bluuebunny/crossref_metadata_2025_split huggingface dataset:
Toward High-Throughput Surface-Sensitive X-Ray Scattering Studies of Electrochemical Interfaces
Authors: Matar Toka , Corts Wieland , Steinruck Hans-Georg 
Published: August 2024

Lithium-ion batteries (LIBs) are widely recognised as essential parts of portable electronics, electric vehicles, and grid storage. As such, LIBs have considerable potential to contribute to our modern society, especially as a fundamental component in the development of a sustainable energy system [1]. Despite their success, many fundamental questions in the context of LIBs still puzzle researchers today. These involve interfaces and interphases [2]. For example, the structure and speciation of the potential- and surface-dependent electric double layer (EDL) (especially in advanced concentrated electrolytes) is currently not well understood. Relatedly, basic knowledge of multiple properties of the solid electrolyte interphase (SEI), a passivation layer formed on anode surfaces by electrolyte reduction products, needs to be unravelled to predict electrolyte behaviour as well as cell kinetics and lifetime [3].
To understand the structural properties of these solid-liquid interfaces and interphases, X-ray reflectivity (XRR) is a powerful method that employs model electrodes such as single crystals or thin films [4,5]. XRR provides surface sensitivity with sub-Ångström resolution, is non-destructive, allows probing buried nanoscale layers, and, importantly, can be carried out in operando modality [3]. One of the main challenges of XRR is that it is typically employed for a single electrochemical cell at a given time, and a single experiment takes on the order of several hours up to one day. In this scenario, the experiments are not photon-limited and continuous data collection is not necessary to obtain meaningful results because changes are slow towards later stages of the experiment (even though initial processes occur relatively fast). To overcome this limitation, we designed a high-throughput setup and corresponding experimental workflow, in which up to ten electrochemical cells can be measured via XRR and other surface-sensitive X-ray scattering methods (e.g., GISAXS and GIWAXS) quasi-simultaneously in an interleave fashion. We will present our novel experimental setup and first results.
Literature:
[1] G. Zubi, R. Dufo-López, M. Carvalho, & G. Pasaoglu,Renewable and Sustainable Energy Reviews, 89, 292-308, 2018.
[2] K. Xu, Journal of Power Sources, 559, 232652, 2023.
[3] C. Cao, H.-G. Steinrück, Encyclopedia of Solid-Liquid Interfaces, 391–416, Elsevier, 2024.
[4] T. T. Fister, X. Hu, J. Esbenshade, ... & P. Fenter, Chemistry of Materials, 28(1), 47-54, 2016.
[5] C. Cao, H.-G. Steinrück, B. Shyam, K. H. Stone, & M. F. Toney, Nano Letters, 16(12), 7394-7401, 2016.
Advancements in Dry Coating for Battery Electrodes: Scalable Extrusion Mixing for Control of Electrode Microstructure and Electrochemical Performance
Authors: Quérel Edouard , Dolder Valentin , Stössel Philipp , Hänsel Christian , Spillmann Adrian , Battaglia Corsin 
Published: August 2024

Dry coating of battery electrodes is emerging as a promising alternative technology to the prevailing slurry coating and drying process widely adopted in the lithium-ion battery industry.1,2,3 To date, the most energy-intensive step in cell manufacturing is the drying of slurry-coated electrodes,1 and the adoption of dry coating aims to mitigate both the environmental impact and production costs associated with electrode production. Beyond environmental and economic concerns, producing higher mass-loading electrodes, a crucial aspect for increasing cell energy density, faces inherent challenges with the slurry-coating process: the drying of thick coatings often leads to issues such as electrode cracking and the formation of inhomogeneous electrode microstructures.
Bühler and Empa have collaboratively developed and are in the process of scaling up a dry-coating manufacturing method.4 Our process centers around the extrusion mixing of electrode components, followed by calendering of the dry mixture to produce the final electrode and direct lamination onto a current collector. In this presentation, we showcase the adaptability of extrusion mixing in inducing shear fibrillation of polytetrafluoroethylene (PTFE) binder, crucial for achieving the desired electrode microstructures (see Figure 1a and 1b). Furthermore, we demonstrate the capability of our dry-coating technology to produce high-mass loading electrodes with areal capacities of 5 mAh cm-2 or more (see Figure 1c).
The presentation encompasses a thorough characterization of dry-coated electrodes, including their microstructure and electrochemical performance in lab-scale batteries. Key aspects, such as rate capability and capacity retention, are evaluated. A comprehensive comparison with slurry-coated electrodes, fabricated using identical active electrode materials, mass fractions, and mass loading, reveals that our dry-coated electrodes exhibit comparable performance to their slurry-coated counterparts.5 The scalability of our dry-coating technology is underscored, highlighting the achievable throughputs necessary for gigafactory-scale production with a single extruder.
References:

