bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Invited) Plasma Sources for Growth of Carbonaceous Materials for Energy Efficient Water Treatments
Authors: Kovacevic Eva , Jagodar Andrea , Marath Santhosh Neelakandan , Zavašnik Janez , Petit Agnes , Gimenez Loic , Hussain Shahzad , Strunskus Thomas 
Published: February 2024

Plasmas can not only be considered as a green technology for the treatment or synthesis of various types of materials, with applications from microelectronics to astrophysics, but they also serve as an excellent source for the green production of 2D materials that are often claimed to be crucial for applications in energy efficient water cleaning processes (in a passive or active way). Two typical examples are carbon nanotubes or nanowalls, stable grown on electrodes, which can be doped with nitrogen or oxygen, decorated with different oxides, or synthesized as MoS2 /C hybrids.
The most important point for the production of such multimaterials in plasmas is targeting the material and control of the synthesis. We show that one of the long known, and yet forgotten parameters important for the growth control concerns the plasma wall conditions.
Design Principles for Heterointerfacial Alloying Kinetics at Metallic Anodes in Rechargeable Batteries
Authors: Zheng Kent J.X. 
Published: February 2024

How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest. Here we consider the relation between the surface chemistry at such interfaces and the reversibility of electrochemical transformations at rechargeable battery electrodes. Using Zn as a model system, we report that a moderate strength of chemical interaction between the deposit and the substrate—neither too weak nor too strong—enables highest reversibility and stability of the plating/stripping redox processes. Focused-ion-beam and electron microscopy were used to directly probe the morphology, chemistry and crystallography of the heterointerfaces of distinct natures. Analogous to the empirical Sabatier principle for chemical heterogeneous catalysis, our finding arises from the confluence of competing interfacial processes. Using full batteries with stringent N:P ratios, we show that such knowledge provides a powerful tool for designing key materials in highly reversible battery systems based on earth-abundant, low-cost metals such as Zn and Na.
Reference: Zheng, Jingxu, et al. "Design principles for heterointerfacial alloying kinetics at metallic anodes in rechargeable batteries." Science Advances 8.44 (2022): eabq6321.
Magnetohydrodynamic Redeposition of Cations Onto the Anode
Authors: Jang Hansaem , Roe Daniel , Teobaldi Gilberto , Cespedes Oscar , Cowan Alexander 
Published: February 2024

Dissolution of metallic and metal-based catalysts occurs at the anode surfaces. The oxygen evolution reaction (OER) has been reported to cause the catalyst to be dissolved into cationic species during the electrolysis.[1–5] This phenomenon is not limited to non-noble metals (e.g. Fe, Co, Cu), but also occurs with noble metals (e.g. Ru, Rh, Pd, Os, Ir, Pt, Au).[1–4] Even with thermodynamically stable stoichiometric oxide catalysts, the dissolution cannot be completely avoided during the OER.[5] Upon dissolution, the as-formed cationic species will be attracted to the negatively charged cathode surface, resulting in catalyst loss from the anode over time.
Mass transport in diffusion layers during electrochemical reactions can be tuned by means of magnetohydrodynamics (MHD). This magnetic convection is a result of the Lorentz force that arises when there is an angular mismatch between the magnetic field and the local current density. Therefore, in the presence of a magnetic field, vortices can be generated around microscale protuberances on the electrode surface, and this phenomenon is often referred to as micro-MHD.[6] Conventional applications of MHD include cathodic electrodeposition and anodic corrosion or electropolishing studies. The difference in application according to the redox tendency of the target reaction is electrochemically rational on the basis of E
H–pH diagrams.
Despite a rather elusive combination, we presume that the magnetically-induced vortex can contribute to the electrochemical redeposition of as-dissolved cationic species onto the anode surface. Provided that a vortex can enhance the retention of the cations remaining in the vicinity of the surface, the chance of oxidative electrodeposition will increase. If this is the case, the protuberances on the anode are expected to grow under magnetic fields over the course of the OER. This will be realized as a result of facilitated O2 bubble detachment or increased local ionic concentration, or both.
In this work, we present that the morphology of the anode surface can change in the presence of a magnetic field. For the demonstration, we prepare a nanometrically-flat electrode consisting of a magnetic superlattice and an electrocatalyst layer. We perform the OER on the flat catalyst surface using magnetic and nonmagnetic samples and compare micrographs of pre-experimental and post-experimental sample surfaces. The findings show that the protuberances build up along their axes on the magnetic sample surface whereas the nonmagnetic sample involves the flattening of the surface.

