bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Invited) Unlocking High-Performance Zero-Cobalt Cathode Active Materials: High-Entropy Doping and Pre-CAM Microstructure Optimization
Authors: Xin Huolin , Jing Yaqi 
Published: August 2024

Our recent work, published in Nature (610, 67–73, 2022) and Nature Energy (695–702, 2023), demonstrates the effectiveness of high-entropy doping (HE) in tackling the stability-capacity challenge of zero-cobalt layered cathode active materials (CAMs). While the HE Ni-80% (HE-N80) CAM exhibits competitive discharge capacity, it slightly lags behind NMC-811. This presentation delves into the broader applicability of the HE strategy and highlights the crucial role of pre-CAM microstructure optimization.
Through pre-CAM microstructure optimization, we significantly reduce layered CAMs' anti-site defects, leading to a notable enhancement in discharge capacity. This optimization strategy increases the discharge capacity of the HE-N80 cathode from 210 mAh/g to 220 mAh/g under 0.1C charging and 2.5-4.4V voltage window. Moreover, cycling stability sees a substantial improvement, with a 99.5% capacity retention at 0.5C after 100 cycles. The effectiveness of this methodology extends to CAMs with higher nickel content, as demonstrated by discharge capacities of 225 mAh/g for zero-cobalt HE-N85 and 235 mAh/g for zero-cobalt HE-N90 under the same conditions.
References:

Nature 610, 67–73 (2022).

Nature Energy, 695–702 (2023).
Scalable One-Pot Synthesis of Nanostructured P2-Type Na2/3Ni1/3Mn2/3O2 Cathode Material for High-Performance Na-Ion Batteries
Authors: Hassan Mohamed H. , Bruzzi Chiara , Detsi Eric 
Published: August 2024

Sodium-ion batteries (SIBs) based on sodium transition metal oxides are considered as a viable alternative to lithium-ion batteries (LIBs) for grid-scale energy storage. This is because the critical elements used in these SIBs, such as sodium, manganese, and nickel, are abundantly available, and their supply chain does not pose any geopolitical risk like lithium and cobalt used in common LIB cathodes.1 Among sodium transition metal oxide cathodes, the P2-type Na2/3[Ni1/3Mn2/3]O2 (NNMO) is a promising material due to its high operating voltage (up to 4.5 V vs Na/Na+) and high capacity. When cycled between 2-4.5 V vs Na/Na+, it has a capacity of 173 mAh/g.2 This combination of high operating voltage and high capacity allows NNMO to outperform common LIBs in terms of energy density. Therefore, SIBs based on NNMO cathode are a scalable alternative to LIBs.
Unfortunately, the current method used to produce NNMO through solid-state conversion is a time and energy-intensive process. It requires a temperature above 800 degrees Celsius and takes at least 12 hours to make a single batch of NNMO. Moreover, NNMO formed using this method has large particle sizes of a few micrometers. In my presentation, I will introduce a new and highly scalable method for synthesizing NNMO. This method can create NNMO in less than 20 minutes, which is much faster than the usual 12+ hours required by existing methods. Additionally, our protocol produces Nano-NNMO particles with size in the sub-200 nm. Nanoscale NNMO is crucial because it enhances the electrochemical performance of the materials, which I will also discuss.

Key words: Sodium-ion batteries, Na2/3[Ni1/3Mn2/3]O2, high capacity, nanoparticles, rapid synthesis.

References

(1) Wang, C.; Liu, L.; Zhao, S.; Liu, Y.; Yang, Y.; Yu, H.; Lee, S.; Lee, G.-H.; Kang, Y.-M.; Liu, R.; et al. Tuning local chemistry of P2 layered-oxide cathode for high energy and long cycles of sodium-ion battery. Nature Communications
2021, 12 (1), 2256. DOI: 10.1038/s41467-021-22523-3.
(2) Zhang, J.; Wang, W.; Wang, W.; Wang, S.; Li, B. Comprehensive Review of P2-Type Na2/3Ni1/3Mn2/3O2, a Potential Cathode for Practical Application of Na-Ion Batteries. ACS Applied Materials & Interfaces
2019, 11 (25), 22051-22066. DOI: 10.1021/acsami.9b03937.
Dewetted Nanoparticles – a Platform to Study Nanoscale Effects in Electrocatalysis
Authors: Altomare Marco 
Published: August 2024

