bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bicontinuous-Structured Elastomeric Electrolytes for High-Energy Solid-State Lithium-Metal Batteries
Authors: Lee Michael J , Han Junghun , Kim Bumjoon J , Lee Seung Woo 
Published: November 2022

The use of lithium (Li) metal anodes in solid-state batteries is a strong strategy as a next-generation battery technology for surpassing the energy density and safety of conventional Li-ion batteries. However, in practice, current solid-state electrolytes have been limited to realize Li metal batteries due to their insufficient electrochemical and mechanical properties. Here, we design a new class of elastomeric electrolytes having a 3D interconnected plastic-crystal phase within the elastomer matrix—plastic crystal-embedded elastomer electrolytes (PCEEs).1 To elucidate the effects of structural changes in PCEEs on Li-ion transport property, mechanical elasticity, and electrochemical performance, we investigate various phase-separated structures of PCEEs by adjusting each phase’s volume ratio. Among these structures, we reveal that bicontinuous-structured PCEE, consisting of an equal volume ratio of elastomer to plastic-crystal phase, is well-balanced to develop the efficient ion-conducting, plastic-crystal pathways within a mechanically robust, cross-linked elastomer matrix. Hence, this optimal PCEE shows a combination of high ionic conductivity (>10-3 S cm-1) at ambient temperature, high Li-ion transference number (>0.70), and good mechanical resilience (elongation at break ≈ 300%). A full cell configured with the optimized PCEE, a limited Li source, and a high loading LiNi0.83Mn0.6Co1.1O2 cathode delivers a high energy density exceeding 430 Wh kganode+cathode+electrolyte
-1. Understanding the structure-property-electrochemical performance relationship of PCEE through structural control can form the basis of structure-controlled elastomeric electrolytes, holding substantial promise in various electrochemical energy storage systems.
References
1. Lee, M. J.; Han, J.; Lee, K.; Lee, Y. J.; Kim, B. G.; Jung, K.-N; Kim, B. J.; Lee, S. W. Elastomeric electrolytes for high-energy solid-state lithium batteries. Nature
2022, 601, 217-222.
Capacity Fade and Impedance Evolution in Tin Phosphide Anodes for Sodium-Ion Batteries
Authors: L'Antigua Alex , Flannagin Megan , Nelson George J. 
Published: November 2022

Sodium-ion batteries (SIBs) offer a potentially more cost effective and environmentally friendly alternative to Lithium-ion batteries for room temperature high density energy storage. To maintain the benefits of SIBs, earth abundance for all the batteries components is paramount. One promising earth abundant anode material for SIBs is tin phosphide (Sn4P3). Tin phosphides are able to retain a high specific capacity for an extended cycle life. Understanding the changes in electrochemistry within a battery as a result of cycling is crucial in the complete understanding of capacity fade mechanisms and subsequent improvement and implementation as an anode material. In this work, the main technique employed to gain this understanding is electrochemical impedance spectroscopy with distribution of relaxation times analysis (EIS-DRT). This mathematical approach to understanding traditional EIS datasets helps distinguish impedance contributions from the following processes: diffusion, counter electrodes, solid electrolyte Interfaces (SEI), and contact resistances.
Tin phosphide active material was synthesized by mechanical milling, with material structure confirmed by X-ray diffraction (XRD). Half cells were assembled with sodium counter electrodes and cycled with intermittent EIS assessment. Capacity retention was tracked during cycling to assess electrode operation. EIS-DRT analysis was performed every 5 cycles and after the end of cycling across the anode’s voltage range (0.01-1.5 V vs Na/Na+). After cycling, cyclic voltammetry (CV) and XRD were employed to further understand changes in electrochemical activity and crystal structure associated with the end of cycle life.
The evolution of impedance signatures across the initial five cycles exhibits significant shifting within the SEI and counter electrode peak at 1000 Hz. Impedance trends across the voltage range switched, in which lower voltages at higher levels of sodiation exhibit larger impedance contributions to the system. These trends are confirmed by a base understanding of SEI formation and sodiation trends. Relative impedance contributions from the diffusion process increase from pristine to cycled electrodes, with diffusion peaks at becoming the dominant impedance contribution as cycling progresses. Significant changes in DRT trends plateaued after the initial SEI formation over the first five cycles.
Abrupt and early failure during cycling of a subset of the cells was marked by a plateau in the working electrode voltage, an increase in contact resistance within EIS-DRT plots and decreased electrochemical activity within CV. Visual post mortem checks correlated well with these findings, with an apparent delamination of the electorate coating from the current collector. Understanding the physical and electrochemical phenomenon within a battery though nondestructive in situ characterization is crucial to simplify work flows in battery testing.
Reevaluating the Stability of the PEO-Based Solid-State Electrolytes for High Voltage Solid-State Batteries
Authors: Wu Xinsheng , Whitacre Jay 
Published: November 2022

