bluuebunny/crossref_metadata_2025_split huggingface dataset:
Polyimide-Based Composite Separators for Super-Stable Li Metal-Based Batteries
Authors: Kim Patrick Joohyun , Choi Junghyun , Park Min Su , Woo Sujeong 
Published: December 2024

Metallic lithium (Li) has garnered significant interest from battery industries and academia investigating next-generation anodes, due to its excellent properties: high specific capacity (3860 mAh g-1), the most negative potential (close to -3.04 V vs. SHE), and low density. Unfortunately, inherent challenges associated with inhomogeneous Li plating/stripping and poor Coulombic efficiency impede the pragmatic use of Li metal anode for conventional batteries. Moreover, thermal shrinkage of polyolefin separators presents a critical issue when Li metal batteries are subjected to high current levels, leading to an inability of the separators to shield the cell from short-circuits effectively.
The fabrication of polyimide-based composite separators via non-solvent-nduced phase separation (NIPS) is particularly promising for enhancing the electrochemical stability of Li metal batteries. A diversity of functional materials has been examined for the preparation of these composite separators, which have subsequently been assessed in Li metal battery systems. Beyond the development of composite structures, the surface modification of polyimide separators has also been explored to further optimize performance in Li metal batteries. Throughout this talk, we are going to give a talk about our research findings and strategic direction in detail. This presentation would assist many researchers in gaining insights into the design of new battery separators.
Data-Driven Design for Electrolyte Additives Supporting High-Performance Lithium-Ion Batteries
Authors: Liao Chen , Wang Bingning , Doan Hieu , Son Seoung-Bum , Abraham Daniel P. , Trask Stephen E. , Jansen Andrew N. 
Published: December 2024

We presented here two cases of data-driven electrolyte additive design, using two cathodes as examples. In scenario 1, LiNi0.5Mn1.5O4 (LNMO), a spinel-structured material with an average lithiation/de-lithiation potential at ca. 4.6-4.7 V, was used as an example for the extreme high working potentials and the resultant strains on electrolytes. In this study, we first selected and tested a diverse collection of 28 single and dual additives for the LNMO//Gr system using descriptors representative of chemical functionality.(1) Subsequently, we trained and employed machine learning (ML) models to suggest 6 binary compositions out of 125 based on predicted final area specific impedance (ASI), impedance rise (ΔASI), and final specific capacity(Q). Notably, this approach led to the discovery of a new dual additive which outperforms the initial dataset.
In Scenario 2, the AI-guided workflow undergoes further enhancement for accelerated additive optimization employing new data featuring an earth-abundant cathode material of 0.3Li2MnO3·0.7LiMn0.5Ni0.5O2. This phase of the study introduces a more robust machine learning (ML) model for performance prediction, utilizing Figure of Merit Energy (FOME) and Figure of Merit Power (FOMP) as predictive metrics. Following three , Bayesian optimization iterations, 15 out of 78,000 binary and tertiary additive combinations was suggested for experiments, and several novel addtive compositions exhibiting unexpectedly high performance were subsequently identified. The optimal formulation surpasses the current standard by achieving a performance enhancement of 15-19%, as confirmed through experimental testing conducted in coin cells.
Overall, our findings not only underscores the efficacy of ML in identifying new additives combinations, but also introduces an accelerated material discovery workflow that directly integrates data-drive methods with battery testing experiments.
(1) ACS Omega 2018, 3, 7, 7868–7874
The Li-Ion Battery, the Electrification Revolution, and the Next Ideal Battery
Authors: Xu Kang , Hu Qichao 
Published: December 2024