To obtain interpretable electrochemical responses and define design criteria for electrocatalysts with enhanced performance, it is crucial to minimize the chemical and material complexity of electrodes [1]. Wet chemical methods are often applied in research to produce high surface area electrocatalysts, typically in the form of inks and coatings, including additives, binders, ionomers, etc., hence featuring complex, often unknown, structure, morphology, and chemical composition. This complexity might also lead to undesired mass transfer limitations and make it difficult to assess intrinsic catalytic properties of electrocatalysts.
This contribution is on designing and nanostructuring binder- and ionomer-free electrodes by solid-state dewetting [2,3], i.e., the heat-induced agglomeration of sputtered thin metal films into nanoparticles (NPs) with tunable loading, size, structure, and composition.
In this context, I discuss the following aspects: i) How dewetting can be steered to produce model, spatially separated and coherently oriented metal NPs with defined exposed facets [4]; ii) The use of dewetted electrodes to study nanoscale effects such as electronic metal support interactions (EMSI) in electrocatalytic reactions [5]; and iii) possibilities to apply scanning electrochemical techniques, in-situ spectroscopic tools or single-particle probes to investigate surface and interfacial phenomena of dewetted NP electrocatalysts.
[1] A.R. Akbashev, ACS Catal. 2022, 12, 8, 4296.
[2] C.V. Thompson, Annu. Rev. Mater. Res. 2012, 42, 399.
[3] Altomare et al., Chem. Sci. 2016, 7, 6865.
[4] Sharma et al., ECS 2023 https://ecs.confex.com/ecs/244/meetingapp.cgi/Paper/180073
[5] Harsha et al., ECS 2023 https://ecs.confex.com/ecs/244/meetingapp.cgi/Paper/179874
Cryogenic Atom Probe Tomograph to Resolve Confined Electrochemical Interfaces
Authors: Waszkiewicz Oliver Richard , El-Zoka Ayman A. , Ryan Mary P. 
Published: August 2024

Atom Probe Tomography (APT) is an analysis technique capable of providing a 3-dimensional, element-sensitive map of needle-shaped samples (where the tip radius is about 50 nm) with sub-nanometre resolution [1]. APT analysis is carried out at temperatures in the range of 25-75 K to limit the thermal motion of surface atoms which improves the spatial and mass resolution. As a result, this enables the analysis of frozen liquids, and by extension solid-liquid interfaces, by so-called “cryo-APT”. While this was historically challenging, recent advancements in UHV-cryogenic transfer and sample preparation methods now make it possible for the atomic scale analysis of interfacial species in electrochemical systems [2-4].
In this study, we will attempt to explore the effect of nanoscale geometrical confinement on the distribution of interfacial ions for the first time and to resolve the electric double layer, using cryo-APT. We will describe the workflow for cryo-APT sample preparation to study confined solid-liquid interfaces, using nanoporous gold as a template material with a frozen sodium iodide solution inside its pores. APT reconstructions will allow 3-dimensional mapping of aqueous interfacial species, helping to develop our understanding of the structure of the electric double layer under nanoscale geometrical confinement. The attached Figure shows an SEM image of the later stages of cryo-FIB milling of an APT tip of frozen deionised water and 50 mM sodium iodide and a segment of the related APT atom map reconstruction.
References
[1] Erwin W. Müller, John A. Panitz, and S. Brooks McLane. “The Atom-Probe Field Ion Mi-
croscope”. In: Review of Scientific Instruments 39.1 (1968), pp. 83–86. issn: 0034-6748.
[2] A. A. El-Zoka et al. “Enabling near-atomic–scale analysis of frozen water”. In: Science Advances
6.49 (Dec. 4, 2020). Publisher: American Association for the Advancement of Science, eabd6324.
[3] T. M. Schwarz et al. “Field evaporation and atom probe tomography of pure water tips”.
In: Scientific Reports 10.1 (Nov. 20, 2020). Number: 1 Publisher: Nature Publishing Group,
p. 20271. issn: 2045-2322.
[4] Stephenson LT, Szczepaniak A, Mouton I, Rusitzka KAK, Breen AJ, Tezins U, et al. (2018) The Laplace Project: An integrated suite for preparing and transferring atom probe samples under cryogenic and UHV conditions. PLoS ONE 13(12): e0209211.