Poly(ethylene oxide) (PEO) is a very popular polymer-based solid electrolyte material with relatively high ionic conductivity and dielectric constant1. However, many previous works mentioned that it could not be used in high voltage cells for its low oxidation potential (~3.9V vs. Li/Li+)2. However, only a handful of prior investigations evaluated the stability of the PEO-based solid-state electrolyte considering the contribution of the cathode surface chemistry to electrolyte oxidation and decomposition. Since most of the previous research exploring high voltage cathodes with PEO used LiCoO2, it could be possible the other cathode compositions will erode the PEO-based solid electrolyte in different and less extreme ways.
Our work revisits the high voltage electrochemical stability of PEO-based solid state-electrolyte materials. Potentiodynamic and galvanostatic tests were performed in test cells using PEO electrolyte layers with either LiNixMnyCozO2 or LiCoO2 cathode materials. We found that the high voltage instability of PEO-based solid-state cells is profoundly affected by the instability of the cathode material used. Specifically, the LiCoO2 electrodes were observed to undergo an irreversible oxidation process where they shattered into small pieces, which then led to a rapid irreversible loss in capacity. In contrast, we found that the PEO-based solid-state electrolytes could be stably cycled with high-nickel content cathodes stably at a voltage up to 4.5V vs. Li/Li+ over many cycles with minimal capacity deterioration.

K. Chrissopoulou, K. S. Andrikopoulos, S. Fotiadou, S. Bollas, C. Karageorgaki, D. Christofilos, G. A. Voyiatzis, and S. H. Anastasiadis, 44, 9710–9722 (2011).

J. Qiu, X. Liu, R. Chen, Q. Li, Y. Wang, P. Chen, L. Gan, S.-J. Lee, D. Nordlund, Y. Liu, X. Yu, X. Bai, H. Li, and L. Chen, Adv. Funct. Mater., 30, 1909392 (2020).
Characterizing Effect of Porous Transport Layers on Electrolyzer Performance Using Neutron Imaging
Authors: Komini Babu Siddharth , Mukundan Rangachary , LaManna Jacob Michael , Yilmaz Abdurrahman , Spendelow Jacob S. , Suarez Federico , Lee Sanghun , Schuler Tobias , Kulkarni Devashish , Stansberry John , Jacobson David , Hussey Daniel , Mauger Scott A , Bender Guido , Zenyuk Iryna V. , Khaykovich Boris 
Published: November 2022

Demand for high purity hydrogen production using renewable energy sources is growing to meet the clean energy demands. Polymer electrolyte membrane water electrolyzer (PEMWE) is one of the viable options for H2 production, but its high capital cost and operational expenditures increase the cost of H2. Improving the interface between the catalyst layer (CL) and the porous transport layer (PTL) is critical to increasing the efficiency of PEMWEs and thereby lowering the cost of H2. Increased contact between the CL and PTL improves catalyst utilization, and the optimal structure of the PTL reduces the mass transport issues related to O2 bubble removal.(1-3) Improved understanding of the PTL microstructure is necessary to improve the performance and efficiency of the PEMWE.
This work presents a systematic study to elucidate the effect of PTL properties (morphology, thickness, and porosity) and their impact on PEMWE performance under different operating conditions. Polarization curves with different anode PTL (felt, sinter and pore graded hierarchical PTL) are presented in Figure 1a. The separation of mass transport resistance and the contract resistance for the different PTLs will be elucidated to show the impact of water management and interfacial contact. Mass transport in an operating electrolyzer is also studied by estimating the water content using neutron imaging. Figure 1b shows water thickness across a membrane electrode assembly (MEA) with a pore graded hierarchical PTL in anode at different current densities. Water content across the MEA with different PTL is also studied. The cells with these PTLs were evaluated in operando using micro x-ray computed tomography (CT) and x-ray radiography. The x-ray techniques revealed oxygen distribution within the PTLs on the pore-scale at varied current densities, complementing neutron imaging water thickness studies and providing micro-scale insight into transport.

