bluuebunny/crossref_metadata_2025_split huggingface dataset:
Computational Investigation of Halide Solid Electrolytes for Na-Based Batteries
Authors: Arraghraghi Hafssa , Bianchini Matteo 
Published: February 2024

Significant scientific and economic challenges are presented by developing battery systems with increased energy storage capacity. Geopolitical issues might pose supply chain risks for lithium (Li)-ion batteries, which are frequently used in portable electronics. As an alternative, sodium-ion batteries (NIBs), have drawn attention from researchers all over the world due to the perspective of being lower cost systems[1]. In comparison to lithium-ion batteries, solid-state sodium-ion batteries (SSSBs) promise as a safe, scalable, and environmentally friendly alternative. For the production of robust and adaptable SSSBs, the development of highly conductive, electrochemically stable, and chemically stable solid electrolytes (SEs) is essential [2]. With greater durability, adaptability, and safety, solid-state batteries with inorganic solid electrolytes are being heavily investigated as safer and perhaps more energy-dense alternatives to liquid electrolyte cells.
Sulfides solid electrolytes have been extensively investigated due to their mechanical softness and high ionic conductivity. However, the electrochemical oxidation stability of those materials are as low as 2 V (vs. Na+/Na)[3]. Alternatively, the excellent ion conductivities and stability at high potentials have made halide compounds, intriguing candidates for solid electrolytes in batteries. These compounds offer fast ion transport, good stability at highly oxidative potentials, and are easily processed. A wide range of chemistries, such as A3MX6 (A = Li, Na; M = Sc, In, Y, Yb, Er, Hf, Ho, Dy, Al, Zr; X = F, Cl, Br, I), have been synthesized with tunable properties and the characterizations of those materials shows relevant electrochemical proprieties [2].
In our work, we investigate different Na-based chloride compounds by Density Functional Theory (DFT). We expand beyond the reported compositions to consider possible cation-substituted compounds. Here, we report on the structures, ionic conduction pathways and ionic conductivity (computed by molecular dynamics methods) expected for such compounds. In the next months, we will also evaluate the compounds´ chemical and electrochemical stability. Our work moves us one step closer towards the development of stable and highly conductive solid electrolytes for Na-based solid-state batteries.
References :
[1] J. Mater. Chem. A, 2021,9, 281-292
[2]J. Mater. Chem. A, 2022,10, 21565-21578
[3] ACS Energy Lett. 2022, 7, 10, 3293–3301
Designing Better Li Metal Anodes for Solid-State Batteries Using a Combined Experiment/Theory Approach
Authors: Wood Marissa , Xiao Yiran , Freyman Megan C. , Wang Bo , Zhu Cheng , Li Sichi 
Published: February 2024

Solid-state batteries have the potential to transform energy storage by providing significantly higher energy densities and improved safety compared to conventional Li-ion batteries. Robust high-capacity Li metal anodes are necessary to realize this technology, but current Li metal anode designs suffer from significant degradation over time due to non-uniform Li plating/stripping and loss of contact with the solid electrolyte during cycling. Carbon scaffold hosts have been shown to mitigate this problem in liquid electrolyte systems by creating a uniform electric field and providing abundant Li nucleation sites, but they have not been well explored in solid-state systems, which require the fabrication of more complicated mixed ion/electron conducting scaffolds to provide transport of both Li ions and electrons throughout the anode. We investigated the effect of scaffold architecture and chemistry on the resulting Li morphology and electrochemical performance using a combined experiment/theory approach. Carbon scaffolds with well-controlled geometries and varied porosities were fabricated using 3D printing and then characterized by SEM, Raman, and XPS before cycling in cells to evaluate their performance as hosts for uniform Li plating/stripping. Atomistic and mesoscale modeling were used to predict how scaffold chemistry and microstructure affect Li nucleation probability and the formation of current density/stress hotspots that can lead to dendrite growth, and these results were used to help guide scaffold design. This work provides further insight into the relationship between anode architecture and Li metal cycling stability in solid-state batteries and demonstrates progress toward an anode-free configuration, which promises to simplify cell manufacturing, decrease cost, and increase energy density by plating the Li metal anode directly from the cathode in situ.
Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the U.S. Department of Energy, National Nuclear Security Administration under Contract DE-AC52-07NA27344.
Multi-Scale Analysis of Lithium-Sulfur Pouch Cells Using Imaging Methods
Authors: Arlt Tobias , Schmidt Florian , Ziesche Ralf F. , Selve Sören , Boenke Tom , Abendroth Thomas , Lu Yan , Dörfler Susanne , Risse Sebastian , Althues Holger , Kaskel Stefan , Manke Ingo 
Published: February 2024