1 F. Degen, M. Schütte, Journal of Cleaner Production, 2022, 330, 129798

2 B. Schumm, S. Kaskel, Next Energy, 2023, 100009

3 Y. Lu, C.Z. Zhao, H. Yuan, J.K. Hu, J.Q. Huang, Q. Zhang, Matter, 2022, 5, 876–898

4 InnoSuisse Flagship project CircuBat

5 E. Quérel, V. Dolder, C. Hänsel, P. Stössel, C. Battaglia, in preparation

Figure 1
Scalable Synthesis of Single Crystal Ni-Rich Cathodes for Advanced Lithium-Ion Batteries
Authors: Bi Yujing , Xu Yaobin , Wang Chongmin , Xiao Jie 
Published: August 2024

Long-range electrical vehicles require high energy density lithium-ion batteries that utilize stable, high-energy cathode materials. Among various cathodes, Ni-rich NMC cathodes with a layered structure, knows for their high capacity, high voltage, and cost-effectiveness, stand out as one of the most promising cathodes. Traditional polycrystalline Ni-rich NMC encounter issues such as pulverization, gas generation and moisture sensitivity, limiting their widespread use in EV batteries on large scale. The single crystal format of Ni-rich cathode can effectively eliminate and mitigate these issues. However, synthesizing of high-performance single crystal Ni rich NMC, especially when Ni ≥0.8, presents a significant challenge.
We’ve explored an innovative phase separation approach for direct synthesis of high-performance single crystal NMC811. The comprehensive investigation into the reaction mechanism of single crystal growth was conducted to understand the relationship between synthesis, morphology, and performance in growing single crystal NMC811. The enhanced performance of these materials was realized through the precise morphological and structural control of precursors and has been confirmed in practical 2Ah pouch cells. The developed approach is readily adaptable to current industry manufacturing processes and provides valuable new insights that can be broadly applied to cost-efficient large-scale synthesis of single crystals and various advanced battery materials technologies.
Characterization and Analysis of Coal-Derived Graphite for Lithium-Ion Batteries
Authors: Paul Abigail , Magee Regan , Wilczewski Warren , Wichert Nathan , Gula Caleb , Olson Rudolph , Shereda Eric , Lowe Jeffrey , Al-Majali Yahya , Trembly Jason , Wolfe Kody D , Staser John A. , Garrick Taylor R. 
Published: August 2024

Graphite is a critical material used as the negative electrode in lithium-ion batteries. Both natural and synthetic graphites are utilized, with the latter obtained from a range of carbon raw materials. In this work, efforts to synthesize graphite from coal as a domestic feedstock for synthetic graphite are reported. The performance in lithium-ion coin cells of this coal derived graphite is compared to commercial battery-grade graphite. This includes characterization of the thermodynamics of the coal derived graphite using the multi-species, multi-reaction (MSMR) model, characterization of the entropy and enthalpy of the material, and estimation of the rate capability. This enables modeling of synthetic coal-derived graphites and virtual evaluation[1] of these materials towards electric vehicle and grid storage applications.
References
1. T. R. Garrick, Y. Zeng, J. B. Siegel, and V. R. Subramanian, "From Atoms to Wheels: The Role of Multi-Scale Modeling in the Future of Transportation Electrification." Journal of The Electrochemical Society 170.11 (2023): 113502.
Sustainable Modification of Naturally Available Resources for Metal-Ion Storage Applications
Authors: Kamali Ali Reza 
Published: August 2024

The adoption of naturally abundant resources for energy storage applications represents a pivotal strategy in advancing large-scale sustainable green energy solutions across diverse sectors. This presentation provides an overview of E2MC's approaches to the green modification of naturally occurring materials at a low cost, focusing on their metal-ion energy storage capabilities. Key natural materials discussed include molybdenum disulfides (MoS2), ilmenite and natural graphite minerals, as well as corn waste. (a) The thermal oxidation of MoS2 is explored as a straightforward and effective method to produce layer-structured molybdenum trioxide (α-MoO3) with crystalline defects, showing enhanced Li-ion storage kinetics. The molten salt treatment of MoS2 produces sodium dimolybdate with improved Li-ion and Na-ion storage performances. Additionally, a hybrid nanostructure comprising metastable monoclinic molybdenum trioxide (β-MoO3), hexagonal MoS2 secondary crystals and graphene nanosheets is produced through mechanochemical-molten salt treatment. This hybrid structure exhibits an interesting Li-ion storage performance. (b) Carbonization of largely available corn lignocellulosic waste in the presence of molten salt is discussed as a facile approach for the preparation of biocarbons with appropriate specific surface area, pore volume, and elemental carbon purity. The partial dissolution of biomass impurities into the molten salt enhances the Li-ion and Na-ion storage performance of the biocarbon. Additionally, the treatment of corn-derived silica with Fe2O3 and graphite-derived graphene nanosheets, leads to the preparation of a nanostructure in which ferric oxide particles are coated with iron silicate, and these hybrid nanostructures are integrated with graphene nanosheets, showcasing an interesting Li-ion storage performance. (c) Efficient exfoliation of naturally available graphite minerals in molten salt is introduced leading to the formation of carbon nanostructures with promising applications in both Li-ion and Na-ion storage. The economic and strategic advantages associated with utilizing such naturally available resources for energy storage applications are also discussed.