Figure 1
Magnetic Field Driven Dynamic Reorganization of Electrocatalytic Interface for Sustainable Enhancement in Oxygen Evolution
Authors: Saha Jayeeta 
Published: August 2024

Hydrogen with high calorific content (150 MJ/kg) and environment-friendly combustion product (H2O) becomes the alternative fossil fuel. Catalytic electrolysis of water is one of the attractive routes for generating H2. Energy-efficient and cost-effective electrolytic production of H2 has predominantly focused on lowering the overpotential for water splitting process by developing newer non-Pt group-based catalysts.
This work demonstrates a new direction towards sustainable oxygen evolution reaction (OER) by exploiting the fundamental interplay of electromagnetic forces. Introducing an external magnetic field (Hext = 100 mT) perpendicular to the heterogeneous electrocatalytic interface produces an unprecedented increase in rate of electrocatalytic OER in phosphate buffer with pH=7. Such
electromagnetic

catalysis
is achieved with metal phosphides (NiCoP and NiCoFeP) with different morphology, leading 2.5 fold increase in the OER current density and concomitant lowering of overpotential by 10% (Hext = 100 mT). Thereby, 50% lowering of charge transfer resistance (Rct) is achieved. This is substantiated by the lowering of the Tafel slope (by 5%) in the presence of Hext. Thus, we report two important observations influenced by the magnetic field: (a) direct effect of magnetic field on the catalyst surface to reduce the charge-transfer resistance, (b) spin-dependant OER process to get influenced under magnetic field and (c) indirect effect of magnetic field to sustain the magneto-electrocatalytic enhancement even after removing the magnetic field. The time-scale of magnetic relaxation is million times higher than conventional spin-lattice relaxation events in para/ferromagnetic systems. Such long-term stability of magnetized states is predominantly proposed to be originating from the NiCoP and NiCoFeP interface. So, we attribute the long-lived states to be additionally contributed from the volumetric expansion and active site expansion of the catalyst upon magnetization. Catalyst interface is arising due to the dendritic structure of catalyst. Such synergism of magnetization, is expected to increase the applicability of magneto-electrocatalysis as a more sustainable electrocatalytic approach towards a hydrogen-driven economy.

Figure 1
An AC and DC Electric Field Effect Based Charged Particle Focusing Scheme for Particle Beam Mass Spectrometer
Authors: Yoon Jong-Min , Lee Seungjae , Park Kihong , Kim Taesung 
Published: August 2024

Particle Beam Mass Spectrometer (PBMS) is a mass analyzer based particle sizer, features a few to hundreds of nanometer (nm) sizing capabilities in environmental pressures above hundreds of mTorr. The above feature makes the PBMS be used as in-situ process monitoring schemes for several kinds of semiconductor process equipment (e.g. Chemical Vapor Deposition). However, it still cannot be used in other process equipment (e.g. Plasma etching, Ion implantation) which requires lower process pressure conditions than the PBMS operation limits. The bottleneck of pressure limits comes from an aerodynamic lens component, which focuses incoming particles in background gas using repetitive fluidic contraction and expansion effects. These effects hard to be happened when the target particles are surrounded in molecular or transition background gas regions. In order to lower the operating pressure limits, other focusing schemes are required.
In this study, an alternative particle focusing scheme which uses AC and DC electric field effects is proposed. The proposed scheme uses a stacked-ring ion funnel structure with variable AC and DC electric sources, for driving AC and DC potential variations along the funnel’s axial direction. While radial electric potential wells produced by AC frequency components induce particles’ radial position concentration to the funnel axis center, potential well depth and axial well depth steepness is controlled by AC amplitudes and DC source values.
Simulation results show that with the proposed scheme, more than 50% of particle transmission efficiencies are obtained for 5 nm – 100 nm sized charged particles moving with Maxwellian velocities in molecular background region. The results come from AC electric sources with 200 Hz - 20 kHz frequency ranges and within 50 V amplitude ranges, and DC electric sources within 50 V ranges which are feasible values for hardware implementation.
(Digital Presentation) A Microfluidic Approach for Direct Immobilization of Extracellular Vesicles on Gold Nanoislands for Efficient Detection Using Localized Surface Plasmon Resonance
Authors: Mohammadi Kyana , Raju Duraichelvan , Badilescu Simona , Ghosh Anirban , Packirisamy Muthukumaran 
Published: August 2024

