bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Invited) Enhancing PET Plastic Circularity and Decarbonization through Process Electrification and Intensification
Authors: Bunke Samantha , Yu Hyejin , Cha Hyun Gil , Tarpeh William Abraham , Kang Donghyeon 
Published: December 2024

Polyethylene terephthalate (PET) production generates roughly 3.2 kg of CO2 per kg of resin.[1] As the most produced plastic globally (82 million metric tons per year), PET contributes to 272 million metric tons of CO2 equivalent annually. Chemical depolymerization of PET into its monomers is a key strategy for achieving plastic circularity. While various methods have emerged in recent decades, current chemical recycling processes are often uneconomical and do not significantly reduce greenhouse gas emissions. For instance, catalytic depolymerization using base catalysts (e.g., NaOH) in alcohols is being commercialized, but NaOH is neither a superior catalyst nor cost-effective due to its production and delivery expenses. Consequently, the high cost leads to PET waste ending up in landfills or incinerators, perpetuating low circularity and high CO2 emissions.[2,3]
To address these limitations in chemical PET depolymerization, our team has developed an innovative electrochemical system for efficient and cost-effective PET recycling. This system selectively decomposes mixed plastic waste at room temperature and ambient pressure, achieving rapid depolymerization into virgin-quality PET monomers. The process is intensified through electrification, significantly reducing overall costs and CO2 emissions while promoting PET circularity. By incorporating renewable electricity, the system can utilize excess energy generated during off-peak hours. Additionally, the process co-produces valuable chemicals like hydrogen and hydrochloric acid (HCl), ultimately making PET recycling economically viable. We are committed to further maturing this electrochemical PET depolymerization technology with the goal of commercialization.
References
[1] Gracida-Alvarez, U. R.; Xu, H.; Benavides, P. T.; Wang, M.; Hawkins, T. R., Circular Economy Sustainability Analysis Framework for Plastics: Application for Poly(ethylene Terephthalate) (PET). ACS Sustainable Chemistry & Engineering
2023, 11, (2), 514-524.
[2] Nicholson, S. R.; Rorrer, N. A.; Carpenter, A. C.; Beckham, G. T., Manufacturing energy and greenhouse gas emissions associated with plastics consumption. Joule
2021, 5, (3), 673-686.
[3] Martín, A. J.; Mondelli, C.; Jaydev, S. D.; Pérez-Ramírez, J., Catalytic processing of plastic waste on the rise. Chem
2021, 7, (6), 1487-1533.

Figure 1
Coatings Based on Single-Ion and Intrinsically Conducting Polymers for High-Voltage Cathode Materials
Authors: Guerrero Mejía Luis Miguel , Ruiz-Zepeda Francisco , Tchernychova Elena , Dominko Robert 
Published: December 2024

One of the main challenges presented by cathodic materials for lithium batteries is to ensure that capacity is maintained during cycling. The Ni-rich cathode LiNi0.8Mn0.1Co0.1O2 (NMC811) is considered a promising material due to its high energy density. However, this material presents a rapid decay in its capacity during the first charging and discharging cycles due to the direct contact of the NMC811 particles with the electrolyte. In this work, we have investigated the development and the effects on the electrochemical properties of a polymer coating based on a lithium single-ion conductor together with a conjugated polymer that prevents direct contact between the NMC811 particles and the electrolyte. These materials are used to create a homogeneous coating that acts as a channel for the transport of lithium only between the two interphases. It also serves as an electronic conductor that promotes good contact between the NMC811 particles, the carbon black, and the current collector. Furthermore, there are no reports on the use of single-ion conducting polymers as coatings for NMC materials, only reports on intrinsically conducting polymers to improve the electronic conductivity between cathodic components and capacity retention. In addition, these coatings act as an artificial cathode-electrolyte interphase to prevent unwanted reactions. X-ray photoelectron spectroscopy (XPS) was carried out to investigate the presence and evolution of these coating compounds during cycling. In addition, SEM and TEM were performed to observe the surface morphology of the particles and determine the thickness of the coating. Finally, electrochemical impedance spectroscopy (EIS) was used to evaluate the effects of the coating compounds on the charging and discharging processes as well as their stability during cycling. This study shows that the development of modulated coatings can provide an innovative approach to obtaining Ni-rich cathode materials with a longer lifespan for lithium batteries.
L.M. Guerrero Mejía et al. manuscript in preparation.
Enhancing the Energy Density and Cycle Life of Li/Sulfurized Polyacrylonitrile (SPAN) Batteries
Authors: Phan An , LE Phung M-L , Wang Chunsheng 
Published: December 2024

