straightforward, surfactant-free, colloidal synthetic route.1 The metallic NPs are ~1.5 nm in diameter and were deposited on carbon Ketjen Black (CKB) as well as on antimony doped tin oxide (ATO) to investigate the active phase as well as potential influences of the support material. After the colloidal synthesis and supporting, the catalysts were activated, thus undergoing a particle growth of ~1 nm. Their performance was benchmarked in terms of activity and stability using our recently developed electrochemical flow cell called gas diffusion electrode (GDE) setup.2 This novel approach allows closing the experimental gap between the two most common methods, namely the rotating disk electrode (RDE) and the membrane electrode assembly (MEA). Independently from the support, Ir0.4Ru0.6Ox shows a higher activity towards OER than IrOx at three tested temperatures, i.e. 30, 40, 60 °C. The two different support materials were also compared, and it was found that independently from the material, NPs deposited on CKB showed slightly higher activity at low current densities (up to 40 mA mgIr
-1). As expected, accelerated potentiostatic stability test reveals a rapid degradation of the IrOx/CKB, while IrOx/ATO and Ir0.4Ru0.6Ox/ATO exhibit similar stability than commercially available Ir black.
[1] Francesco Bizzotto, Jonathan Quinson, Alessandro Zana, Jacob J. K. Kirkensgaard, Alexandre Dworzak, Mehtap Oezaslan, Matthias Arenz, Catal. Sci. Technol., 2019, 9, 6345-6356.
[2] Johanna Schröder, Vladislav A. Mints, Aline Bornet, Etienne Berner, Mohammad Fathi Tovini, Jonathan Quinson, Gustav K. H. Wiberg, Francesco Bizzotto, Hany A. El-Sayed, Matthias Arenz, JACS Au, 2021, 1, 247-251.

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AuCu Nanostructures Active in the Visible Light – Optical and Photoelectrochemical Properties
Authors: Lipinska Wiktoria , Grochowska Katarzyna , Karczewski Jakub , Siuzdak Katarzyna 
Published: July 2022

Nowadays, due to global warming and increasing environmental pollution, intensified research on materials for energy harvesting from renewable sources is being carried on. Solar energy is one of the most abundant energy resources that can be converted into electric energy. Here, we demonstate that AuCu bimetallic nanostructures placed on structured titanium foil can be applied in solar driven processes [1, 2].
The electrode material is fabricated via Ti foil anodization process, chemical etching, thin AuCu layer (10 nm) magnetron sputtering and rapid thermal treatment at 600°C in varius atmospheres (air, vacuum, argon, hydrogen). AuCu nanoparticles are obtained only for annealing in air, while in argon and hydrogen porous structures and nanoplates are formed, respectively. UV-vis spectroscopy and X-ray diffraction studies of marterials indicate that the shape of the reflectance spectra differ significantly due to the changes in material morphology as well as its structure. The reflectance band minima are located at 380 nm and 750 nm for electrode material annealed in air and hydrogen, respectivetly. Moreover, sample thermally treated in air exhibits wide absorbance band from 300 to 1000 nm, whereas the one annealed in hydrogen from 500 to 1000 nm. Linear voltammetry measurements in dark and under light illumination were carried out in 0.1M NaOH solution in order to evaluate the photoactivity. The highest photocurrent in visible light is obtained for AuCu electrode annealed in hydrogen (5 times higher than in air), however, under Uv-vis light for electrode processed in air.
All in all, thermal treatment in various atmospheres has a great impact on morphology, optical and photoelectrochemical activity of AuCu structures placed on Ti support material. We believe that presented results provide new opportunities in designing advanced photoactive materials.
Research is financed by National Science Centre (Poland): Grant no. 2019/35/N/ST5/02604.
[1] W. Lipińska, K. Grochowska, J. Ryl, J. Karczewski, K. Siuzdak,
Influence of Annealing Atmosphere on Photoelectrochemical Activity of TiO2 Nanotubes Modified with AuCu Nanoparticles, ACS Applied Materials and Interfaces, 13 (2021) 52967–52977, DOI: 10.1021/acsami.1c16271
[2] W. Lipińska, K. Grochowska, J. Karczewski, J. Ryl, A. Cenian, K. Siuzdak, Thermally tuneable optical and electrochemical properties of Au-Cu nanomosaic formed over the host titanium dimples, Chemical Engineering Journal, 399 (2020) 125673–125685, DOI: 10.1016/j.cej.2020.125673

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(Invited) Effects of the Local Chemical Environment on the Anode and Cathode Processes of CO2 Electrolyzers
Authors: Janaky Csaba 
Published: July 2022