References

[1] Angew. Chem. Int. Ed. 60 (2021) 13343–13349
[2] J. Electrochem. Soc. 161 (2014) H822
[3] J. Phys. Chem. Lett. 5 (2014) 2474–2478
[4] ChemCatChem 6 (2014) 2219–2223
[5] Nat. Catal. 1 (2018) 508–515
[6] Electrochem. Commun. 442 (2014) 38–41

Figure 1
Gold Ultralow Loading on Nickel Foam for Nitrogen Electrochemical Reduction
Authors: Milazzo Rachela Gabriella , Tranchida Giuseppe , Leonardi Marco , Scalese Silvia , Condorelli Guido Gugliemo , Lombardo Salvatore , Privitera Stefania M. S. 
Published: February 2024

Gold electroless deposition on nickel foam offers several advantages over traditional electrodeposition techniques. One of the main advantages is that it can produce uniform thickness coatings on complex shapes and geometries, such as porous and three-dimensional substrates like nickel foam. The resulting gold-nickel foam composite has high surface area and good electrical conductivity, making it suitable for various electrochemical applications, including catalysis, sensing, and energy storage.
In this work we focused on the development of synthetic strategies to grow and optimize the surface coverage of gold on nickel foam and the evaluation of its suitability for the electrochemical reduction of nitrogen for ammonia synthesis.
The gold electroless deposition on Ni Foam has been obtained by immersion in aqueous solution containing KAuCl4 and HCl, with or without stirring and addition of a surfactant agent (Isopropyl Alcohol). Depositions were performed by varying the immersion time from 30 seconds to 30 minutes. Scanning electron microscopy (SEM) has been employed to compare different deposition conditions and to optimize the morphology of the nanofilms, allowing higher catalytic activity. The electrochemical performance of the gold deposited on nickel foam was evaluated in a standard two compartments electrochemical cell using a Pt wire as counter electrode (CE), a saturated calomel electrode (SCE, saturated KCl) as reference and 0.1 M Na2SO4 solution as electrolyte. Electrochemical active surface area (EASA) and linear sweep voltammetry (LSV) have been adopted to evaluate the active area and the overpotential toward hydrogen evolution reaction (HER). Chronoamperometry experiments were carried out at various potentials to evaluate the performance of the catalyst for the electroreduction of nitrogen and ammonia synthesis.
The amount of ammonia produced was measured by the indophenol blue method.
The maximum NH3 yield of 2.8x10-11 mol s-1 cm-2 was achieved at -0.045 V vs RHE. The maximum faradaic efficiency of 5.8% was achieved at more positive potential (0.015 V vs RHE) due to the HER.
The results show that the gold on nickel foam exhibits excellent electrochemical stability and high conductivity.
This project has received funding from the European Union’s Horizon 2020 Research and Innovation programme under grant agreement No 101006941. This project started on the 1st of November 2020 with a duration of 42 months.
Metal Filled Nanostructured Silicon a Platform to Interlink Magnetism and Optics
Authors: Granitzer Petra , Rumpf Klemens , Gonzalez-Rodriguez Roberto , Coffer Jeffery 
Published: February 2024

