bluuebunny/crossref_metadata_2025_split huggingface dataset:
Multilayer Porous Transport Layers for Polymer Electrolyte Water Electrolysis to Replace Thin Protective Pt Coating at Low IrO2 Loading
Authors: Turtayeva Zarina , Weber Carl Cesar , Herranz Juan , Buechi Felix N. 
Published: December 2024

The use of expensive PGM catalysts for the OER and HER leads to high production costs of Polymer electrolyte water electrolysis (PEWE). Moving towards lower iridium oxide (IrOx) catalyst loadings for the anode side can severely affect performance and stability [1]. Recent studies revealed that the structure of the interface between the anodic porous transport layer (PTL) and the catalyst layer (CL) is a crucial factor limiting cell efficiency and contributes significantly to the performance and use of the CL. The coarse structure PTL can develop inactive zones of the catalyst layer, which happens when the catalyst layer is not “close” to the connecting titanium structure [2]. The situation becomes worse when the IrO2 catalyst loading is reduced, and the catalyst layers become thinner. Recent evidence has shown that having additional Microporous layers (MPL) can overcome some of these issues by maximizing catalyst utilization and increasing cell efficiency. However, at low Ir loadings, a thin protective Pt coating on MPL is needed to avoid formation of TiOx passivation layer on the MPL surface and increase surface conductivity [3].
In this work, we attempt to replace the thin protective Pt coating by adding an additional layer of Ti or TiN on the existing MPL aiming when using low loadings of IrO2 (0.5 – 0.1 mgIr cm-2). Vacuum plasma spraying (VPS) technology was used to apply TiN on the surface of MPL, while Ti was spray-coated, and vacuum sintered to create a hierarchically structured 3-layer PTL. Electrochemical performances of both Ti and TiN coated MPLs were evaluated by polarization curves and Electrochemical Impedance Spectroscopy measurements. The results are compared with a Pt coated MPL reference.
References:
[1] M. Yasutake, D. Kawachino, Z. Noda, al -, E.M. Bernt, C. Schramm, J. Schröter, S.M. Alia, K.S. Reeves, J.S. Baxter, Analysis of Voltage Losses in PEM Water Electrolyzers with Low Platinum Group Metal Loadings, J. Electrochem. Soc. 165 (2018) F305. https://doi.org/10.1149/2.0641805JES.
[2] T. Schuler, J.M. Ciccone, B. Krentscher, F. Marone, C. Peter, T.J. Schmidt, F.N. Büchi, Hierarchically Structured Porous Transport Layers for Polymer Electrolyte Water Electrolysis, Adv. Energy Mater. 10 (2020) 1–12. https://doi.org/10.1002/aenm.201903216.
[3] C.C. Weber, S. De Angelis, R. Meinert, C. Appel, M. Holler, M. Guizar-Sicairos, L. Gubler, F.N. Büchi, Microporous transport layers facilitating low iridium loadings in polymer electrolyte water electrolysis, EES Catal. 2 (2024) 585–602. https://doi.org/10.1039/d3ey00279a.
Techno-Economic Analyses on Electric Ship By NH3 Fueled Solid Oxide Fuel Cells
Authors: Horita Teruhisa , Bagarinao Katherine Develos , Kishimoto Haruo , Matsui Toshiaki , Muroyama Hiroki , Kakinuma Yasuo , Sumi Hiroshi , Adam Paul , Rothe Stefan , Megel Stefan , Kusnezoff Mihails , Hartmann Mark , von Einstedel Julius 
Published: December 2024

We have been conducting an international collaboration study on “Green ammonia synthesis and utilization by solid electrolysis cells for maritime application” between Germany and Japan (term 2022-2024) under the SICORP program of the Japan Science and Technology Agency (JST). The contributors of this project are AIST, Kyoto University, and Morimura SOFC Technology from the Japanese side and Fraunhofer IKTS and EDL from the German side.
The purpose of this project is to establish a new concept for an energy loop based on ammonia synthesis and utilization with maritime applications. One of the work packages of this project is to evaluate the feasibility of electric ships by using Solid Oxide Fuel Cells (SOFCs) with ammonia fuels. The important point of this project is to give a concept for such NH3-fuel SOFC ships based on techno-economic evaluation.
As a preliminary evaluation of this concept, we have started the feasibility study on the SOFC system based on the literature data so far. A 200 kW SOFC system is considered for a small boat (less than 100 ton class) with an NH3 tank. Const evaluation and technical barriers are presented, and the technical target will be presented to achieve the realization of such a ship.

