bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Invited) Layered Electrodes for Lithium-Ion Batteries
Authors: Li Jianlin , Kalnaus Sergiy , Livingston Kelsey , Wood David L. 
Published: July 2021

Development of lithium-ion batteries has dramatically boosted market adoption of electric vehicles. However, extending driving range is still necessary to further widespread adoption of lithium-ion batteries in electric vehicles, which relies on increased energy density. Increasing electrode areal loading is one effective approach to boost energy density as it reduces the weight fraction of current collectors and the volume fraction of separators, which do not contribute to battery capacity [1]. However, increased energy density in thick electrodes is usually achieved at the expense of power density mainly due to transport limitation of lithium ions through the porous electrodes. This results in electrolyte depletion and lower utilization of the electrodes [2].
To tackle the sluggish mass transport rates, novel electrode architectures are required. There have been various methods for creating unique electrode architectures to reduce electrode tortuosity and facilitate lithium ion diffusion, including laser ablation, co-extrusion, advanced slot-die coating, and freeze tape casting [3-5]. In this presentation, we will discuss design of layered electrodes for superior energy and power performance. Results from both experiment and simulation are included where effect of particle size of active materials, thickness ratio between layers and electrode porosity in each electrode layer were explored. It is demonstrated that the appropriate layered structure can more than double the power density compared to a traditional one.

Acknowledgment

This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) Advanced Manufacturing Office (AMO).

References:

[1] Jianlin Li, Zhijia Du, Rose Ruther, Seong Jin An, Lamuel David, Kevin Hays, Marissa Wood, Nathan Phillip, Yangping Sheng, Chengyu Mao, Sergiy Kalnaus, Claus Daniel, and David Wood, JOM, 89(9) (2017), 1484-1496.
[2] Zhijia Du, David Wood, Claus Daniel, Sergiy Kalnaus, and Jianlin Li, Journal of Applied Electrochemistry, 47 (2017) ,405-415.
[3] Corie Cobb, Scott Solberg, Journal of The Electrochemical Society 164 (7) (2017) A1339.
[4] Y. Zheng, H. J. Seifert, H. Shi, Y. Zhang, C. Kubel, W. Pfleging, Electrochimica Acta 317 (2019) 502.
[5] Ruhul Amin, Benjamin Delattre, Antoni Tomsia, and Yet-Ming Chiang, ACS Applied Energy materials, 1 (2018) 4976.
Alignment Design in Consideration with Tertiary Current Distribution of Thick Electrodes
Authors: Oh Hyeseong , Jeong Kyeong-Min 
Published: July 2021

With the increasing demands of lithium-ion batteries in electric vehicles (EVs) and energy storage systems (ESSs), high energy density and extreme fast-charging (XFC) characteristics are required. The easiest way to design high-energy-density cells is to make thick electrodes by minimizing separators and current collectors and maximizing active compounds, but for thicker electrodes, the kinetic losses increased with C-rate, and cycle stability deteriorated.1 On the sidewall of an electrode, there exists a current difference due to the current distribution by the location. This effect gets maximized in case of the thick electrode because there is a non-uniformity of the kinetics through the electrode thickness direction due to the difference of ionic and electronic conductivity within the pores of the electrode. Besides, different alignment margin of cathode and anode causes another current distribution on the sidewall.
In this study, pouch full cells with different alignment margin of LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode and graphite anode are considered to investigate the difference of the current distribution. N/P ratio is set under 1 to induce complete intercalation of lithium-ion from the cathode into graphite anode so that distinguish the capacity from lithium-ion intercalation and lithium plating onto the surface of an anode. Through the calculation of the current distribution of the edge of the thick electrode, the optimal alignment design of the anode is suggested. There exists the optimal alignment margin of anode and cathode with respect to the dimension of the electrode and the current density (C-rate) applied into the electrode.
References

Kuang, Yudi, et al. "Thick electrode batteries: principles, opportunities, and challenges." Advanced Energy Materials
33 (2019): 1901457.
Identification and Quantification of Aging Modes with Deep Learning Models
Authors: Kim Sangwook , Yi Zonggen , Tanim Tanvir R. , Dufek Eric J. 
Published: July 2021