References

W. Zhu, A.R. Kamali*, J. Alloy Compd. 932 (2023) 167724
W. Zhu, A.R. Kamali*, J Alloy Compd. 968 (2023) 171823
A.R. Kamali*, H. Zhao, J. Alloy Compd. 949 (2023) 169819
W. Zhu, A.R. Kamali*, J. Alloy Compd. 831(2020) 154781
H. Zhao, A. Rezaei, A.R. Kamali*, J. Electrochem. Soc. 169 (2022) 054512
A.R. Kamali*, J. Ye, Miner. Eng. 172 (2021) 107175
S. Li, A.R. Kamali*, Chem. Eng. Sci. 265 (2023) 118222
S. Li, A.R. Kamali*, Gels 9 (2023) 701
S. Li, A.R. Kamali*, Colloids Surf. A 656 (2023) 130275
H. Fu, A.R. Kamali* et al, Chem. Eng. J. (2023) 146936
W. Zhu, A.R. Kamali*, J. Electrochem. Soc. 168 (2021) 046517
Fabrication of 60μm-Thick Free-Standing Bilayer Solid Electrolytes for Solid-State Batteries Using Solution Processing and Lamination
Authors: Kim Younggyu , Juarez Yescaz Carlos , Liao Daniel W. , Jangid Manoj K. , Joshi Prerna , Yang Heng , Zahiri Beniamin , Braun Paul V. , Dasgupta Neil P. 
Published: August 2024

Development of solid-state batteries with a high voltage cathode and lithium metal anode could enable high energy density while avoiding safety issues of flammable liquid electrolytes. However, the solid electrolyte (SE) should meet multiple requirements, including 1) electrochemical stability at both the cathode and anode side interfaces, 2) small thickness (tens of μm) to maximize energy density of the cell, and 3) fabrication with a scalable manufacturing method. Using bilayer SEs with different electrochemical stability windows could enable stability at both cathode|SE and anode|SE interfaces. In this work, we developed a manufacturing process to fabricate thin (60 μm) free-standing bilayer SE films from slurry casting and lamination, which can be used for large scale manufacturing of SSBs.
Halide SE (Li3InCl6) and sulfide SE (Li6PS5Cl) were slurry casted on different substrates, and then were dried in vacuum before being laminated onto each other to make a free-standing bilayer film. The parallel slurry casting approach eliminates cross-compatibility requirements of the solvents used for slurry preparation. The resulting bilayer films after densification were pin-hole free without intermixing between the two phases. The ionic conductivity of the bilayer SE film was ~70% of the bilayer SE pellet (1 mm thickness in total) made with a conventional powder pressing method. However, because the thickness of bilayer SE film (60 μm) was much smaller than the bilayer SE pellet (1 mm), the bilayer SE film had ~10x lower area-specific resistance (ASR) compared to the bilayer SE pellet. Because of the lower total cell resistance, the cell made with the bilayer SE film had a better rate capability compared to the reference cell in pellet geometry.
The strategy developed in this work could be integrated into current manufacturing infrastructure of battery fabrication as it is based on slurry casting, which is already a well-established fabrication method for lithium-ion batteries. Moreover, it could be used to fabricate multi-layered solid-state architectures in general, which are challenging to manufacture due to solvent compatibility issues during slurry casting. The study will assist the progress of solid-state battery manufacturing by providing a scalable manufacture method to prepare thin free-standing bilayer SEs.
Bridging the Gap: Unraveling the Mechanisms of Nanobubble Detachment from Electrode Surfaces
Authors: Aydin Fikret , Gemeda Hawi Bacha , Yu Henry , Lin Tiras Y , Davis Jonathan T. , Kang Shinyoung 
Published: August 2024