Figure 1
Insights into Crystallography and Electrochemical Performance of Doped Li-Rich Layered Oxides for Lithium-Ion Batteries
Authors: Celeste Arcangelo , Silvestri Laura , Brutti Sergio 
Published: December 2024

The development of new materials is imperative to meet the growing demand for systems delivering higher capacity, energy density, cycle life stability, and safety. Lithium-Rich Layered Oxides (LRLOs) are at the forefront of enabling high-capacity and high energy density positive electrodes for Lithium-Ion Batteries, addressing the challenges of green and safe transportation and sustainable stationary energy storage from renewable sources [1]. LRLOs, with the general formula Li1+xTM1-xO2 (where TM represents a blend of transition metals such as Mn, Co, Ni...), belong to the layered material family but their crystal structure remains elusive [2]. On the other hand, they exhibit excellent reversible performance in aprotic lithium-metal and lithium-ion batteries over numerous charge/discharge cycles. Their higher specific capacity compared to commercial cathodes can be attributed to cumulative cationic and anionic redox processes, wherein anionic redox reactions involve lattice oxygen, balancing lithium extraction with the activation of the O2-/O- redox couple. However, inadequate cycle life stability and capacity retention hinder their commercial adoption, owing to structural rearrangements and phase transitions upon cycling. Moreover, reducing costs and toxicity of raw materials such as cobalt is crucial for large-scale production [3].
In this communication, we elucidate the significant influence of extensive defectivity on the description of LRLOs crystal structure. Specifically, we illustrate how the utilization of supercells or defects (antisite defects, stacking faults ...) contribute to a more accurate structural description. Additionally, doping strategies were used to enhance the electrochemical behavior and mitigate the structural rearrangements. Our findings showcase optimized layered materials boasting exceptional electrochemical performance, enhanced environmental compatibility, and reduced manufacturing costs relative to the current state-of-the-art.

References

[1] S. Zhao, Z. Guo, K. Yan, S. Wan, F. He, B. Sun, G. Wang, Energy Storage Mater
2021, 34, 716–734.
[2] A. Celeste, M. Tuccillo, A. S. Menon, W. Brant, D. Brandell, V. Pellegrini, R. Brescia, L. Silvestri, S. Brutti, Small Methods
2024, DOI 10.1002/smtd.202301466.
[3] A. Celeste, F. Girardi, L. Gigli, V. Pellegrini, L. Silvestri, S. Brutti, Electrochim Acta
2022, 428, DOI 10.1016/j.electacta.2022.140737.
Nearly All-Active-Material Disordered Rock-Salt Cathodes for Ni- and Co-Free Li-Ion Batteries
Authors: Lee Jinhyuk , Seo Dong-Hwa , Lee Eunryeol , Lee Dae-Hyung 
Published: December 2024

The global shift towards electric vehicles and large-scale energy storage systems necessitates cost-effective and abundant alternatives to commercial Co/Ni-based cathodes, such as LiNi0.6Mn0.2Co0.2O2, for Li-ion batteries (LIBs). Manganese-based disordered rock-salts (Mn-DRXs) have shown promising potential to outperform conventional cathodes at a lower cost, achieving energy densities exceeding 900 Wh kg-AM (per active material, AM).[1-4] However, previous demonstrations of such performance have been conducted in cell constructions that are far from commercially viable, utilizing diluted electrode films (∼70 wt%-AM) containing excessive carbon and binder.[3]

In this presentation, I will address the challenges associated with attaining AM-concentrated Mn-DRX cathodes (>95 wt%-AM).[5] It will be revealed that the failures observed in AM-concentrated electrodes of Mn-DRXs stem from their remarkably low electrical conductivity (ranging from 10−10 to 10−8 S/cm) and the subsequent collapse of the electrode's electrical network due to volume changes over cycling. I will then outline strategies to mitigate these challenges through electrical percolation engineering and the enhancement of electrode mechanical properties. Through these approaches, we have successfully demonstrated nearly all-AM Mn-DRX cathodes (∼96 wt%-AM) and achieved the highest application-level energy density (∼1050 Wh kg-cathode) reported to date.[5]

Furthermore, I will discuss the trade-off associated with the manganese content in Mn-DRXs concerning their electrical conductivity and volume change behavior. This discussion will provide valuable insights and guidelines for material design aimed at advancing Co/Ni-free LIBs' technology readiness.
Overall, this presentation will shed light on the current status, challenges, and breakthroughs in the development of Mn-DRX cathodes, offering a pathway towards more efficient and sustainable LIB technology.