Identifying the dominating aging modes and mechanisms uniquely with higher confidence using early life-cycle data is a significant scientific challenge. In general, lithium-ion batteries experience different aging modes depending on use conditions—e.g., loss of lithium inventory and loss of active material in both electrodes, loss of power capability, etc.—due to different relevant aging mechanisms. The existing body of research almost exclusively uses extended-calendar or cycling-life data along with different post-testing to identify and quantify different dominating aging modes and mechanisms. Early identification of battery aging modes/mechanisms will enable accurate forecasting of battery state-of-health along with the root cause and shorten the design and testing cycle for new battery chemistries and cell designs for emerging applications.
In this presentation, we present a deep learning (DL) modeling framework to enable early identification and quantification of dominating cell aging modes using battery incremental capacity (IC) information at different aging states (Figure 1). The DL model utilizes coin cell data with altered offset and N:P ratio simulating different aging conditions to train and construct two categories of DL models, serving two consecutive steps in the hierarchical learning framework: (i) a classification model to identify the dominating aging modes, e.g. LLI + LAMPE or LLI + LAMNE, (ii) a regression model to quantify the percentages for dominating aging modes, e.g., percentages of LLI and LAM. The deep learning models are built using a 1-D convolutional neural network structure.
The deep learning model’s performance is verified with experimental Gr/NMC pouch cells data with different loadings and utilization conditions. It is demonstrated that the classification model can identify dominating aging modes successfully for current experimental validation sets within 50 cycles, and the quantification model can further determine their percentages of LLI and LAM under aging modes.

Figure 1
(Invited) Calorimetry of Cell Failure in Multiple Formats and Capacity
Authors: Lamb Joshua , Torres-Castro Loraine 
Published: July 2021

Accelerating Rate Calorimetry (ARC) has previously been used to evaluate differences observed in various active materials with a typical comparison shown in the figure below. This evaluation is usually performed on small cells of roughly the same capacity (~1 AH) to allow for an easy comparison of active materials as they are developed. However, this and similar calorimetry methods present a means to perform more quantitative measurements of the heat generated and kinetics of thermal runaway. Sandia National Laboratories has performed testing on cells in the 10s of amp hours and analyzed the thermal runaway behavior of these cells.
This work uses accelerating rate calorimetry to evaluate the impact of cell chemistry, state of charge, cell capacity, and ultimately cell energy density on the total energy release and peak heating rates observed during thermal runaway of Li-ion batteries. This work seeks to better understand how applicable small cell data is to understand the thermal runaway behavior of large cells as well as determine if thermal runaway behaviors can be more generally tied to aspects of lithium-ion cells such as total stored energy and specific energy. We have found a strong linear correlation between the total enthalpy of the thermal runaway process and the stored energy of the cell, apparently independent of cell size and state of charge. We have also shown that peak heating rates and peak temperatures reached during thermal runaway events are more closely tied to specific energy, increasing exponentially in the case of peak heating rates.
Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Figure 1
Heat Generation in Lithium Iron Phosphate/Graphite Batteries: Simulation with Validation through Isothermal and Adiabatic Calorimetric Measurements
Authors: Schimpe Michael , Gillich Elisabeth Irene , Santhanagopalan Shriram , Saxon Aron , Jossen Andreas 
Published: July 2021

This work evaluates the heat generation characteristics of a cylindrical lithium iron phosphate/graphite battery. Two experimental approaches are used: Heat flow measurements in an isothermal calorimeter and temperature measurement-based heat generation rate measurements in a quasi-adiabatic Accelerating Rate Calorimeter (ARC).
The experimental results are compared to simulation results of an equivalent circuit model featuring a single resistance, voltage hysteresis representation, and reversible heat generation through entropy representation. The thermal model parameters are adapted to the respective experimental setups.
Results visualize the specific use-cases of the experimental approaches. Isothermal calorimeter measurements enable a strict control of temperature for the battery, however, smooth the higher dynamics of the battery heat transfer due to the thermal mass of the setup. The high rate of heat transfer to ambient enables an evaluation of specific operating temperatures as well as long-duration tests, e.g., full cycles or dynamic current profiles.
Instead, quasi-adiabatic measurements vary strongly in temperature during the operation but provide highly-dynamic information about heat generation rates. The rapid rise in temperature approaches safety limits and thus only low current, charge or discharge tests are possible, with a following rest period required.
Simulation results are discussed with a focus on the heat generation rate and the heat transfer to ambient rate. While in general good agreements between simulation and experiment is achieved, specific differences reveal improvement potential for the model as well as for its parametrization.