Li/sulfurized polyacrylonitrile (Li/SPAN) batteries are garnering attention for their potential in sustainable energy storage with notable advantages such as a high theoretical energy density exceeding 1000 Wh kg-1, surpassing the 750 Wh kg-1 of Li/NMC811, and being free of transition metals. The absence of transition metals addresses concerns related to their cost, scarcity, uneven distribution, and potential toxicity. However, current Li/SPAN batteries have yet to realize their full potential in terms of energy density and cycle life. This shortfall can be attributed to a lack of comprehensive understanding across various system levels, resulting in a dearth of well-directed research efforts.
In this work, we conduct a thorough study of the energy density and cycle life of practical Li/SPAN cells using internally developed models. Our analysis revealed refreshed perspectives from the common consensus among the Li/SPAN battery community. Concerning energy density, we find that this output is notably influenced by SPAN voltage, electrolyte weight, and inactive weights. In addition to the conventional method of enhancing SPAN specific capacity, these parameters present fresh opportunities to boost the energy density of Li/SPAN batteries. Details about potential executive strategies and practical viability regarding each parameter are also discussed.
Regarding cycle life, while the Coulombic efficiency of Li plating/stripping (Li CE) is widely recognized as a critical factor, our analysis reveals that its impact primarily lies in regulating the consumption of the electrolyte rather than that of Li metal. Therefore, controlling the chemistry of side reactions, represented by the average equivalent molecular weight (i.e., molecular weight over number of exchanged electron) and electrolyte density, emerges as a complementary approach to improve cycle life. Overall, our findings suggest that transitioning from heavy hydrofluoroether-based localized high-concentration electrolytes (LHCEs) to lightweight alkyl ether-based weakly-solvating electrolytes is beneficial for advancing Li/SPAN batteries, both in terms of energy density and cycle life.
(Invited) Thin Organic Crystal Films of Single Li+ Ion Conductors for Lithium-Ion Batteries
Authors: Byon Hye Ryung 
Published: December 2024

Despite the significant attention given to polymeric electrolytes in lithium (Li)-ion batteries, their practical use has been hindered by low ionic conductivity. The sluggish Li+ transport is primarily attributed to the segmental motion of the polymer backbone. Thus, it is crucial to develop rigid and well-defined crystal structures. Covalent organic frameworks (COFs) present a promising solution as electrolytes, composed of well-ordered and stacked layers encompassing ionic channels. By tethering anionic substitutes associated Li+ to the edges of the channels, the COF becomes the Li+ ion conductors. Typically, a COF electrolyte is prepared using powdery particles, and subsequent pelletization forms a thick film with a thickness exceeding 100 µm. Unfortunately, this electrolyte results in significant roughness and tortuosity, leading to a high contact resistance of over 1 kΩ and disrupting the ionic channel.
To address this issue, we developed a one-pot synthetic method to create a uniform COF film with approximately 20 µm thickness and a roughness of ~4 nm. The introduction of the sulfonate group resulted in ~2 nm pore size, and the COF layers are stacked through pi-pi interactions with high crystallinity. We varied the thickness of the COF film from 20 to 60 µm and compared their crystallinity and ionic conductivity. The result showed that both crystallinity and logarithmical ionic conductivity increased as the film thickness decreased. In the COF film with a thickness of 20 µm, the ionic conductivity reached around 10-4 S cm-1 at 30 oC. The interfacial resistance at metallic Li was approximately 250 Ω, eight times lower than that of the pellet-type COF. These films exhibited stable cyclability in symmetric Li cells over 1000 hours at room temperatures. Additionally, Li|LiFePO4 cells with the COF electrolyte demonstrated 86% capacity retention over 300 cycles and a 99.95% Coulombic efficiency at a 0.5 C rate.
Highly Reversible Lithium Deposition and Stripping Under Practical Conditions through Improved Wettability of Polyolefin Separator to Highly Concentrated Electrolytes
Authors: Ugata Yosuke , Yabuuchi Naoaki 
Published: December 2024