Acknowledgment

This research is supported by the U.S. Department of Energy (DOE) Hydrogen and Fuel Cell Technologies Office, through the H2NEW consortium.

References

J. K. Lee, C. Lee, K. F. Fahy, B. Zhao, J. M. LaManna, E. Baltic, D. L. Jacobson, D. S. Hussey and A. Bazylak, Cell Reports Physical Science, 1, 100147 (2020).

T. Schuler, J. M. Ciccone, B. Krentscher, F. Marone, C. Peter, T. J. Schmidt and F. N. Büchi, Advanced Energy Materials, 10, 1903216 (2020).

P. Lettenmeier, S. Kolb, F. Burggraf, A. S. Gago and K. A. Friedrich, Journal of Power Sources, 311, 153 (2016).

Figure 1
Tuning Catalyst-Ink Formulations for Blade Coating of Hydroxide-Exchange-Membrane Water Electrolyzers
Authors: Tricker Andrew W. , Fornaciari Julie C. , Lee Jason Keonhag , Danilovic Nemanja , Peng Xiong , Weber Adam Z. 
Published: November 2022

Clean hydrogen, produced by splitting water into H2 and O2 using renewable electricity, will play a crucial role as a renewable energy carrier and in decarbonizing industrial and hard-to-decarbonize transport sectors in the future.1 Hydroxide-exchange-membrane water electrolyzers (HEMWEs) have the potential to be more cost effective compared to the incumbent technology, proton-exchange-membrane water electrolyzers (PEMWEs) through the use of cheaper and more abundant catalysts and cell components.2 However, compared to PEMWEs, HEM systems have been studied significantly less and generally have much lower performance. Here, we systematically investigated a series of pivotal parameters that are related to catalyst inks, catalyst-layer structures, and porous-transport layer/catalyst-layer interfaces for HEMWEs. An integrated reference electrode is utilized to differentiate each individual effects on the cathode and anode when studying cell performance and durability. Catalyst-ink formulations are studied by varying ionomer-to-catalyst ratios, solid concentration, and solvent compositions. Additionally, parameters around the ink coating process are explored to study their impacts on catalyst-layer structures and provide guidance on key considerations for manufacturing robust catalyst layers. Finally, the impacts of porous-transport-layer architecture and cell configuration on the cell performance are probed. The findings elucidate critical properties and highlight urgently needed experimental practices towards high-performing HEMWEs.
Acknowledgements
This work was funded under the HydroGEN Consortium by the Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231.
References
1. B. Pivovar, N. Rustagi and S. Satyapal, The Electrochemical Society Interface, 27, 47 (2018).
2. K. Ayers, N. Danilovic, R. Ouimet, M. Carmo, B. Pivovar and M. Bornstein, Annual Review of Chemical and Biomolecular Engineering, 10, 219 (2019).
(Digital Presentation) Nickel Iron Layered Double Hydroxide As a Promising Anode for AEM Water Electrolyzer Presenting High Performance and Durability
Authors: Galkina Irina , Jiang Wulyu , Faid Alaa Y. , Borowski Patrick , Sunde Svein , Galkina Irina , Lehnert Werner 
Published: November 2022