This presentation deals with the utilization of nanostructured silicon (porous silicon and silicon nanotubes) for deposition of various metals, especially magnetic ones, within the pores/tubes. The novel magnetic properties of the semiconducting/magnetic composites which arise due to the nanoscopic size of the used materials are investigated with respect to optical and magnetic on-chip applications.
Porous silicon is fabricated by anodization of a silicon wafer in an aqueous hydrofluoric solution. The morphology of the porous structures depends on the doping density of the used wafer and on the applied current density as well as the electrolyte concentration. The ferromagnetic metals are deposited within the porous structures electrochemically in using the corresponding metal salt solution as electrolyte. A modification of the electrochemical parameters results in adjustable size and shape of the deposits. Ni and Co, both metals are electrodeposited within the nanostructured silicon in using aqueous NiSO4 and CoSO4 solutions by applying a current density between 10 and 20 mA/cm2 and a frequency between 0.05 and 0.2 Hz.
One of our key topics is luminescent porous silicon loaded with magnetic metals to enhance the photoluminescence, with the final aim to influence/control the optical properties by a magnetic field. The metal deposits affect the optical properties but also give rise to specific magnetic behavior (1). Due to the metal filling of the porous silicon the photoluminescence is blue-shifted and furthermore an increase of the intensity is observed. The influence of the magnetic metal filling on the optical properties (photoluminescence, decay time) is discussed, and the magnetic characterization of the nanocomposites is presented.
A further issue, the deposition of hard and soft magnetic materials within the nanostructures, aiming in the fabrication of arrays of permanent nanomagnets is presented (2). Here the investigation of the magnetic behavior of bi-metal nanostructures within nanostructured silicon with the aim to exploit the magnetic properties of both metals and gain control of the exchange coupling between the two metals especially with respect to their volume ratio is discussed. Furthermore, a variation of the structure size and the proximity of the metal deposits modify the exchange coupling and thus the energy product. Nanocomposite systems with an energy product as high as possible should be achieved to give rise to on-chip applications using permanent nanomagnets, especially arranged in arrays.
(1) P. Granitzer, et al, Frontiers in Physics, 8 (2020) 121
(2) K. Rumpf, et.al, Phys. Stat. Sol. A, 217 (2020) 1901040
Influence of Moisture on the Electrochemical Performance of Prelithiated C/SiOx Composite Anodes for Li-Ion Batteries
Authors: Fenske Hans , Lombardo Teo , Gerstenberg Jessica , Steckermeier Dominik , Kern Christine , Janek Jürgen , Kwade Arno 
Published: February 2024

Prelithiation of Si containing anodes has commonly been acknowledged as a potential solution to the challenge of the high irreversible lithium losses that still hinder the widespread adoption of this next-generation anode active material. However, upscaling and implementation in the process chain remain major hurdles for most proposed prelithiation processes. A significant part of this comes down to the high reactivity of prelithiation agents and prelithiated electrodes towards moisture. In industrial scale electrode production, dry rooms with dew point controlled atmospheres are already in use, but are a significant cost factor. Therefore, the compatibility of prelithiated electrodes with dry room conditions is a major factor for the implementation of prelithiation into existing production lines.
In this work C/SiOx composite anodes are electrochemically prelithiated and subsequently subjected to industry relevant moisture levels. The influence of dew point and exposure time is examined. After exposure, the anodes are assembled into half-cells and their electrochemical performance during the first lithiation/delithiation cycle is analysed using a 3-electrode setup. The evaluation of the specific capacities and the potential curves provides information about the extent of the damage to the electrode. The results indicate a promising stability window for dew points of up to -40° C and realistic exposure times of up to one hour. Additional aging investigations in full cells against NMC622-based cathodes confirm these findings. Furthermore, electrochemical impedance spectroscopy, XPS and ToF-SIMS measurements are performed to elucidate the effect of moisture exposure on the solid electrolyte interface (SEI) composition. The results suggest the development of a double-layered SEI structure, where the first layer forms during prelithiation and is altered by moisture exposure, while the second layer forms on top of the first layer during formation.