Lithium metal is regarded as a promising negative electrode material for rechargeable batteries, but several challenges such as the dendritic growth of lithium metal and side reactions between lithium metal and electrolyte hinder the practical application of lithium metal batteries (LMBs). In recent years, several research groups reported that highly concentrated electrolytes (HCEs) are effective in suppressing side reactions and improving the electrode reversibility of lithium metal.[1] However, the poor wettability of conventional polyolefin separators toward HCEs remains a critical issue to be addressed. Although porous glass fiber filters are often used as separators for HCEs, lithium dendrites easily penetrate the separator during repeated lithium deposition/stripping at areal capacities over 1 mA h cm−2, leading to an internal short circuit. Here, we present the effective strategies to solve the electrolyte wettability issue and to achieve stable cycling of LMBs under practical conditions. The use of a functional polyolefin separator coated on both sides with an aramid layer improves the electrolyte wettability because polar functional groups provide a better affinity between the polyolefin separator and HCE.[2] The combined use of HCE (5 mol dm-3 LiN(SO2F)2 in 1,2-dimethoxyetahne) and aramid-coated polyolefin separator increases the reversible lithium deposition capacity up to >10 mA h cm−2 and results in stable lithium deposition/stripping cycling with high Coulombic efficiency of ~99% at practical areal capacity of 4 mA h cm−2. From these results, the possibility of developing practical high-energy LMBs with HCEs will be discussed.
References
[1] Yosuke Ugata and Naoaki Yabuuchi, Trends in Chemistry, 5, 672–683 (2023).
[2] Yosuke Ugata, Chihaya Motoki, Satoshi Nishikawa, and Naoaki Yabuuchi, Energy Advances, 2, 503-507 (2023).
Understanding Electrolyte Stability and Instability in Lithium-Ion Batteries with Nickel-Rich Cathodes
Authors: Terreblanche Jason S , Luo Tongjun , Piper Louis F. , Dose Wesley M. 
Published: December 2024

Developing electrolyte solutions that are stable at the electrode-electrolyte interfaces is critically important to enable high performance lithium-ion batteries. The discovery in the early 1990s that a mixture of ethylene carbonate (EC) and alkyl carbonate(s) could passivate graphite led to a step change in the cell energy density,1,2 and modern batteries still retain this skeleton electrolyte formulation and graphite anode combination. However, as the battery industry shifts to nickel-rich layered oxide cathodes for lower cost and higher energy density cells,3,4 an incompatibility between EC-containing electrolytes and the cathode is starting to be revealed. This is driving research efforts to, firstly, understand the chemical reactions at the nickel-rich cathode-electrolyte interface5-9 and, secondly, explore new EC-free electrolyte solutions.10-13

Here we examine the dominant degradation phenomena in nickel-rich NMC/graphite full cells with EC-containing and EC-free electrolytes. We combine a range of methods including cell cycling, operando pressure measurements, OEMS, XPS, XRF, and solution NMR to understand the behaviour of the two electrolyte systems throughout the full cell. The results of these studies will be discussed in conjunction with their implications for further development of compatible electrolytes for advanced lithium-ion battery chemistries.
References:

Xu, Nat. Energy, 2021, 6, 763.

Fujimoto, N. Yoshinaga, K. Ueno, N. Furukawa, T. Nohma, M. Takahashi, Japanese patent, 3,229,635, 1991.

Xu, X. Liu, A. Daali, R. Amine, Z. Chen, K. Amine, Adv. Funct. Mater., 2020, 30, 2004748

Li, E.M. Erickson, A. Manthiram, Nat. Energy, 2020, 5, 26.

Wandt, A.T.S. Freiberg, A. Ogrodnik, H.A. Gasteiger, Mater. Today, 2018, 21, 825.

T.S. Freiberg, M.K. Roos, J. Wandt, R. de Vivie-Riedle, H.A. Gasteiger, J. Phys. Chem. A, 2018, 122, 8828.

Zhang, Y. Katayama, R. Tatara, L. Giordano, Y. Yu, D. Fraggedakis, J.G. Sun, F. Maglia, R. Jung, M.Z. Bazant, Y. Shao-Horn, Energy Environ. Sci. 2020, 13, 183.

M. Dose, I. Temprano, J.P. Allen, E. Bjorklund, C.A. O'Keefe, W. Li, B.L. Mehdi, R.S. Weatherup, M.F.L. De Volder, C.P. Grey, ACS Appl. Mater. Interfaces, 2022, 14, 13206.

M. Dose, W. Li, I. Temprano, C.A. O’Keefe, B.L. Mehdi, M.F.L. De Volder, C.P. Grey, ACS Energy Lett., 2022, 7, 3524.

Xia, R. Petibon, D. Xiong, L. Ma, J.R. Dahn, J. Power Sources, 2016, 328, 124.