Anion exchange membrane (AEM) water electrolyzers is an attractive alternative approach for green hydrogen production. The alkaline environment allows the use of non-PGM catalysts and, based on recent research in catalysts and membranes, may soon challenge the established proton exchange membrane water electrolyzers1,2. Transition metal-based catalysts have attracted much attention because they provide an excellent oxygen evolution reaction in alkaline media3. In particular, Ni-Fe-layered double hydroxides (LDH) have been intensively studied in recent years and have shown fast intrinsic electrocatalytic activity for water splitting4,5. In this work, we used Ni3Fe-LDH as an anode catalyst, DURAION® as ionomer and membrane and investigated the effects of electrode design and cell operation on the performance and stability of AEM electrolyzers. The optimized electrode was operated stably for 1000 hours at 1 A cm-2 with an overall degradation rate of 0.014 V h-1. At the end of the lifetime, the cell was disassembled and subjected to a series of experiments to investigate the physical and chemical degradation.
This work provides a fundamental understanding and specific approach to the use of nickel-iron-based electrodes and promotes the further development of AEM water electrolyzers through highly stabilized, Ni-rich, and low-cost anodic electrocatalysts.
This work has been performed in the frame of the CHANNEL project. This project has received funding from the Fuel Cells and Hydrogen 2 Joint Undertaking (now Clean Hydrogen Partnership) under grant agreement No 875088. This Joint undertaking receives support from the European Union's Horizon 2020 Research and Innovation program, Hydrogen Europe and Hydrogen Europe Research.

Vincent, I. & Bessarabov, D. Low cost hydrogen production by anion exchange membrane electrolysis: A review. Renew. Sustain. Energy Rev.
81, 1690–1704 (2018).

Miller, H. A. et al. Green hydrogen from anion exchange membrane water electrolysis: A review of recent developments in critical materials and operating conditions. Sustain. Energy Fuels
4, 2114–2133 (2020).

Gong, M., Wang, D. Y., Chen, C. C., Hwang, B. J. & Dai, H. A mini review on nickel-based electrocatalysts for alkaline hydrogen evolution reaction. Nano Res.
9, 28–46 (2016).

Zignani, S. C., Faro, M. Lo, Trocino, S. & Aricò, A. S. Investigation of NiFe-based catalysts for oxygen evolution in anion-exchange membrane electrolysis. Energies
13, (2020).

Mohammed-Ibrahim, J. A review on NiFe-based electrocatalysts for efficient alkaline oxygen evolution reaction. J. Power Sources
448, 227375 (2020).
Formation of Three-Dimensional Ion Transport Channels in Composite Solid Polymer Electrolyte for Use at Room Temperature
Authors: Nguyen An-Giang , Song Geon-Chang , Park Chan-Jin 
Published: November 2022

Lithium-ion batteries (LIBs) have widely revolutionized our lifestyle, from electronic devices and electric vehicles (EVs) to energy storage systems (ESSs) along with decarbonization trends for sustainable perspective. Unfortunately, the future application of conventional LIBs using liquid organic electrolytes has shown limitation in terms of their energy density and safety concerns. All-solid-state battery (ASSB) are attractive as a next-generation battery to address these issues. Among various solid-state electrolytes, composite solid polymer electrolyte (CSPE) is of particular interest by inheriting the advantages of both inorganic and solid polymer electrolytes. The CSPEs are generally constructed by dispersing (in)active fillers into the polymer matrix to facilitate the dissociation of lithium salts and decrease the crystallinity of polymer matrix, leading to an increase in the ionic conductivity of CSPEs. To further improve the ionic conductivity of CSPEs, the fillers with various morphologies from 0D, 1D, 2D, and 3D frameworks can be used to enhance the conductive pathways for lithium-ions diffusion. In particular, the 3D frameworks greatly improved ionic conductivity by supplying “highways” for lithium-ion diffusion. In addition, 3D frameworks can also prevent the agglomeration of filler particles and the growth of lithium dendrite.
In this study, by employing a 3D ionic transport framework, Li|3D-CSPE|Li symmetric cell could cycle over 1000 h at a current density of 0.1 mA cm-2. Moreover, all-solid-state Li|3D-CSPE|LiNi0.8Co0.1Mn0.1O2 cell retained a high capacity retention of 79.4% after 230 cycles at 30 °C. In addition, this novel concept is successfully applied to all-solid-state sodium batteries. The Na|3D-CSPE| Na3V1.97Mg0.03(PO4)3/C cell demonstrateed long-term cycling stability at 2 C. This approach provides a practical strategy to address the bottleneck of CSPE to enable safe and high-energy solid-state batteries.
Printable Lithium - LIOVIXTM Assisted All Solid-State Lithium-Ion and Lithium-Metal Batteries for Enhanced Electrochemical Properties
Authors: Black Rebecca , Navulla Anantharamulu , Fitch Brian , Xia Jian , Watson Andrew , Cabaniss Joseph Emory , Reid Julian , Yakovleva Marina 
Published: November 2022