Following Whittingham’s first reversible intercalation electrode (1976) and Goodenough’s identification of oxides as more viable materials (1980), it took more than a decade for the modern lithium-ion batteries (LIBs) to be invented (Asahi Kansai 1986, Sony 1990 and Sanyo 1994). It would take another decade for someone to finally integrate these tiny LIBs into a car (AC Propulsion, 2000) and then verify their commercial viability in mass produced electric vehicles (Tesla, 2004).
Fast forwarding into 2020s, LIB is regarded a strategic technology of national security significance, driven by the compounded forces intertwined with geopolitical animosity, supply chain anxiety as well as climate change concern and responsibility for the environment and future generations. This new complicated scenario, starting about a decade ago but only becoming pronounced in the last 5 years, undoubtedly accelerated the penetration of LIB technology in every aspect of our life, from mobile to transportation to grid-storage, with new application scenarios such as Urban Air Mobility looming over the horizon.
Due to the thermodynamic limits imposed by the intercalation chemistry nature, LIBs cannot meet the expectations of most new applications. The call for a better battery chemistry is never so urgent, and we certainly do not have another four decades to develop such an ideal battery.
In this talk I will discuss the opportunities and challenges of designing the next generation batteries, and highlight the bold and ambitious initiatives of SES in addressing these challenges by leveraging the contemporary AI revolution to explore the large chemical universe.
(Invited) Tracking Lithiation with Advanced Transmission Electron Microscopy
Authors: Su Dong 
Published: December 2024

The primary advantages of Li ion batteries (LIBs) over traditional energy storage devices include high voltage, large capacity and stable cycling ability [1]. Despite their tremendous success in the market of portable devices and electric vehicles, people are developing next generation of batteries for large-scale energy storage or severe working environment, which demands LIBs with better cycling stability, safety and higher energy-density. Investigations on how Li ions transport through the components in a battery, such as anode, cathode, and electrolyte, would be helpful to understand the performances of LIBs, and therefore to realize reversible lithiation/delithiation during cycling.
Transmission electron microscopy (TEM) is an indispensable tool in probing real-space local structures at atomic resolution. Recently, advanced TEM techniques have been applied into tracking the transportation of lithium ions in battery materials [2]. Emerging methods like ABF, e-ABF, iDPC, EELS and ptychography offer possibilities to atomically observe Li ions' occupations, identify their chemical environment, and track the dynamics of their insertion and extraction [3-6]. At present, cryo-TEM technique is a hot spot to study the solid-electrolyte interphase where Li contained organic or inorganic compounds are very beam sensitive [7]. In-situ TEM techniques have unparallel merits to track the migration of lithium ions or see the phase transmission of electrode materials [8-9]. In this talk, we introduce the techniques for direct observation of Li species and their research advances in LIB materials. Perspectives for the current challenges and future development to investigate Li-containing materials are discussed.
References:
[1] A. Manthiram, et al., Nature Energy, 6 (2021) P.323.
[2] X. Lei, et al.,Science China Chemistry, (2023) https://doi.org/10.1007/s11426-022-1486-1
[3] L. Gu, et al.,Journal of the American Chemical Society, 133 (2011) p.4661.
[4] S. Li, et al., Angew. Chem. Int. Ed., 59 (2020) p.22092.
[5] S. Weng, et al., Carbon Energy, 5 (2023) p.e224.
[6] X. Lu, et al., Nano Letters, 12 (2012) p.6192.
[7] X. Wang, et al., Nano Letters, 17 (2017) p.7606.
[8] K. He, et al., Nature Communications, 7 (2016) p.11441.
[9] J. Li, et al., Nature Communications, 10 (2019) p.2224.
[10] This work is supported by National Key Research and Development Program of China Grant [No. 2020YFB2007400], the National Natural Science Foundation of China [No. 22075317], and the Strategic Priority Research Program (B) [No. XDB33030200] of Chinese Academy of Sciences.
Electrode Design and Processing for Enhancing Performance of LiMn0.6Fe0.4PO4 Positive Electrode in Lithium-Ion Batteries
Authors: Go Nan Young , Cho Min Seo , Ryu Ji Heon 
Published: December 2024