Lithium-sulfur batteries (Li-S) are promising energy storage technologies. Its high gravimetric energy density, the abundance of sulfur and low costs at high production volume, this battery type is especially applicable for automotive and aerospace applications. In recent years, the number of reported prototype cells has increased, as well as their accessible energy density. This underlines the progress of technology readiness of the Li-S system. However, despite this important breakthrough density and cycling stability have to be overcome in the Li-S research. Additionally, the influence of the cathode porosity as well as the surface of the carbon material and the electrolyte composition play an important role on the conversion of sulfur and the performance of prototype cells.
Hard X-ray beamlines, as BAMline at the electron storage ring BESSY II in Berlin, Germany, have now been in service for over two decades. Several improvements have been implemented, allowing for operando tomography and fast radiographic measurements on the micrometer scale by using well-shaped synchrotron X-ray beam. In this study, operando X-ray imaging measurements on Li-S pouch cells are complemented by scanning and transmission electron microscopy and focused-ion-beam measurements on the nanometer scale delivering unique and multi-scale results about the morphology of sulfur inside the porous cathode material. Therefore, tiny pouch cells designs have been developed, allowing for operando tomography of stacked cells.

Figure 1
New Gel-Polymer Electrolyte for High-Performance Li‖LiFePO4 Cells with Enhanced Safety
Authors: Li Qi , Wang Jian , Wan Mintao , Passerini Stefano , Bresser Dominic 
Published: February 2024

The use of lithium-metal anodes promises batteries with substantially higher energy densities due to their high theoretical capacity of 3860 mAh g-1 and low redox plateau of -3.04 V vs. the standard hydrogen electrode [1, 2]. Of particular interest in this regard is the combination with (quasi-)solid electrolytes, potentially enabling a stabilized interface with the lithium electrode compared to solely liquid electrolyte systems [3].
Herein, a new gel-polymer electrolyte based on a non-toxic, nitrogen-containing polymer is reported that provides flame-retarding properties and decreases the volatility of the liquid electrolyte phase, thus, reducing the flammability of the electrolyte system as a whole [4, 5]. In addition, this electrolyte enables very stable cycling of symmetric Li‖Li cells and superior cell performance in Li‖LiFePO4 compared to the liquid analogue. In fact, the commercial availability of this polymer renders a potential use in future rather straightforward.

References

[1] X. Dong, A. Mayer, X. Liu, S. Passerini, D. Bresser, ACS Energy Letters, 8 (2023) 1114-1121.
[2] H.P. Liang, M. Zarrabeitia, Z. Chen, S. Jovanovic, S. Merz, J. Granwehr, S. Passerini, D. Bresser, Advanced Energy Materials, 12 (2022) 2200013-2200024.
[3] K. Sashmitha, M.U. Rani, Polymer Bulletin, 80 (2022) 89-135.
[4] K. Kiran Kumar, M. Ravi, Y. Pavani, S. Bhavani, A.K. Sharma, V.V.R. Narasimha Rao, Physica B: Condensed Matter, 406 (2011) 1706-1712.
[5] J. Zieba, Y. Zhang, P. N. Prasada, Sol-Gel Optics 11, 1758 (1992) 403-409.
Probing the Mo-Redox in Alluaudite Battery Materials
Authors: Barman Pubali , Jha Pawan Kumar Kumar , Gopalakrishnan Sai Gautam , Canepa Pieremanuele , Barpanda Prabeer 
Published: February 2024

Alluaudites are essentially naturally occurring mixed metal (Mn and Fe) phosphate-based minerals [1] consisting of an open framework structure to support fast alkali migration. The general formula for alluaudite can be expressed by A(1)A(2)M(1)M(2)2(XO4)3 where A and M sites are alkali ion and transition metals respectively and X can be S, P, As, Mo, W, V and so on [2]. The presence of polyanionic moieties (XO4) assures structural stability and high-voltage operation arising from the inductive effect [3]. Till date, a variety of phosphate and sulfate-based alluaudites have been reported as cathodes for Li-ion and Na-ion batteries [4,5].
In 2017, the first molybdate-based alluaudite material, Na2.67Mn1.67(MoO4)3, was reported as a 3.45 V Mn-based cathode [6]. Inspired by this work, we have explored other 3d (Co, Ni) based molybdate alluaudite homologues as potential compounds with desirable electrochemical and electrocatalytic activities.