References

J. Lee et al., Science 343, 519−522 (2014).

J. Lee et al., Nature 556, 185–190 (2018).

H. Li, R. Fong, D.-H. Seo, J. Lee et al., Joule 6, 53–91 (2022).

E. Lee, H. Lee, J. Lee, D.-H. Seo et al., Adv. Mater. 35, 2208423 (2023).

E. Lee, D.-H. Lee, D.-H. Seo, J. Lee et al., Energy Environ. Sci. (2024) https://doi.org/10.1039/D4EE00551A.
Comparison of Characterization of High Nickel Single Crystal Cathode Materials According to Pre-Heating and Reheating Temperature
Authors: Yun Ye Ji , Sung Ye Jin , OH Eun-Suok 
Published: December 2024

A high-nickel cathode with high reversibility Li[NixCoyMn1–x-y]O2 (x ≥ 0.6) is one of the most commonly used cathode materials in lithium-ion batteries. However, as the nickel content increases, the instability of the layered structure of the cathode increases, which adversely affects the life performance. In addition, such a high-nickel polycrystalline cathode material causes cracks in particles during pressing or charging and discharging, ultimately leading to the deterioration of cycle performance. To solve this problem, a single crystal cathode material synthesized at 900 Celsius degrees or higher has been proposed. However, research on specific temperature conditions of a high-nickel single crystal cathode is insufficient. In this study, a method of synthesizing LiNi0.8Co0.1Mn0.1O2 (NCM811) high-nickel single crystal cathode is presented, and the physical characterization and electrochemical performance of the cathode material are compared according to the pre-heating temperatures and the reheating temperatures.
Keywords: Lithium-ion battery, Cathode material, single crystal cathode’s calcination temperature, LiNi0.8Co0.1Mn0.1O2

Figure 1
Rapid Scalable Plasma Processing of Lithium Lanthanum Zirconium Oxide (LLZO) Separators for Solid State Batteries
Authors: Crane Gabriel Badillo , Holmes Sarah , Colburn Thomas William , Barrera Francisco , Cui Yi , Dauskardt Reinhold Horst 
Published: December 2024

Metal oxide based solid state batteries have proven to be a hot topic in the search for next-generation battery materials, with materials such as Lithium Lanthanum Zirconium Oxide (LLZO) taking the spotlight for their promise of improved safety, reduced flammability, and stability against lithium-based anodes. However, there are still outstanding challenges in repeatably creating low-defectivity thin films at thicknesses thin enough to function as effective battery separators, as well as preventing the loss of lithium due to high-temperature sintering. Furthermore, much of the research on the synthesis of such materials uses expensive or lab-scale methods such as spin coating or magnetron sputtering, meaning these syntheses will require significant changes in implementation to allow for the jump to materials production for large-scale applications such as grid scale energy or electric vehicles.
We present here an alternative approach for the synthesis of aLLZO thin films using an ambient pressure, low temperature nitrogen plasma curing to rapidly and repeatably produce lithium-containing metal oxide thin films with negligible loss of lithium. The films are rapidly processed in-line with a sub-5-minute plasma curing step (an order of magnitude improvement over conventional methods) using a dry-air ambient-pressure environment. The multiple energy sources inherent in the plasma, including radical ions, UV light, and heat, allow for a low processing temperature of less than 300°C. We demonstrate that we have obtained a high aLLZO conductivity of 2E-6 S/cm at room temperature, which improves to 1E-3 S/cm at the expected operating temperature for electric vehicles (typically on the order of 95-100°C). XRD and XPS analysis demonstrate a uniformly amorphous phase with the expected elemental stoichiometry, with negligible lithium loss. SEM and AFM analysis show a smooth morphology with <40 nm roughness. This novel synthetic approach opens the door to scalable manufacturing of next generation metal oxide battery separators.
Technological Advances for Temperature-Dependent Operando Electrochemical Liquid Cell Scanning Transmission Electron Microscopy Studies of Energy Materials
Authors: Stephens Katherine Marusak , Yang Yao , Walden Franklin Stampley , Marthe Nelson Luis , Wellborn Patrick Smith , McConnell Jennifer , Damiano John 
Published: December 2024