Lithium-ion batteries (LIBs) are used in various fields such as electronic devices and electric vehicles. The high energy density of LIBs has traditionally been a significant advantage. However, there is now an increasing demand for enhanced cost-effectiveness and safety. Phosphate-based positive electrode materials have been proposed as alternatives to Ni-based layered oxide materials. However, LiFePO4 is limited by its low operating voltage, leading to decreased energy density, while LiMnPO4 exhibits inadequate electrochemical performance. Consequently, there is increasing anticipation surrounding LMFP (LiMn1-xFexPO4), which leverages the benefits of combining Fe and Mn. LFMP offers the safety advantages of phosphate materials and the cost-effectiveness from the natural abundance of Fe and Mn, further enhanced by the complementary operating voltage and electrochemical activity derived from the Fe-Mn combination.
In this study, we conducted different studies depending on electrode design and manufacturing process in order to improve LiMn0.6Fe0.4PO4 (LMFP64) performance. To comprehend the typical characteristics of the LMFP64 positive electrode, various electrodes with differing compositions and loading levels were fabricated. The physical properties of the fabricated electrode were assessed, alongside the evaluation and comparison of electrochemical properties, including cycle performance and rate capability. Subsequently, modifications to the electrode design were made to incorporate new components or additives with the aim of improving LMFP electrode performance.
The electrode fabrication process was expanded to enhance the electrochemical performance of LMFP. Adjustments to the pore structure with electrode composition led to further performance improvements. Additionally, nano-sized LMFP powder was blended with commonly used micro-sized NCM-based active materials. Although the blending did not exhibit notable synergy, the higher electrode density was achieved than that of the individual electrodes and ensured the required electrode performance based on the properties of both active materials due to the appropriate mixing ratio. Thus, it becomes feasible to configure electrodes that align with user demands in terms of cost and performance, thereby diversifying the battery design.
Operando FTIR Characterization of Interphases from Organosulfur Electrolytes in High Voltage Lithium-Ion Batteries
Authors: Liu Ziqi , Lopez Jeffrey 
Published: December 2024

The widespread adoption of renewable energy storage technologies like electric vehicles and grid storage largely relies on the improvements of the energy density of the batteries inside those devices. Lithium-ion batteries (LIBs) are typically used for these applications due to their high energy density,[1] but the operating voltage of LIBs is limited by the electrochemical stability windows of the electrolyte. Resistive interphase layers form as a result of the breakdown of electrolyte molecules and limit LIB cycling stability. However, there is significant difficulty in the study and characterization of both the components and structure of the electrode-electrolyte interphases formed via electrolyte degradation.[2] Traditional characterization techniques provide information on what the interphase layers look like after cell disassembly, but sample preparations are difficult and destructive.[3] Therefore, it is crucial to develop in operando techniques to better understand the relationship between the interphase layers and battery performance.
In this work, we develop a custom surface-enhanced infrared absorption spectroscopy in the attenuated total reflectance mode (ATR-SEIRAS) setup for in operando studies of the solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in organosulfur electrolyte systems. Organosulfur molecules are potential components for high voltage LIBs due to their excellent performance.[4] We apply our custom ATR-SEIRAS setup to study ethyl methyl sulfone (EMS) containing electrolytes and propose possible reduction routes with the help of ex situ and postmortem characterization techniques. We study both SEI and CEI formed and correlate favorable interphase components with contributing molecules to identify important functional groups for novel molecular design. The work provides an opportunity to elevate our understanding of currently elusive electrochemical phenomena like the structure-reactivity relationships of SEI and CEI, and why certain sulfone systems outperform other formulations. Furthermore, it will provide molecular design principle for electrolyte systems in high performing and high voltage LIBs.
References