Figure 1
Optimizing Extreme Fast Charging Strategy for Lithium-Ion Batteries: A Model Predictive Control Approach
Authors: Kim KyungHyun , Choi Jung-Il 
Published: February 2024

With the increasing demand for extreme fast charging (XFC) in electric vehicles (EVs), there is an urgent need to develop health-conscious fast charging strategies for lithium-ion batteries. However, simply increasing the charging current can disproportionately accelerate battery aging, resulting in severe capacity and performance loss, while posing unacceptable safety risks during operation. In addition, the battery management system (BMS) needs to know the state of each cell for reliable and accurate management, but this involves significant computational burden. In other words, new fast charging strategies need to be developed to solve the dilemma between charging rate, battery aging, and computational complexity.
In this work, we propose a novel framework for modelling, estimating, and balancing different types of state heterogeneities in a multi-cell battery module. This framework facilitates the development of optimal fast charging strategies based on battery electrochemical models and model predictive control (MPC). First, an electrochemical and thermal coupling model is formulated at the unit cell level, and a module model is formulated at the system level, taking into account various factors such as connection resistances and system terminals. Then, a non-linear MPC is used to achieve fast charging while considering the health of the battery module. Battery performance is tracked by accurately estimating the battery's internal state, which can support the balancing of all state heterogeneity types represented in the model by controlling the charging current according to the internal state. The proposed framework has three main advantages: (1) The modelling strategy has a flexible and configurable structure that can be applied to battery modules of any size. Using this, (2) the internal state of the battery can be estimated with reduced computational complexity. (3) MPC can be applied to cell-to-cell balancing and XFC strategy. The results of the proposed method provide important insights for achieving XFC and show promise for real-time online estimation and control.

Figure 1
Impact of Metallic Impurities on the Synthesis and Properties of NMC Cathode Material Obtained by Co-Precipitation
Authors: Chable Johann , Bohn Nicole , Raab Monika , Geßwein Holger , Bergfeldt Thomas , Binder Joachim R. 
Published: February 2024

Among the different factors that influence lithium-ion batteries (LIB) performances, the properties of the cathode active material (CAM) play a crucial role. The composition, the crystallinity and also the particle size and morphology of these materials are part of the major parameters governing the CAM behaviour. These parameters are strongly dependent of the synthesis method, especially in the case of the hydroxide precursor of the layered LiNixMnyCozO2
[1].
One of the most widely spread synthesis method of such precursors is the synthesis by co-precipitation, where metal salts of Ni, Mn and Co are precipitated together in a continually-stirred tank reactor (CSTR) in carefully controlled pH- and temperature conditions[2]. Any parameter of the co-precipitation must be precisely tuned to obtain the desired material, as highlighted in the figure here after.
Considering the increasing presence of wanted (coating/doping)[3] and unwanted (impurities after recycling)[4] elements in the co-precipitation process, extensive knowledge of their impact on it is of great interest. Therefore, the synthesis of NixMnyCoz(OH)2 was conducted by co-precipitation with the controlled addition of increasing amounts of elements such as Cu and Al.
The effects of these additions were investigated by thoroughly characterizing the morphology of the obtained hydroxides with the help of SEM, BET, particle size distribution and porosity measurements. The composition of the synthesized hydroxides was determined by the ICP-OES technique. The possible influence on the further step of CAM synthesis, i.e. calcination, was followed by in-situ X-Ray thermodiffraction and the electrochemical performances were assessed by galvanostatic cycling the obtained CAM in lithium half-cells. This helped to evidence the varying impact of the added elements, depending on their concentration in the synthesis process.
This work is supported by the German Ministry for Economy and Climate Protection (BMWK).

References

[1] Malik, M., et al., Materials Today Energy, 2022, 28, 101066
[2] Van Bommel, A., Dahn, J.R., Chemistry of Materials, 2009, 21, 1500-1503
[3] Feng, Z. et al., ACS Applied Materials and Interfaces, 2021, 13, 43039-43050
[4] Kim, S. et al., Journal of Alloys and Compounds, 2021, 857, 157581

Figure 1
Niobate Anodes for High Rate Lithium-Ion Batteries
Authors: Huijben Mark , Xia Rui , Zheng Jie , Jager Maarten , Boukamp Bernard , Kaghazchi Payam , ten Elshof Johan E. 
Published: February 2024