The study of in situ or operando electrochemistry entails observing electrochemical behavior of samples in environments as close to “real working conditions” as possible. Scanning/transmission electron microscopy (S/TEM) enables researchers to characterize physical behavior on the sub-nanometer scale, but conventional S/TEM techniques require sample imaging and analysis in a high-vacuum environment. Recent advances in sample holder technology for S/TEM – specifically, the introduction of closed-cell S/TEM holders and the development of MEMS-based sample supports – have overcome this limitation. Closed-cell holders allow researchers to study their electrochemical systems in liquid, including the option to flow or exchange electrolyte across the sample, by hermetically sealing the experiment from the high-vacuum environment of the S/TEM column. MEMS-based sample supports with integrated electrodes, thin membrane windows, and controlled flow of electrolyte allow researchers to apply electrical stimuli while imaging. Together, these technologies allow the direct observation of processes at the nanoscale that influence material performance, such as the formation of the solid electrolyte interphase (SEI) layer during lithium-ion battery cycling [1], the preferential corrosion of stainless steel at sulfite [2] and silicate [3] inclusions, and the dynamic evolution of shape-controlled nanocrystals for CO2 reduction [4-6]. Understanding the structure-function relationship of these materials at the nanoscale facilitates the efficient innovation of new materials that are more functional, cost-efficient, and environmentally friendly.
In this presentation, we will share initial results from the next generation of in situ electrochemistry systems, pushing closer to “real working conditions” through advanced temperature control of the electrode-electrolyte interface. Many applications require increased temperatures, including research on fuel cell catalysts and corrosion. We will discuss the kinetics of well-known redox couples (Figure 1a) and of dendrite formation (Figure 1b) as a function of the temperature at the anode surface, the different spectroscopic techniques available when in situ electrochemistry is coupled with electron microscopy, and the implications of this new technology to research across numerous application fields including fuel cells, ionic liquids, batteries, corrosion, and electrocatalysis.
[1] W. Dachraoui, et al.
ACS Nano
2023
17(20), 20434-20444
[2] D. Kovalov, et al. Corros. Sci.
2022 199, 110184
[3] M. Tian, et al. Corros. Sci.
2022 208, 110659
[4] Y. Yang, et al.
Nature
2023 614, 262-270
[5] Y. Yang, et al.
J. Am. Chem. Soc.
2022
144(34), 15698-15708
[6] A.M. Abdellah, et al.
Nat. Commun.
2024 15, 938

Figure 1
(Invited) Co-Doping of Tungsten Suboxide for Enhancing the Performance of Flexible Supercapacitors
Authors: Shim Jae-Jin , Thalji Mohammad R , Chong Kwok Feng 
Published: December 2024

A crucial hurdle in developing supercapacitors is the creation of metal oxides with nanoscale structures that possess improved chemically active surfaces, ion/charge transport kinetics, and minimized ion-diffusion pathways. A metal-doping strategy to produce oxygen vacancies and increase electrical conductivity has proven effective for designing high-performance materials for energy storage devices. Herein, cobalt-doped tungsten suboxide (Co-doped W18O49) is grown on carbon cloth (CC) using a solvothermal approach and used as an electrode material for supercapacitor applications for the first time. Through this strategy, structurally distorted W18O49 is obtained by detecting a more apparent amorphous area caused by forming more oxygen vacancies with the bending of the lattice fringes. Benefiting from the synergy of more oxygen vacancies, increased lattice spacing, a high specific surface area, and accelerated ion diffusion, the Co-doped W18O49/CC electrode achieves a specific capacity of 475 C g−
1 (792 F g−
1) at a current density of 1.0 A g−
1, which is superior to that of the undoped W18O49/CC (259 C g−
1, 432 F g−
1) and among the highest reported to date. Interestingly, the asymmetric supercapacitor device assembled using Co-doped W18O49/CC//AC/CC can provide a high energy density of 35.0 Wh kg−
1. This strategy proves that the distortion of the W18O49 structure by Co doping improves the ion storage performance and self-discharge behavior. Also, it can enhance the energy storage performance of other electrode materials.
.