All solid-state lithium-ion and lithium-metal batteries, which utilize a solid electrolyte in place of liquid electrolytes, are considered next-generation devices for energy storage due to their advantages in safety and potentially higher energy density. However, currently many solid-state lithium-ion and lithium-metal batteries are limited by their low Coulombic efficiency, poor power performance, and short cycling life due to the high resistance at the solid-state interfaces. Because of the diverse physical, chemical, and mechanical properties of various solid components in all solid-state batteries as well as the nature of solid-solid contact, many types of interfaces are present in a solid-state battery that can result in loose physical contact, formation of grain boundaries, and undesired chemical and electrochemical side reactions. All of these contribute to increasing resistance at the interface, which diminishes the cell performance, making solid state batteries not suitable for practical application.
LIOVIXTM is a unique printable formulation of lithium metal and other specialty materials, which can be used in both lithium-ion and lithium metal-based rechargeable batteries. In the case of lithium-ion batteries, it can be printed on a range of anode materials including silicon-containing anodes for the pre-lithiation process to improve the first cycle columbic efficiency and cell performance. In the case of lithium metal-based batteries, LIOVIXTM can be printed directly onto the current collectors or solid electrolyte separators to fabricate all solid-state batteries utilizing printed lithium metal anodes. This approach has the potential to enable improved performance, safety, recyclability, and lower cost compared to the current advanced lithium-ion systems. In both categories, printable lithium formulation can reduce the interface resistance between the anode and solid electrolyte layer, which enhances the cell performance enabling practical application. The printable lithium formulation is easily scalable using industry standard coating and printing equipment and is adaptable to any anode or cathode chemistry where an independent source of lithium is required. In addition, the lithium loading can be accurately controlled based on the applications’ requirements. We have demonstrated improved electrochemical performance of silicon containing anodes with liquid electrolytes in a full cell format. The present work will demonstrate the concept of all solid-state batteries incorporating printable lithium with enhanced electrochemical properties compared to conventional solid-state batteries.
Understanding Ion-Exchange Reaction Mechanisms in Layered Oxide Cathodes for Beyond Li-Ion Batteries
Authors: Kim Haegyum , Byeon Young-Woon 
Published: November 2022

Ion-exchange reactions are frequently used to develop novel metastable electrode materials for alkali-ion batteries that cannot be synthesized using direct chemical reactions. In fact, the ion-exchange reaction has been proven as an effective approach to develop novel transition metal oxide cathodes for lithium, sodium, and potassium ion batteries.[1-4] However, the solid-state ion-exchange mechanism and the resulting phase evolution are barely understood. In this work, we investigated the electrochemical ‘K-to-Na’ and ‘Na-to-K’ ion-exchange reaction mechanisms in layered oxide cathodes as it occurs using operando and ex situ structure characterization techniques.[5-6] Our study demonstrates that the ion-exchange occurs not by a simple Na/K interdiffusion in a given host structure. Instead, we discovered intriguing multi-phase evolutions according to the relative Na/K content, indicating that the ion-exchange systems may be more complex to interpret than the previously understood. We found that not only Na (or K)-layered oxide host interaction but also Na-K interaction affect the ion-exchange reactions. In this presentation, we will discuss how and why those parameters determine the ion-exchange reactions and resulting phase evolutions.

References

[1] S. Baskar et al. ECS Transactions
2017, 80, 357.
[2] N. Naveen et al. Chem. Mater.
2018, 30, 2049.
[3] C, Delmas et al. Mater. Res. Bull.
1982, 17, 117.
[4] A. R. Armstrong et al. Nature
1996, 381, 499.
[5] H. Kim et al. Chem. Mater.
2020, 32, 4312.
[6] H. Kim et al. Energy Storage Materials.
2022, 47, 105