Gas evolution reactions play a fundamental role in the functionality of various electrochemical devices. Recent experimental studies have provided valuable insights into the behavior of gas bubble formation on nanoelectrodes; however, the experiments have limited spatial resolution to fully understand the underlying mechanisms governing the formation of nanobubbles and their stability on the surface as well as the effects of nanoscopic surface defects on their behavior. A comprehensive understanding of how bubbles behave on electrode surfaces and in the electrolyte is essential for optimizing and designing electrochemical processes. In this work, we employ all-atom molecular simulations to explore the effects of surface chemistry and defect geometry on detachment behavior of hydrogen gas bubbles on nickel electrodes at molecular level. Analyzing the dynamics of bubble detachment on the surfaces with different chemistries reveals that the rate of bubble detachment is higher on the strongly hydrophilic surface compared to the surface exhibiting weak hydrophilicity. In addition, our findings indicate that the defect geometry has significant effects on the detachment of bubbles from the surface. Specifically, the width and depth of canonical-shaped defects are demonstrated to be critical parameters affecting the behavior of the hydrogen bubbles on the nickel surface. Overall, our results show there is a complex balance between the degree of surface wettability and surface defects, determining the stability of nanobubble formation on the electrode surfaces. The results of this study could enhance our understanding of bubble detachment dynamics on the electrode surfaces, providing valuable insights for the future design of practical applications.
This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC5207NA27344. Release: LLNL-ABS-858292
Development of Thin-Film Nanoporous Ruthenium Electrocatalysts Using Atom Probe Tomography
Authors: Hatipoglu Ezgi , Saksena Aparna , Schneider Jochen , Gault Baptiste , El-Zoka Ayman A. 
Published: August 2024

Dealloying corrosion has been used to create high surface area nanoporous metals with promising catalytic properties towards alkaline water electrolysis [1], [2]. The selective dissolution of the less-noble metal from a solid-solution alloy results in a 3D open-pore, nanostructured substrate which is chemically rich in the more noble metal. Ruthenium, the cheapest Pt-group metal [3], has desirable catalytic properties for the hydrogen evolution reaction, however making nanoporous ruthenium (NPR) substrates by dealloying has been challenging due to its limited miscibility with Ag and Cu, compared to the more widely studied Au. Hence, the potential improvement of Ru catalytic properties through dealloying Ru-based systems remains unexplored
In this study, we use magnetron sputtering to make metastable, single-phase, Ag-Ru thin films, with the aim of electrochemically dealloying them to create uniformly NPR substrates. The impact of thin-film structures and chemistry on subsequent dealloying behaviors were investigated by integrating electrochemical measurements with high-resolution characterization techniques including atom probe tomography (APT), electron backscatter diffraction (EBSD), and scanning electron microscopy (SEM). Furthermore, we correlate the thin-film properties studied with the structure and chemistry of NPR formed during dealloying. Amongst the valuable insights attained, we reveal atomic-scale compositional fluctuations in as-deposited non-equilibrium Ag-Ru, that impact the nanoligament compositions in dealloyed nanoporous ruthenium. Finally, the electrocatalytic performance of different NPR substrates are reported for hydrogen evolution reaction. Thereby, advancing the development of novel Ru-based nanoporous electrocatalysts and outlining pathways for future guided optimization.
[1] Erlebacher, J., Newman, C. & Sieradzki, K. Fundamental physics and chemistry of nanoporosity evolution during dealloying. RSC Nanosci. Nanotechnol. 11–29 (2012). doi:10.1039/9781849735285-00011
[2] J. Tian et al., “Dealloying of an amorphous TiCuRu alloy results in a nanostructured electrocatalyst for hydrogen evolution reaction,” Carbon Energy, vol. 5, no. 8, Aug. 2023, doi: 10.1002/cey2.322.
[3] Johnson Matthey Inspiring science, enhancing life. Available at: https://matthey.com/products-and-markets/pgms-and-circularity/pgm-management (Accessed: 18 December 2023).
Leaded Bronze Foams As Innovative Electrodes for Organic Electrosynthesis
Authors: Gálvez-Vázquez María de Jesús , Moreno Garcia Pavel , Prenzel Tobias , Winter Johannes , Gálvez-Vázquez Liliana , Broekmann Peter , Waldvogel Siegfried R 
Published: August 2024