Solution combustion synthesis was employed to prepare phase pure Na36Co1.32(MoO4)3 by restricting the annealing duration to one minute as compared to the reported solid-state route warranting prolonged (100 h) annealing. It was found to act as a high-voltage cathode (4 V vs Na/Na+ and 4.1 V vs Li/Li+) involving Co3+/Co2+ redox center [7] while cycling between 3.0 V to 4.3 V.

The above-mentioned alluaudite consists of Mo species, which can be redox-active at lower voltages. When cycled in a low-voltage window (0.01 V to 3.0 V), this material was found to act as an anode for both Li-ion and Na-ion batteries. High capacity (ca 400-500 mAh/g) was obtained with a central potential ~0.6 V involving conversion and (de)insertion reaction mechanism.

The Ni-analogue, Na4Ni0.8(MoO4)2 alluaudite, was studied as an anode material in both Li-ion and Na-ion batteries involving conversion and (de)intercalation redox mechanisms like the Co- analogue. The underlying redox mechanism will be described for both cases involving post-mortem diffraction, electron microscopy, and spectroscopic tools as well as with the help of the density functional theory (DFT) approach.

Finally, alluaudite Na4Cu(MoO4)3 was prepared by soft chemistry route, which was found to work as an anode material in the voltage window of 0.01 V to 3.0 V. The phase transformation and underlying redox mechanism will be elucidated.

References:

[1] D. J. Fisher, Am. Mineral. 40 (1955) 1100-1109.
[2] D. Dwibedi, P. Barpanda, A. Yamada, Small Methods 4 (2020) 2000051.
[3] P. Barpanda, L. Lander, S. Nishimura, A. Yamada, Adv. Energy Mater. 8 (2018) 1703055.
[4] P. Barpanda, G. Oyama, S. Nishimura, S.-C. Chung, A. Yamada, Nat. Commun. 5 (2014) 4358.
[5] D. Dwibedi, R. Araujo, S. Chakraborty et al, R. Ahuja, P. Barpanda, J. Mater. Chem. A 3 (2015) 18564-18571.
[6] J. Gao, P. Zhao, K. Feng, Chem. Mater. 29 (2017) 940-944.
[7] P. Barman, P.K. Jha, A. Chaupatnaik et al, P. Barpanda, Mater. Today Chem. 27 (2023) 101316.
Digital-Twin Modeling and Simulations on All-Solid-State Batteries
Authors: Lee Yong Min 
Published: February 2024

The use of digital twin technology for investigating all-solid-state batteries (ASSBs) has gained significant attention. Digital twin modeling is crucial in obtaining key design parameters such as effective ionic or electronic conductivity, specific contact area, which are difficult to obtain through experiments. This work presents two methods, bottom-up and top-down, for creating 3D microstructures of composite electrodes and discusses recent progress in upgrading both methods to uncover veiled parameters in ASSBs. Furthermore, the digital-twin electrode structures are coupled with electrochemical, thermal, and mechanical changes. This work is a valuable guideline for researchers working on ASSBs and related fields.
References:
1. Energy Storage Materials, 19 (2019) 124-129
2. Nano Energy, 62 (2019) 810-817
3. Chemical Engineering Journal, 391 (2020) 1235282
4. Advanced Energy Materials, 10(35) (2020) 2001563
5. ACS Energy Letters, 5(9) (2020) 2995-3004
6. Nano Energy, 79 (2021) 105456
7. Energy Storage Materials, 41 (2021) 289-296
8. Advanced Energy Materials, 12 (2022) 2103108
9. Energy Storage Materials, 49 (2022) 481-492
10. Nano Energy, 102 (2022) 107679
(Invited) Multiscale Modeling of Heterogeneous Interfaces for Hydrogen Production
Authors: Pham Anh Tuan 
Published: February 2024