Petibon, J. Xia, L. Ma, M.K.G. Bauer, K.J. Nelson, J.R. Dahn, J. Electrochem. Soc. 2016, 163, A2571.

Li, A. Dolocan, J. Li, Q. Xie, A. Manthiram, Adv. Energy Mater., 2019, 9, 1901152.

Pan, Z. Cui, M. Yi, Q. Xie, A. Manthiram, Adv. Energy Mater., 2022, 12, 2103806.

Figure 1
Synthesis and Characterization of Advanced Thin-Film Metallic Glass Anodes for Lithium Metal Batteries
Authors: Howard Jerry , Carlson Krista , Chidambaram Dev 
Published: December 2024

Instability of the solid-electrolyte interphase (SEI) formed on the surface of the anode is a major cause of capacity degradation in Li-ion and Li metal batteries. High-capacity anode materials which form a stable SEI are desirable for improving the lifetime performance of batteries made using these technologies. One such class of materials that has been suggested are Si-based metallic glasses. Si alloys have a high theoretical capacity, and the amorphous structure has been shown to improve capacity. The SEI layer that forms on these anodes is thin and highly stable. In this research, a genetic algorithm method was used to locate optimal compositions of Si-based metallic glasses for use in Li metal batteries. Sputtering was then employed as a high-throughput, combinatorial method to produce a library of compositions for initial characterization and electrochemical testing. Nanostructured metallic glass anodes with improved capacity and high electrochemically active surface area were then synthesized. The capacity and stability of these anode materials were tested in Li metal batteries. After battery testing, the SEI formed on the anode was characterized to understand its chemistry and structure.
This work is funded by NASA under grant 80NSSC19M0152. JRH is funded as a fellow under the NSF GRFP.
(Invited) High-Performance Ni-Rich Cathodes through Microstructure- and Surface-Modification for Electric Vehicle Batteries
Authors: Sun Yang-Kook 
Published: December 2024

The surge in battery production has prompted the diversification of battery chemistries to strengthen the resilience of battery supply chains. Among battery components, cathodes are considered defining features because they primarily determine both battery cost and performance. Among the existing cathode materials available in LIBs, Ni-rich layered lithium transition-metal oxides, NCM(A) are the most practical candidates for EVs and have been studied extensively in the past two decades because of their high reversible capacity and good rate capability. As the Ni content approaches more than 90%, however, it is challenging to realize high-energy Ni-rich NCM(A) cathodes without sacrificing durability. Capacity fading of Ni-rich NCM(A) cathodes largely originates from microcracking which exposes a large portion of the cathode interior to deleterious electrolyte attack. To suppress the development of microcracks on cathode materials, Ni-rich cathode materials should guarantee mechanical stability even in highly charged states. Furthermore, various side reactions at the cathode–electrolyte interface contribute to the rapid capacity fading of the Ni-rich cathode materials.
In this presentation, Ni-rich layered cathodes through microstructure- and surface-modification are presented. We improved the cycling stability of a Ni-rich NCMA cathode using a combination strategy involving microstructural refinement via high valence dopant and surface modification by F coating. The introduction of high valence dopant into the NCMA cathode, refines, elongates, and radially aligns its bulky primary particles by impeding the coarsening of primary particles of hydroxide precursor, thereby preserving the microstructure until the cathode attains optimal crystal structure. Furthermore, F coating promotes the formation of a stable LiF layer by reacting with the residual lithium on the surface of the cathode material. The preformed LiF on the cathode surface impedes the decomposition of salts, preventing their by-products from triggering the autocatalytic side reactions at the electrolyte–cathode interface and thereby suppressing gas generation during cycling. The combination of the elimination of the residual lithium, microstructure refining, and formation of a LiF layer on the near-surface can significantly extend the cycle life of Ni-rich cathodes to simultaneously satisfy the energy density, durability and safety requirements of next-generation batteries for practical applications.
Deep Learning Analysis of Solid Electrolyte Interface Microstructures in Lithium-Ion Batteries
Authors: Borshon Ishraque Zaman , Jabbari Vahid , Kingston Todd A. , Mashayek Farzad , Shahbazian-Yassar Reza , Yurkiv Vitaliy 
Published: December 2024