S. Chu, Y. Cui, and N. Liu, Nat. Mater., 16, 16–22 (2017).

H. Wan, J. Xu, and C. Wang, Nat. Rev. Chem., 8, 30–44 (2024).

A. Dopilka, Y. Gu, J. M. Larson, V. Zorba, and R. Kostecki, ACS Appl. Mater. Interfaces, 15, 6755–6767 (2023).

M. A. Dato et al., Adv. Energy Mater., 2303794 (2024).
Anode Properties of Si-Based Composite Electrodes Containing Two Silicides with Different Functions for Lithium-Ion Batteries
Authors: Tanaka Ryuto , Domi Yasuhiro , Usui Hiroyuki , Yamaga Takuya , Nishikawa Kei , Sakaguchi Hiroki 
Published: December 2024

A LaSi2/Si composite electrode has longer charge-discharge cycle life than a pure Si electrode. However, the capacity of the composite electrode decreases gradually over repeated cycles. We identified the microstructure of the electrode to ascertain factor of capacity fading by transmission electron microscopy. Before cycling, the pure Si phase was highly dispersed in the LaSi2 matrix phase. In such microstructure, the elastic LaSi2 could alleviate the stress caused by Si volume change during lithiation and delithiation; and hence it suppressed electrode disintegration.1 On the other hand, prior to capacity decline, the positions of LaSi2 and pure Si were reversed. The LaSi2 phase was surrounded by the pure Si matrix phase and the LaSi2 could not relax the stress. Hence, we added stiff silicide which withstands the Si-generated stress into the LaSi2/Si. As a result, the LaSi2/NbSi2/Si exhibited superior cycle life. Herein, we investigated the effect of difference in elastic silicides on cycle life.
The MSi2/CrSi2/Si (M = Ni, La, or Sm) powder was prepared by mechanical alloying method. The composite powder was deposited on the Cu substrate using a gas-deposition (GD) method. The fabricated GD electrode was mounted in a 2032-type coin-cell as the working electrode. Li metal foil and glass fiber filter were also used as the counter electrode and separator, respectively. In addition, we used 1 mol dm–3 lithium bis(fluorosulfonyl)amide dissolved in N-methyl-N-propylpyrrolidinium bis(fluorosulfonyl)amide as an ionic liquid electrolyte. We conducted galvanostatic charge-discharge tests in constant current mode with a charge capacity limitation of 1000 mA h g(Si)–1. In the present study, we did not consider the capacity of the silicides: the Si-alone and silicide-alone electrodes stored Li, while the silicide in the silicide/Si electrodes did not show the reversible capacity2.
Figure 1 shows the cycle life of the MSi2/CrSi2/Si electrodes with the different indentation work rates of MSi2. The indentation work rate means an indicator of elasticity: it indicates that how much the MSi2 layer returns to its original shape after deformation. The cycle life was the shortest when NiSi2 with the lowest indentation work rate was used. In contrast, when SmSi2 was used, it achieved the longest cycle life with high reversible capacity of 1000 mA h g(Si)–1 over 1900 cycles. We predicted that the cycle life improved using a more elastic silicide. However, the cycle life adversely lowered when LaSi2 with the highest elasticity was used. Thus, the excellent performance should be achieved based on the synergistic effects of stiff and elastic silicides.
1) Y. Domi, H. Usui, K. Nishikawa, and H. Sakaguchi, ACS Appl. Nano Mater., 4, 8473 (2021).
2) Y. Domi, H. Usui, K. Nishikawa, H. Sakaguchi, et al., Electrochemistry, 88, 548 (2020).

Figure 1
Enhancement of Electrochemical Properties of Carboxylate-Based Single-Ion Conducting Polymers through Complexation with Ionic Liquids for Lithium-Ion Batteries
Authors: Kim Dongwook , Okada Shizuka , Nakajima Hideto , Inokuchi Daisuke , Yamada Izumi , Hwang Jinkwang , Abe Takeshi , Ouchi Makoto , Matsumoto Kazuhiko , Inui Naoki 
Published: December 2024