Continuous-flow electrolyzers allow CO2 reduction at industrially relevant rates, but long-term operation is still challenging. In this talk, I am going to present some interesting findings on the role of different ions, crossing the anion exchange membrane in zero-gap electrolyzer cells, contributing to unstable operation.
In the first part of my talk, I will show that while precipitate formation in the cathode gas diffusion electrode is detrimental for the long-term stability, the presence of alkali metal cations at the cathode improves performance. To overcome this contradiction, we develop an operando activation and regeneration process, where the cathode of a zero-gap electrolyzer cell is periodically infused with alkali cation-containing solutions. [1] This enables deionized water-fed electrolyzers to operate at a CO2 reduction rate matching that of those using alkaline electrolytes (CO partial current density of 420 ± 50 mA cm−2 for over 200 hours). We deconvolute the complex effects of activation and validate the concept with five different electrolytes and three different commercial membranes. Finally, we demonstrate the scalability of this approach on a multi-cell electrolyzer stack, with a 100 cm2 / cell active area.
In the second part of the presentation, I will discuss the role of anode catalyst in CO2R cells. The urge to substitute Ir is driven by its high- and steeply rising market price as well as its limited stability in alkaline media. Although Ni is a ~ten thousand times cheaper, active, and stable oxygen evolution reaction (OER) catalyst in alkaline media, I will demonstrate that there are factors, which hinder its application in CO2 electrolysis. While Ni is a suitable OER catalyst in short experiments, the cell voltage increases, and the measured total Faradaic efficiency decreases continuously during prolonged electrolysis. This is caused by the local acidic pH at the anode surface, the crossing CO3
2- ions and by the gradual change in the anolyte composition, leading to Ni dissolution. The catalyst loss is only a minor part of the problem; the dissolving metal ions also penetrate into the anion exchange membrane, where precipitate forms due to the high local carbonate ion concentration, inducing cell failure.
Finally, I will present a complex machine learning based approach, through which we aim to find the optimal operating conditions of such CO2 electrolyzer cells.
Multi-Material Additive Manufacturing of Coreless Transformers By Aerosol Jet Printing and Electrochemical Deposition
Authors: Tsui Lok-kun , Sui Yongkun , Pillars Jamin R. , Hartmann Thomas Michael , Dye Joshua , Lavin Judi 
Published: July 2022

Coreless transformers are an attractive technology for power electronics due to their light weight and the absence of a brittle magnetic core material.[1] A coreless transformer consists of a primary spiral inductor with few turns and a secondary spiral inductor with many turns stacked together. Aerosol jet printing (AJP) is an additive manufacturing technology which can be used to print metals and polymers with linewidths as narrow as 10 µm. In this work we have used a combined AJP, electroless deposition, and electrodeposition approach to fabricate multi-layer coreless flyback transformers. This combined approach makes accessible both the high-resolution patterning from AJP and the high-density, high-conductivity materials such as Cu and Ni from electrochemical deposition techniques.[2]
We have designed two-layer primary and secondary inductors separated by AJP-deposited UV-curable dielectric layers. Micrographs of the primary and secondary inductors are shown in Figure 1(a) and 1(b) respectively. Electroless deposition of Cu and electrodeposition of Cu and Ni are optimized in order to minimize resistive losses and promote uniform film growth. The typical inductances measured on the 2-layer primary are 0.2 µH and the inductances measured on single layers of the secondary are on the order of 4 µH. Initial testing of the transformer for flyback voltage conversion demonstrated the capability of generating an output to input voltage ratio of >50. Comparisons of the experimentally measured inductance of the primary and secondary inductors as well as the transformer voltage ratio will be compared with simulated models.

SNL is managed and operated by NTESS under DOE NNSA contract DE-NA0003525. SAND2021-15239 A

References:
[1] S.C. Tang, S.Y. Hui, H.S.-H. Chung. IEEE Transactions on Power Electronics. 15 (2000) 931–941.
[2] L. Tsui, S.C. Kayser, S.A. Strong, J.M. Lavin. ECS J. Solid State Sci. Technol. 10 (2021) 047001.

Figure 1. Additively manufactured coreless transformer showing (a) the two-layer Ag-Cu-Ni primary inductor spiral and (b) the addition of a dielectric separation layer and one secondary inductor layer.

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(Invited) Scalable Printing of Flexible/Wearable Energy and Sensor Systems
Authors: Zhang Yanliang 
Published: July 2022

Nanoscale materials are attractive and promising building blocks for a broad range of emerging technologies due to their unique and superior properties compared to the bulk form. However, converting nanoscale materials into high-performing functional systems while translating their unique properties from nanoscale to macroscale remain a major challenge due to many scientific and technological obstacles.
This talk will focus on our research on developing versatile and synergistic additive manufacturing and nanomanufacturing methods to manufacture and transform a broad range of emerging functional nanomaterials into innovative and sustainable energy and sensor systems in a highly scalable, controllable and affordable manner. This talk will present our recent research progresses scalable printing and photonic sintering to fabricate flexible thermoelectric generator (f-TEG) for energy harvesting. Our printed p-type and n-type flexible films demonstrate peak thermoelectric figure of merit ZT greater than unity near room temperature, which is among the highest reported ZT values in flexible thermoelectric materials. In addition, this talk will also present a novel hybrid printing method that can integrate functional materials and soft structural materials and fabricate highly stretchable and wearable sensors for a broad range of physical and chemical sensing applications.