Understanding the structure of the solid-electrolyte interface (SEI) in lithium-ion batteries (LIBs) is crucial for improving battery performance and safety. This study introduces a novel deep learning (DL) framework to analyze transmission electron microscopy (TEM) images of SEI, specifically focusing on identifying different types of grains and grain boundaries. Utilizing advanced machine learning (ML) algorithms, including deep convolutional neural networks, our approach enables the accurate segmentation and classification of complex microstructural features in SEI layers based on the experimental high-resolution TEM images.
The DL model was trained on a comprehensive dataset of simulated SEI TEM images, generated through density functional theory (DFT) calculations and cryogenic high-resolution TEM (cryo-HRTEM) imaging. These simulations provided a diverse range of SEI microstructures, reflecting the polycrystalline nature of real battery interfaces. The model's ability to discern between various grains and grain boundaries in the SEI was fine-tuned through this training process, ensuring high accuracy and reliability in subsequent experimental image analyses.
Experimental validation was performed using cryo-HRTEM images of lithium-based batteries' SEI layers. The results demonstrated the model's proficiency in identifying and classifying different grain and grain boundary types, with significant accuracy. Particularly, the model successfully mapped the distribution of Li2O, LiF, and Li2CO3 components within the SEI, as well as adeptly identified the crystallographic orientations of grains, such as the LiF(111)/Li2CO3(200) and Li2O(111)/Li2CO3(111) boundaries, unraveling the complex structure of the SEI at a nanoscopic level. Consequently, these structural features were correlated with ion diffusion pathways and potential sites for lithium dendrite formation – a detrimental phenomenon in LIBs leading to thermal runaway.
This DL-based analysis provides new insights into the microscopic mechanisms governing ion transport and degradation in battery SEI layers. By offering a detailed characterization of grain and grain boundary structures, our method sets the groundwork for targeted improvements in battery design and materials selection. The study underscores the potential of integrating ML with advanced microscopy techniques to unravel the complex interplays within battery materials, propelling the field towards more resilient and efficient energy storage solutions.
VY and TAK gratefully acknowledge financial support from the Department of Defense (DoD) Office of Naval Research (ONR) through the Defense Established Program to Stimulate Competitive Research (DEPSCoR).
Investigation of Sodium Leaching into Electrolytes during Electrochemical Testing
Authors: Kerber Brian M , Garg Shipra , Hennek Matthew , Usrey Monica Lee , Sriramulu Suresh 
Published: December 2024

Many mechanisms and degradation pathways have been identified in the literature that result in leaching of transition metals from the cathode, resulting in loss of capacity during cycle life testing due to fewer sites for lithium intercalation into the cathode during discharge1. But electrode formulations contain more components than just active material- there are also binders, conductive carbon, other additives, and coatings. The extent to which these other components can break down and cause electrode degradation and any subsequent effects on cell performance is not well known.
This poster explores the chemical and electrochemical influences on extraction of materials from electrodes, such as sodium, that may be harmful to battery performance. Post mortem analyses of electrolytes after electrochemical testing in multilayer pouch cells have found sodium content in the range of 200-300 ppm, well above typical specifications for battery-grade products (1-10 ppm). The most probable source of sodium in the battery is sodium carboxymethyl cellulose (CMC), often used in graphite anodes as a rheology modifier during production. In this study, the leachability of sodium from CMC in various extraction solutions was investigated through model systems. Model system experiments have shown that while the sodium in CMC was insoluble in organic solvents and electrolyte, sodium can be extracted by contact between salt-containing electrolytes and CMC-containing anodes. The amount of sodium recovered in the model system closely corresponds with the amount that was recovered from cells after electrochemical operation. Other anode and cell components were also analyzed as potential sources of sodium, and the prospect of each of these as a source of sodium was explored. Finally, the effect of different levels of sodium content on cell performance was rigorously tested by doping lithium-ion electrolytes with NaPF6 and testing these electrolytes in pouch cells. Overall, we show that sodium can be a major contaminant extracted into the electrolyte during cycling in pouch cells, and investigate the impact of sodium content on critical performance metrics.
1 Ochida, M.; Domi, Y.; Doi, T.; Tsubouchi, S.; Nakagawa, H.; Yamanaka, T.; Abe, T.; Ogumi, Z. Influence of Manganese Dissolution on the Degradation of Surface Films on Edge Plane Graphite Negative-Electrodes in Lithium-Ion Batteries. Journal of the Electrochemical Society 2012, 159(7), A961-A966.