Figure 1
Promoting the Radical-Mediated Pathway and Li₂S Conversion By N-Doped Carbon-Embedded Cobalt-Doped Titanium Nitride Electrocatalyst with High Donor-Number Solvent for Lean Electrolyte Lithium-Sulfur Batteries
Authors: Park Gwan Hyeon , KIM Minho , Kang Song Kyu , Ji Junhyuk , Kim Won Bae 
Published: December 2024

Lithium-sulfur (Li-S) batteries are recognized as some of the most promising candidates for next-generation batteries, owing to their high specific capacity, cost-effectiveness, and lightweight properties. Despite these advantages, the dissolution of the sulfur leads to the shuttling effect of long-chain lithium polysulfides (Li2Sx, 4≤x≤8). Moreover, the lean electrolyte system experiences a reduction in ionic transport due to the formation of ion-pairing and clusters of polysulfides. Therefore, the development of electrolytes that can stabilize the solvation structure of lithium-polysulfide and the introduction of electrocatalysts to suppress the shuttling effect are required for lean electrolyte lithium-sulfur batteries.
High donor-number solvents can stabilize the Li+-solvated structure by effectively shielding the Li+ ion’s effective nuclear charge. This Li+-solvated structure, in coordination with high donor-number solvents, can effectively interact with tri-sulfur radicals and long-chain polysulfides, which possess relatively delocalized negative charges. As a result, a high donicity electrolyte can enhance sulfur utilization by increasing the solubility of polysulfides. However, the poor compatibility of high donor-number solvents with Li metal presents a challenge, making their excessive use impractical. Therefore, optimizing the amount of high donor-number solvent is essential. Through careful optimization, it is possible to achieve high donicity electrolyte conditions that are compatible with Li metal. The 1 vol% N,N-Dimethylacetamide (DMA) in 1,2-dimethoxyethane (DME)/1,3-dioxolane (DOL) co-solvent (DMA:DME:DOL=1:49.5:49.5 vol%) electrolyte achieved a higher discharge capacity after 20 cycles compared to both a low donicity (DME/DOL, 1:1 vol%) and a high donicity (DMA/DOL, 1:1 vol%) electrolyte.
Electrolyte modification alone cannot completely suppress the shuttling effect, as the radical-mediated pathway activated by high donor-number solvent leads to the presence of tri-sulfur radicals. Recent research has investigated the ferromagnetic catalysts to enhance the adsorption of polysulfides through the Lorentz force and facilitate the conversion of Li2S with spin polarization in lithium-sulfur batteries. Introducing ferromagnetism through cobalt-doping into N-doped carbon embedded titanium nitride nanowires electrocatalysts could improve the adsorption of polysulfides and tri-sulfur radicals, as well as their conversion to Li2S and promote radical-mediated pathways with high donor-number solvents in lean electrolyte lithium-sulfur batteries. Consequently, N-doped carbon-embedded cobalt-doped titanium nitride nanowires on separator within the 1 vol% DMA electrolyte achieves a high discharge capacity of 454.8 mA h g−1 after 120 cycles with sulfur loading of 3.6 mg cm−2 and E/S ratio of 10 μL mg−1.
Analysis of the Initiation of Pitting Corrosion in Al Alloys Using Model Specimens Prepared by Spark Plasma Sintering
Authors: Katsuyama Tomoki , Nishimoto Masashi , Muto Izumi 
Published: December 2024

In Al alloys, intermetallic particles (IMPs) play an important role in the initiation of pitting corrosion though the process of growing pit is unclear. IMPs in commercial Al alloys are fine and it is difficult to elucidate the mechanism of pitting corrosion by using the alloys. Therefore, in this study, model specimens were fabricated in which coarse IMPs were dispersed, and analysis of pitting corrosion was conducted by using these specimens.
Pure Al powders were mixed with Pure Fe or Cu powders and then they were sintered. After sintering, they were hot forged, and heat treated. To analyze the corrosion behavior, open circuit potential was measured in 0.1 M NaCl solution adjusted to pH 6.0.
These specimens contained dispersed phases of different colors from the Al matrix phase. In the Cu powders added specimens, the phases were Al2Cu and in the Fe powders added specimens, the phases were Al3Fe. After open circuit potential measurement, in specimens containing Al2Cu, the IMPs turned from grey to black and trench formed around the IMPs. In specimens containing Al3Fe, crystallographic pits occurred.