References

M. Keyser, A. Pesaran, Q. Li, S. Santhanagopalan, K. Smith, E. Wood, S. Ahmed, I. Bloom, E. Dufek and M. Shirk, Journal of Power Sources, 367, 228 (2017).
A. Pesaran, M. Keyser, G. Kim, S. Santhanagopalan and K. Smith, Tools for designing thermal management of batteries in electric drive vehicles (presentation), in, National Renewable Energy Lab.(NREL), Golden, CO (United States) (2013).
M. Schimpe, M. Naumann, N. Truong, H. C. Hesse, S. Santhanagopalan, A. Saxon and A. Jossen, Applied Energy, 210, 211 (2018).
A. R. Saxon, Battery Extreme Fast Charge: A Thermal Prospective, in, National Renewable Energy Lab.(NREL), Golden, CO (United States) (2019).
J. Geder, R. Arunachala, S. Jairam and A. Jossen, in 2015 IEEE Green Energy and Systems Conference (IGESC), p. 24 (2015).
Kinetic Mechanisms Driving Ag+ Reduction and Nanoparticle Synthesis By Atmospheric Pressure Plasma-Driven Solution Electrochemistry
Authors: Exarhos Stephen , Yue Yuanfu , Bruggeman Peter 
Published: July 2021

Plasma-driven solution electrochemistry (PDSE) is an emerging technique for processing novel materials among other applications. PDSE has a key advantage over conventional electrolysis in that it can inject electrons into solutions without the presence of a metal surface. Current applications of PDSE are limited because of prohibitive energy efficiencies and a lack of understanding in the underpinning processes, including the importance of plasma-injected species relative to solution-generated species and kinetics-limiting effects. Recent studies have shown that there are several factors that differ between PDSE and conventional electrolysis, meaning new and expanded models are required to precisely describe PDSE. For example, it is commonly assumed that reduction processes in PDSE are predominantly mediated by solvated electrons – as is the case in conventional electrolysis – while the influence of ions, photons, and radicals present in the system are considered to be negligible or not studied. However, recent work studying plasma-liquid interactions from ours and other groups have indicated that, while solvated electrons are certainly significant in PDSE reduction processes, they are not wholly deterministic of the plasma-induced solution phase kinetics. The work presented is an investigation of reduction kinetics of Ag+ using a quasi-continuous flow pulsed-DC atmospheric pressure PDSE system. We focus on the evolution of the solution phase from pre- to post-plasma exposure. We present experimental results that, although gathered from indirect characterization techniques, allow us to infer information about the kinetics mediating Ag+ reduction and ensuing nanoparticle nucleation and growth. Specifically, we seek to deconvolve UV-photon induced reactions, neutral hydrogen-driven reduction, and neutral hydroxide-driven processes, in addition to solvated electron-driven reduction. A refined understanding of PDSE in a model system like Ag will enable access to more complex, more efficient, and higher yield chemical processes in PDSE systems that are not possible with conventional electrochemistry.
This work was supported by the Army Research Office under Grant Number W911NF-20-1-0105.
(Invited) 3D Epitaxially-Connected Quantum Dot Superlattices: Formation, Structure, and Transport
Authors: Law Matt 
Published: July 2021