Improving performance of hydrogen production devices requires a detailed understanding of physicochemical processes at solid-gas and solid-liquid interfaces. However, probing behavior of these interfaces under working conditions remain a significant challenge for both simulations and experimental techniques. In this talk, I will provide an overview of our strategy for simulating heterogeneous interfaces within the HydroGEN Advanced Water Splitting Materials Consortium, ranging from first-principles calculations of chemical reactivity to machine learning approaches for accelerating theory-experiment integration and continuum methods for understanding microstructure effects. In particular, I will discuss how computational models can be used to elucidate mechanisms of interface chemical reactions and mass transport, as well as the formation of new phases and their impacts on materials stability and performance. I will also show how simulations have been integrated with experimental probes, such as X-ray spectroscopy, to obtain new understanding of materials interfaces under operating conditions. Finally, I will discuss how this understanding is being used to guide new strategies for improving materials functionality for hydrogen production.
This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
(Invited) Water Splitting Materials for Solar Thermochemical Hydrogen Production
Authors: Bishop Sean R , Smith Andrew I , King Keith R , Clauser Arielle L , Sugar Josh D , Ambrosini Andrea , Sanders Michael , Coker Eric N , McDaniel Anthony H 
Published: February 2024

Solar thermochemical hydrogen (STCH) production uses concentrated sunlight to produce hydrogen using reduction/oxidation of metal oxides. Typically, the metal oxide is heated to high temperature (>1400 oC) causing it to release oxygen, then it is cooled to a lower temperature (<1000 oC) in steam whereby it re-oxidizes, stripping oxygen from water molecules and producing hydrogen. Due to improved stability, non-stoichiometric oxides that do not change phase during the STCH process are typically used, even though the reversible oxygen content is less than phase changing materials. HydroGEN (h2awsm.org) is an Energy Materials Network supported by the U.S. Department of Energy’s Hydrogen and Fuel Cell Technologies Office, and is focused on the development of new water splitting materials for STCH by fostering collaboration between U.S. national laboratories and external entities such as academia and industry. In this presentation, recent progress in developing new water splitting materials led by Sandia National Laboratories (SNL) will be presented. STCH performance of select materials predicted from a defect Graph Neural Network trained on crystal structures derived from density functional theory, subsequently synthesized and characterized using thermogravimetric analysis and flow reactor measurements, will be presented. Additionally, there will be discussion of benchmarking metrics and characterization of exemplar STCH materials. Lastly, trends in water splitting materials and durability considerations and challenges for commercialization will be discussed.
SNL is managed and operated by NTESS under DOE NNSA contract DE-NA0003525
(Invited) Hydrogen Benchmarking Project: Progress and Future Opportunities
Authors: Ayers Katherine E. , Carmo Marcelo , Roberts George , Marina Olga A , Stechel Ellen B , Xiang Chengxiang("CX") , Gross Karl 
Published: February 2024

The DOE Benchmarking project was created to foster consistency in testing and standards for advanced water splitting technologies, including high and low temperature electrolysis, solar thermochemical pathways, and photoelectrochemical water splitting. The goal was also to bring the water splitting community together in order to learn from each other and leverage synergies in methodology, knowledge, and tools across different technologies.
Over the first phase of the project, accomplishments have included establishing a regular series of workshops, discussing priority areas for each technology as well as cross-cutting areas. The outcomes of these workshops have included a set of frameworks defining tests which would be useful to standardize across the field, priority research directions and relative risk level/time to develop, and a first set of protocols focused on material development.
Next steps include refreshing the priority areas outlined 4 years ago, continuing to develop standardized protocols with a higher focus on component and device level especially for the more mature technologies, validating the existing protocols, and continuing to engage the community including international researchers. Validation includes ensuring that the protocol can reproducibly achieve consistent results for standard materials, and could involve setting up qualified labs for testing novel materials. The workshops will continue to be an essential part of advancing the benchmarking, protocols, and roadmaps, through providing a community forum to discuss research needs, share best practices, and maintain cohesive direction.
This talk will describe the success of the program to date, and plans for the next phase of the program.
(Invited) The Need for Standardized Benchmarking of Solid Oxide Cells
Authors: Lenser Christian , Menzler Norbert H. 
Published: February 2024