The electrification of organic synthesis represents an outstanding green alternative to prepare valuable and fine chemicals. However, the design of electrode materials for organic electrosynthesis remains as an open field to investigate. Motivated by the superior performance of leaded bronzes as electrodes for reductive transformations,[1, 2, 3] we have developed highly porous binary and ternary leaded metal foams through the dynamic hydrogen bubble template method [4] and tested them as cathodes in the electro-organic synthesis of 2,6-dichlorobenzonitrile from 2,6-dichlorobenzaldoxime.[5]
The electrocatalytic performance of the novel leaded foams was compared to the one of the planar CuSn7Pb15 leaded bronze. The novel porous leaded foams outperformed the CuSn7Pb15 electrodes in terms of chemical yield and energy efficiency. Furthermore, due to their highly crystalline surface, these materials are mechanically more stable and less prone to cathodic corrosion than flat Pb and CuSn7Pb15 electrodes.
References:
1) C. Gütz, V. Grimaudo, M. Holtkamp, M. Hartmer, J. Werra, L. Frensemeier, A. Kehl, U. Karst, P. Broekmann, S. R. Waldvogel, ChemElectroChem 2018, 5, 247.
2) T.Wirtanen, E. Rodrigo, S. R.Waldvogel, Chem. - Eur. J. 2020, 26, 5592.
3) C. Gütz, M. Selt, M. Bänziger, C. Bucher, C. Römelt, N. Hecken, F. Gallou, T. R. Galvão, S. R. Waldvogel, Chem. - Eur. J. 2015, 21, 13878.
4) S. Vesztergom, A. Dutta, M. Rahaman, K. Kiran, I. Zelocualtecatl Montiel, P. Broekmann, ChemCatChem 2021, 13, 1039.
5) P. Moreno-García, M. de J. Gálvez-Vázquez, T. Prenzel, J. Winter, L. Gálvez-Vázquez, P. Broekmann, S. R. Waldvogel, Self-Standing Metal Foam Catalysts for Cathodic Electro-Organic Synthesis, Adv. Mater. 2024, 36, 2307461.

Figure 1
Preliminary Electrochemical Analysis of Carbon Nanoparticles from Candle Soot
Authors: Lubanjar Binita , Avila-Gutierrez Mario , Trinh Minh Quang , Corona-Elizarraras Luis , Jaisi Shankar , Alpuche-Aviles Mario A. 
Published: August 2024

Nanoparticles (NPs) generated by candle soot are of interest due to their potential applications. Because of their electronic properties, carbon-based zero-dimensional, one-dimensional, and two-dimensional nanomaterials such as graphene, fullerene, carbon nanotubes, and carbon nanofibers are extensively studied (1).However, synthesis of these nanomaterials is complex and expensive. Candle soot also contains fluorescent carbon NPswhich can be used for the preparation of fluorescent makers (2). The potential applications of candle soot NPs include energy storage [e.g., can be used for supercapacitor electrode material (3)], and conversion [fuel cells (4)]. Candle soot can be an excellent source of carbon NPs. In this presentation, we cover some challenges associated with carbon NPs, such as (a) instability of NPs due to agglomeration with time and increase in temperature and (b) separation and isolation of NPs. Thus, we focus on stabilization of NPs, isolation and characterization of NPs and to study electronic, optical, and electrochemical properties to determine whether they are promising candidate in the field of energy conversion.
Candle soot formation depends on various parameters like substrate material, deposition time, flame temperature, wick dimension, and flame height (5). We developed a protocol for the collection of candle soot. With this proposed protocol, the carbon NPs generated from candle soot ranges from 50 nm to larger particle size which is confirmed by dynamic light scattering (DLS) technique shown in Fig. 1, and transmission electron microscope (TEM). We will include the electrochemical analysis such as investigation of oxidation/reduction processes to determine fundamental thermodynamic parameters of standard potential in organic solvents and aqueous solutions.

References

Jariwala, V.K. Sangwan, L.J. Lauhan, T.J. Marks, M.C. Harsam, Carbon nanomaterials for electronics, optoelectronics, photovoltaics, and sensing, Chem. Soc. Rev., 43 (2013), 2824-28.

J. Campbell, M.J. Andrews, K.J. Stevenson, New nanotech from an ancient material: Chemistry demonstrations involving carbon-based soot, J. Chem. Educ., 89 (2012) 1280-1287.

Zhang, D. Wang, B. Yu, F. Zhou, W. Liu, Candle soot as a supercapacitor electrode material, RSC. Adv., 4 (2014), 2586-2589.

Khalakhan, R. Fiala, J. Laukova, P. Kus, A. Ostroverkh, M. Vaclavu, M. Vorokhta, I. Matolinova, V. Matolin., Candle Soot as an efficient support for proton exchange membrane fuel cell catalyst, Fuel Cell., 16 (2016) 652-655.

N. Sahoo, B. kandasubramanian. An experimental design for the investigation of water repellent property of candle soot particles, Mater. Chem. Phys.,148 (2014), 134-142.

Figure 1