Colloidal quantum dots (QDs) that are epitaxially interconnected (necked or partially fused) to form highly-ordered, highly-coupled superlattices are an exciting new class of materials for optoelectronics. These epitaxially-fused QD superlattices (epi-SLs), which are typically made by self-assembly and ligand exchange on a liquid surface followed by stamp transfer to a solid substrate (the Langmuir-Schaefer technique), promise to combine the size-tunable photophysics and solution processability of QDs with delocalized, bulk-like carrier transport.
In this talk, I describe recent progress in making epi-SLs of sufficient spatial and energetic order to delocalize carriers into mini-bands. I discuss the fabrication of high-quality 3D epi-SL films, along with the determination of their structure (the complete superlattice unit cell) and physical formation pathway from the parent oleate-capped SL using a combination of X-ray scattering and correlative electron microscopy and diffraction of single SL grains. The oleate- to epi-SL phase transition occurs by nearly-pure translation of the QDs with minimal rotational motion, resulting in a rhombohedrally-distorted simple cubic epi-SL with fusion along the PbSe {100} facets. This simple translational phase transition is facilitated by the rhombohedral distortion of the initial oleate-capped SL and results in >5 μm epi-SL grains free of linear or planar defects. While large epi-SL grains are useful, several types of intra-grain structural defects conspire to reduce order within the grains and localize charge carriers. Quantitative characterization of these intra-grain defects and a better understanding of the molecular processes involved in epi-SL formation have enabled fabrication improvements that enhance intra-grain order and overall film uniformity. Measurements probing mini-band formation and the impact of SL surface chemistry on charge transport will be discussed.
Cation Effect on Anion Exchange in CsPbX3 (X = Cl, Br, I) Perovskite Nanocrystals
Authors: Ahn Junhyuk , Lee Yong Min , Kim Woosik , Oh Soong Ju 
Published: July 2021

Colloidal quantum dot and nanocrystals have been shown to be promising materials for device applications because of their
unique size-dependent properties and solution processability. We present general methods to engineer the
electronic, optoelectronic, electromechanical, and electrothermal properties of nanocrystals through their
surface and interface engineering. Unconventional materials design and strategy are introduced to
fabricate semiconducting devices such as field effect transistors, photodetectors, solar cells, and wearable
sensors including temperature sensors, strain sensors, and pressure sensors. This technique provides a
pathway for designing low cost, high performance, and multifunctional electronic skins or wearable
devices.
Electrophoretic Deposition of Aluminum Particles and Control of the Coating Microstructure
Authors: Wagner Julien , Ansart Florence , Taberna Pierre-Louis , Gani Léa , Knittel Stéphane 
Published: July 2021

Electrophoretic deposition (EPD) is an efficient process for the elaboration of homogeneous thickness and tunable microstructure coating on conductive substrates [1]. EPD displays several advantages such as a low operating cost, a relatively simple equipment and the ability to plate uniformly onto complex shape parts [1]. Among all studies on electrophoretic deposition, metallic particles are widely less investigated than ceramic ones. However metallic materials offer interesting properties (optics, catalysis, etc.). The use of alcoholic media is widely advantageous for electrophoretic deposition process because a significant voltage range can be investigated while avoiding water electrolysis and bubbles formation. Moreover, as some metals present high reactivity towards aqueous media, the choice of alcohols as dispersing media looks appropriated. Electrophoretic deposition of an aluminum powder was performed in different alcoholic media: ethanol and propan-2-ol. The nature of the dispersing medium appears to strongly influence the process deposition. Direct EPD from pure ethanol suspension is not convenient [2] whereas deposition from propan-2-ol medium leads to an homogenous coating (Figure 1). Nevertheless, addition of ionic species into the ethanol suspension allows an increase of the number of aluminum particles deposited. The addition of these species also lead the formation of homogenous thickness coating up to 100 µm. The influence of the key parameters (relative to the suspension and the electrophoretic process) has been investigated in relationship to the coatings thickness and the microstructure.
Keywords: electrophoretic deposition, aluminum, coating, microstructure.
Figure 1: FIB-prepared cross-section of Al coating deposited under 10 V.cm-1 during 10 min from propan-2-ol suspension.
References:
1. L. Besra and M. Liu, “A review on fundamentals and applications of electrophoretic deposition (EPD),” Prog. Mater. Sci., vol. 52, no. 1, pp. 1–61, 2007.
2. K. S. Yang, Z. Jiang, and J. S. Chung, “Electrophoretically Al-coated wire mesh and its application for catalytic oxidation of 1,2-dichlorobenzene,” Surf. Coatings Technol., vol. 168, no. 2–3, pp. 103–110, 2003.