[Introduction] Single-ion conducting (SIC) polymers, wherein anions are covalently bonded to the polymer chain, selectively facilitate the movement of lithium ions, making them promising polymer electrolytes for lithium-ion batteries (LIBs) due to their high lithium-ion transference number. However, in the application of highly basic carboxylate-based SIC polymer electrolytes, there is a drawback of difficultly in dissociating Li+ ions. In this study, the complexation with ionic liquids (ILs) was investigated to promote the dissociation of Li+ ions.
[Experiment] The carboxylate-based SIC polymer (MAA-St) was synthesized through a 1:1 radical copolymerization of methacrylic acid derivatives and styrene. A polymer electrolyte was fabricated by compounding the obtained polymer with ILs, and its electrochemical properties were evaluated.
[Results and Discussion] Electrochemical evaluations were conducted on the polymer electrolyte, which was a composite of MAA-St and ILs. In the absence of ILs, the ionic conductivity (σ = 7.13×10–4 mS cm–1 at room temperature) and critical current density (CCD) were extremely low because of the high basicity and difficulty in dissociating Li+ ions. However, the incorporation of ILs led to a significant improvement in electrochemical properties (σ = 7.13×10–4 → 1.98 mS cm–1, critical current density = 0.1 → 2.1 mA cm–2). Furthermore, ionic conductivity and CCD were substantially enhanced with an increase in the quantity of ILs (Figure 1). The addition of ILs weakened the interaction between the SIC polymer and Li ions, facilitating the dissociation of Li ions.
The effect of ionic species of ILs on electrochemical properties was investigated. To examine the dependence on anion species, the cation of the IL was fixed to (N-butyl-N-methylpyrrolidinium: P14
+) and five different anions (PF6, TFSA, FSA, OTf, and N(CN)2) were used for evaluation. As a result, it was observed that the CCD varied significantly according to the donor number (DN) of the anion species. On the other hand, the impact of cation species on CCD was minimal because they interacted with the anionic part of the SIC polymer.
The interaction between SIC polymer and ILs was observed through IR measurements, and the peak of the polymer-derived carbonyl group (C=O) underwent significant changes upon the addition of ILs (1680 cm–1: substantial decrease, 1572 cm–1: red-shift). Additionally, the movement of the anion species of the IL was confirmed by Raman spectroscopy, revealing distinct movements based on the DN of the anion species. Consequently, it became evident that the interaction between SIC polymer and ILs results in the dissociation of Li+ ions and the counteranions.

Figure 1
H-Cell Evaluation of Electrolyte Solvation Energies in the Presence of Silicon Electrodes
Authors: McBrayer Josefine , Schulze Maxwell C. , Rich Chaz , Harrison Katharine L. 
Published: December 2024

Poor calendar life of Li-ion batteries with silicon anodes has been identified as an important obstacle that must be addressed for silicon to be fully commercialized in applications such as electric vehicles. The silicon-electrolyte interface likely plays a key role in calendar life performance since silicon’s reactivity and unstable solid electrolyte interphase (SEI) may lead to increased lithium loss and self discharge. New electrolytes that will better stabilize the SEI are a promising direction to improve calendar life. We hypothesize that the solvation energy of lithium ions in the electrolyte is related to observed lifetimes. Here, we use an H-cell, demonstrated previously as a method to quantify relative solvation energies of Li-ions in promising electrolytes to improve silicon calendar life and compare to performance data. We observe that the solvation energy is dependent on the electrode present, giving further credence to the need to optimize the electrolyte specifically for silicon anodes, accounting for both cycle and calendar life.
Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC (NTESS), a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration (DOE/NNSA) under contract DE-NA0003525. This written work is authored by an employee of NTESS. The employee, not NTESS, owns the right, title and interest in and to the written work and is responsible for its contents. Any subjective views or opinions that might be expressed in the written work do not necessarily represent the views of the U.S. Government. The publisher acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this written work or allow others to do so, for U.S. Government purposes. The DOE will provide public access to results of federally sponsored research in accordance with the DOE Public Access Plan.

Figure 1