Solid Oxide Cells (SOC) have been the subject of intense scientific research in the past few decades, and significant progress has been achieved to increase the power output. While promising efforts to further industrialize the technology are underway, an increase in the performance of SOCs is still the scope of many scientific publications. However, progress in cell performance is increasingly hard to gauge due to a lack of comprehensive testing standards. Furthermore, many researchers publish performance data without providing all the necessary information about the testing conditions, or use metrics that do not allow comparison to other works.
In particular, the “peak power density” (PPD) is often used to characterize cell performance. The PPD is unsuitable as a performance indicator since it is far removed from a relevant working point for an SOFC, and depends to a large extend on the experimental conditions. To make matters worse, the PPD of high-performance cells is located at very high current densities, exacerbating the influence of the experimental conditions (which are often not described in detail or at all) and experimental artifacts on the measured performance. As a result, claims of increased cell performance may not hold up when applying standardized testing criteria.
This contribution summarizes the most important aspects that are relevant for performance evaluation of SOCs, focusing on those with the highest impact on apparent cell performance. Furthermore, the limitations of performance indicators on the cell level will be illustrated by comparing them to stack-level performance, and additional losses incurred under application-oriented operation conditions will be discussed. Since cell testing is often the key test to assess performance of novel materials and processing routes, comparability of the results is critical to scientific progress and therefore relevant for the community as a whole.
Forward-Bias 3D-Junction Bipolar Membranes for Electrochemical CO2 Reduction to CO
Authors: Kwen Jiyun , Herranz Juan , Schmidt Thomas J. 
Published: February 2024

The ongoing, rapid increase in atmospheric CO2 concentration has led to a growing interest in the electrochemical reduction of CO2 to value-added products like CO. To attain high current densities, the latter reaction is often performed using an anion exchange membrane(AEM) electrolyte that is well known to operate through the transport of (bi)carbonate ions from cathode to anode. This can in turn result in a CO2 pumping effect that decreases the device’s net CO2-consumption, and that can be prevented by using a bipolar membrane in a so-called forward-bias configuration (i.e., with the anion vs. cation exchange layers (AEL, CEL) contacting the cathode vs. anode electrodes, respectively). However, the recombination of protons and (bi)carbonate and concomitant production of H2O and CO2 at the AEL-CEL interface in this operative mode can also lead to the delamination of the membrane and cell failure.
In order to prevent such a delamination, this study proposes the introduction of a three-dimensional (3D) AEL-CEL junction, utilizing Nafion® as the cation exchange layer and PiperION as the anion exchange one. Two different methods were applied to fabricate the 3D junction bipolar membrane. The first method involves the fabrication of a 3D interlocking layer using polystyrene (PS) beads that are sprayed (along with Nafion ionomer) onto a Nafion membrane, and removed using toluene. This results in an inverse-opal structure atop the Nafion membrane whose pores can be filled with anion exchange ionomer (AEI). Complementarily, the second method involves the introduction of a layer, consisting of a mixture of AEI and cation exchange ionomer (CEI) between the AEM and CEM. Additionally, a non-conductive oxide material is added to this ionomer layer to increase the contact area of AEI and CEI. Finally, the electrochemical CO2 reduction performance and durability of the resulting, 3D junction bipolar membranes are evaluated and compared to those of an equivalent, 2D junction bipolar membrane, in all cases in a forward bias configuration.
(Invited) Materials Challenges for the Green Hydrogen Economy at Scale
Authors: Swider-Lyons Karen , Mittelsteadt Cortney 
Published: February 2024

Research and development projects over the last 30 years have successfully shown the value of hydrogen as a fuel and energy storage medium, and now hydrogen is seen as a key solution to decarbonization. Green hydrogen can be made by electrolysis anywhere that there is ample hydroelectric, solar and wind electric power. The hydrogen energy can be converted back to useful work in a fuel cell, turbine, or engine, or directly to manufacture products such as ammonia, cement, and steel. However, world decarbonization at scale also requires the demonstration of hydrogen at scale, and the widescale adoption of hydrogen for a green economy requires a reimagining of how energy is created, stored and used.
Leading technologies for the green hydrogen economy include proton exchange membrane fuel cells (PEMFCs) and PEM water electrolyzers (PEMWE), both which operate under acidic conditions. In addition to high electrocatalytic activity, the electrode materials must be designed for two- phase flow of water and gas. All of the materials should be durable, low cost, manufacturable, recyclable, and have the appropriate electronic and thermal properties.
This talk will describe some of the materials challenges needed to meet commercialization goals for PEMFCs and PEMWEs, and some of the constraints of manufacturing and recycling.