Fast charging is one of the key performance requirements for next generation lithium ion batteries, and is directly related to the ease of ionic and electronic transport. However, lithium ion diffusion rates of promising anode materials, such as Li4Ti5O12, anatase TiO2, T-Nb2O5 and Nb18W16O93, are still insufficient. Therefore, nanosizing of the active electrode material is a common strategy to increase the effective lithium ion diffusion transport rate, which unfortunately also decreases the volumetric energy/power density and stability of the battery.
Recently, we demonstrated nickel niobate, NiNb2O6, for the first time as a new intrinsic high-rate electrode material,[1] which exhibits an intrinsic high rate performance enabled by its suitable host crystal structure without the requirement of realizing nano-architectures. The NiNb2O6 host crystal structure exhibits only a single type of channel for lithium ion intercalation and can be fully lithiated up to Li3NiNb2O6 with a capacity of about 244 mAh/g at low current densities. Interestingly, a high diffusion coefficient of 10-12 cm2/s at 300 K enables fast (dis)charging at high current densities resulting in high capacities of 140 and 50 mAh/g for respectively 10C and 100C. The minimal volume change during lithiation is the origin of the stable reversible lithiation process in NiNb2O6 and leads to a capacity retention of 81% after 20.000 cycles at 100C. The structural stability and electrochemical behaviour were investigated by various experimental techniques and confirmed by density functional theory (DFT) calculations. Finally, full cell systems against LiFePO4 and NCM811 cathodes demonstrate the promising energy storage performance of nickel niobate anodes in practical battery devices.
Our results strongly suggest that niobate-based materials are intrinsic high-rate anode materials without the requirement of realizing nano-architectures as typical for numerous titanium- and niobium-based oxides through complex synthesis procedures to minimize the length scales for lithium diffusion. Recently, we have replaced nickel by other transition metal ions to widen the exploration of niobate compounds for fast lithium ion diffusion. Large variations in electrochemical performance are observed, and the latest results will be presented. This will provide a new perspective on the role of intrinsic high-rate electrode materials for realizing ultrafast anode materials for future energy storage devices.
[1] R. Xia et al., Advanced Energy Materials 12 (2022) 2102972.
Machine Learning Based Identification of Lithium-Ion Battery Cell Chemistries
Authors: Wett Christopher , Goerick Dominik , Turan Bugra 
Published: February 2024

With a rapidly growing market for lithium-ion batteries in commercial applications and electrical vehicles, it is foreseeable, that in upcoming years a large number of batteries will return to manufacturers, recycling companies and testing facilities. Unfortunately, recycling companies already struggle with the fast identification of used and unknown batteries. Especially for the material re-use, a profound knowledge of the cell chemistry and its mass fraction is crucial. As of today, this issue is barely discussed in lithium-ion battery research as the focus mainly lies on battery simulation and state estimation.
In this work, we present a machine learning based approach for the fast identification of unknown cell chemistries. The approach makes use of differential voltage analysis (dV/dQ) of open circuit voltage (OCV) curves for the training of the machine learning model. The training data was synthetically generated using electrochemical models from PyBaMM. Significant model parameters like the amount of cyclable lithium and the ambient temperature were used to create thousands of differently aged models under different conditions. Besides training the model for lithium iron phosphate (LFP) and lithium nickel manganese cobalt oxides (NMC) cell chemistries, two NMC cells with different mass fractions (811 and 532) were used for training and testing.
Different machine learning approaches like decision trees, support vector machine classifiers and different ensemble learning methods were tested and compared against each other. Each of them showed excellent forecast accuracies for the tested chemistries. Moreover, the method was validated by successfully identifying measured OCV curves of real cells. Analysis of the identification techniques showed that the models only need a few significant points to distinguish the chemistries. Hence, the number of OCV points and the duration of the identification time can be drastically reduced for real world applications. In a next step, the OCV curves may even be reduced to partial curves.
The proposed method is a promising way of reliably identifying lithium-ion battery cell chemistries in a short time frame. It furthermore provides a straightforward solution for a neglected issue, that will most likely occupy battery research in the future.

Figure 1