Figure 1
Revealing Active Sites in Atomically Dispersed Metal Catalysts on N-Doped Carbon for Electrocatalytic CO2 Reduction By Operando XAS
Authors: Li Tao , Fang Lingzhe 
Published: July 2021

Abstract

Single-atom catalysts (SACs) represent a promising class of low-cost materials with high catalytic activity and 100% atom-utilization efficiency, widely applied in energy conversion fields.[1-2] Benefit from tunable coordination environment, the uniformly dispersed SACs on diverse supports exhibit satisfied catalytic ability. More importantly, different from the multiple crystal facets of nanomaterials can serve as active sites. There is only one active site consisting of the single metal atom and coordinated atoms in SACs, thereby improving the selectivity of products some catalytic reactions. Moreover, atomically dispersed metal catalysts exist in cations, which exhibit better stability than traditional nanoparticulated counterparts.[3] However, SACs are susceptible to undergo restructuring during the reactions because of high surface free energy. Therefore, exploring the active sites of SACs through in-situ characterization techniques plays a critical role in studying the reaction mechanism and guiding the design of optimum SACs.
As a synchrotron-based element-specific technique, X-ray absorption spectroscopy (XAS) is influential in studying the probed element's structural information. X-ray absorption near edge structure (XANES) spectra reflect the electronic structure, while extended X-ray absorption fine structure (EXAFS) spectra provide local atomic structural information such as coordination number, bond length, and structural disorder. Thus, in-situ XAS is promising and widely used for monitoring electronic structure and atomic configuration changes of SACs during real-time working conditions. We have prepared Ni, Cu single atoms on nitrogen-doped carbon (NiCu@NC-900), which exhibit improved catalytic ability compared with Ni SACs and Cu SACs. Nuclear magnetic resonance results show only ethanol as a liquid product during CO2 reduction reaction (CO2RR). To explore the origin of improved catalytic performance of SACs toward CO2RR, we are going to monitor changes of SACs under open-circuit voltage (OCV) and working conditions by Operando XAS.
[1] Li, Z., Ji, S., Liu, Y., Cao, X., Tian, S., Chen, Y., Niu, Z., Li, Y. Chem. Rev. 120, 2 (2020).
[2] Ji, S., Chen, Y., Wang, X., Zhang, Z., Wang, D., Li, Y. Chem. Rev. 120, 21 (2020).
[3] Speck, F. D., Paul, M. T. Y., Ruiz-Zepeda, F., Gatalo, M., Kim, H., Kwon, H. C., Mayrhofer, K. J. J., Choi, M., Choi, C. H., Hodnik, N., Cherevko, S. J. Am. Chem. Soc. 142, 36 (2020).
Electrochemical Animal Waste Remediation: Multi-Factor Effect Analyses on Nutrient Reduction and Struvite Deposition
Authors: Ojoawo Babatunde IBRAHIM , Pindine Garrett , Trembly Jason , Daramola Damilola 
Published: July 2021

Proper usage of land to meet the global growing demand in the area of food supply, safe environment and good quality of water bodies requires the delivery of fertilizer for specific nutrient needs. Most of the farmers directly use animal waste as a fertilizer on the farm, which causes eutrophication to the water bodies due to excess nutrient accumulation.
A lot of research has been conducted on the use of chemical means to recover the amount of phosphorus and nitrogen in wastewater as struvite (MgNH4PO46H2O), however this project explores the use of an electrochemical method for struvite deposition using a (graphite) anode and a stainless steel cathode in an undivided cell. Therefore, this electrochemical technique is relatively simple and cheap.
In a prior study, the efficacy of this technology was examined with key operating parameters affecting struvite deposition identified as temperature, turbulence, applied potential and competing ion (Ca2+) concentration [1]. In addition, a thermodynamic simulation was developed to further investigate the impact of Ca2+ in animal waste on the technology’s performance [2]. However, the effect of parameter interactions on electrochemical nutrients reduction is unknown. In this new study, multi-factor analyses will be conducted based on the combination of the previously identified operating parameters and N:P ratio, to characterize optimal nutrient reduction and resource recovery from animal waste.
References
[1] Z. Belarbi and J. P. Trembly, “Electrochemical Processing to Capture Phosphorus from Simulated Concentrated Animal Feeding Operations Waste,” J. Electrochem. Soc., vol. 165, no. 13, pp. E685–E693, Jan. 2018, doi: 10.1149/2.0891813jes.
[2] Z. Belarbi, D. Daramola and J. P. Trembly, “Bench-Scale Demonstration and Thermodynamic Simulations of Electrochemical Nutrient Reduction in Wastewater via Recovery as Struvite,” J. Electrochem. Soc., vol. 167, no. 4, Nov. 2020, DOI: 10.1149/1945-7111/abc58f