Extracellular vesicles (EVs) are crucial for intercellular communication and are potential biomarkers for cancer diagnosis. To improve the detection of EVs, we have developed a platform that uses an ultra-thin film of gold to form gold nanoislands. This platform allows for the direct immobilization of EVs onto the gold nanoislands, using a simple microfluidic device. Detection of the EVs is based on the Localized Surface Plasmon Resonance (LSPR) method. With this innovative approach, we aim to enhance the accuracy and efficiency of EV detection, which could ultimately lead to faster detection and therefore the possibility of an early-stage diagnosis of cancer.
Gold nanoparticles are deposited on glass substrates using physical vapor deposition to create an ultra-thin layer of gold. Annealing the nanoparticle film forms gold nano-islands, which are drops with varying shapes and sizes from solid dewetting. A PDMS microfluidic device with a tapered channel of 200-micron depth and a 4mm diameter collection chamber bonded to gold-coated substrates is used to detect EVs from MCF7. The EVs flow through the channel at a rate of 10 µL/min, and the LSPR spectrum of the gold nanoislands is measured before and after EV immobilization. Changes in the refractive index of the surrounding medium due to the presence of EVs cause a shift in the Au LSPR band, which can be used to detect EVs.
In this study, we will utilize extracellular vesicles (EVs) obtained from a breast cancer cell line (MCF7) that had been grown in a small bioreactor. A simple microfluidic device will be designed and fabricated to evaluate the Localized Surface Plasmon Resonance (LSPR) shift of the gold plasmon band for different EV concentrations. The microfluidic device was chosen due to its high reproducibility, sensitivity, and ability to work with small amounts of EVs. To understand the sensitivity of this platform, a calibration curve will be plotted and compared with the results of other platforms that we have previously studied. To validate the LSPR detection using the microfluidic device, the eluted exosomes from the device will be characterized using TRPS and FESEM techniques.
Overall, our findings will demonstrate the potential of utilizing EVs and LSPR-based microfluidic devices as a promising tool for the detection of EVs and further clinical analysis for cancer diagnosis.
Preparation and Application of Manufactured Electrochemical Sensors for the Multiplexed Detection
Authors: Janegitz Bruno , Silva Luiz , Crapnell Robert , Stefano Jessica , Brazaca Lais , Banks Craig E. 
Published: August 2024

Monkeypox is a zoonotic viral infection caused by MKPV (1). This disease causes skin lesions, fever and headache among other symptoms, which appear within a few days after the infection, and can led to the hospitalization of the infected person (2). Herein, we present the first 3D-printed electrochemical bio-device for multiplex analysis, enabling portable detection of the Monkeypox Virus (MKPV). The electrochemical device consists of two working biosensors, an immunosensor, and a genosensor, specifically designed for the detection of the protein A29 (antigen) and the DNA target of MKPV. The electrodes were manufactured using lab-made ultra-flexible conductive filaments composed of carbon black, recycled PLA from coffee capsules, and castor oil as plasticizer. The sensors created through 3D printing technology exhibited good reproducibility and repeatability of analytical responses. Furthermore, both the immunosensor and genosensor demonstrated excellent MKPV detection capabilities, with a linear range from 0.01 to 1.0 µmol L-1 for the antigen and 0.1 to 20.0 µmol L-1 for the DNA target. The biosensors achieved limits of detection of 2.7 nmol L-1 and 29.0 nmol L-1 for the immunosensor and genosensor, respectively. Interference tests conducted with the biosensors demonstrated their selectivity for MKPV. Moreover, analyses of fortified human serum samples showed recoveries close to 100%, confirming the absence of significant matrix effects in MKPV analysis. Therefore, the 3D-printed multiplex device represents a viable and highly promising alternative for on-site, portable, and rapid point-of-care MKPV monitoring.
(1) Shafaati, M., Zandi, M., 2022. State-of-the-art on monkeypox virus: an emerging zoonotic disease. Infection 50, 1425–1430.
(2) Halvaei, P., Zandi, S., Zandi, M., 2023. Biosensor as a novel alternative approach for early diagnosis of monkeypox virus. Int. J. Surg. 109, 50–52.
Hybrid Piezoresistive 2D MoS2/PEGDA/PANI Covalent Hydrogels for Wearable Strain Sensors
Authors: Domenici Sara , Crisci Matteo , Gatti Teresa 
Published: August 2024

The continuous research on electronics, biocompatible materials and nanomaterials has led to the design of a new generation of wearable devices that can be employed in direct contact with the body of the user, which is attractive for real-time, non-invasive health monitoring1. For the satisfaction of such requirements, hydrogel-based conductive devices are often proposed as promising candidates for these applications, thanks to their softness, flexibility, and biocompatibility.
Here we report the synthesis of conductive hybrid hydrogels containing two-dimensional (2D) MoS2. The nanoflakes are integrated in the polymeric matrix creating an anisotropic structure, which helps to generate mismatch stress for a strain sensing under a certain stimulus2, thus allowing the gel to give an electrical response to pressure. 2D MoS2 nanoflakes were produced via top-down chemical exfoliation3 and were incorporated in the hydrogel through a covalent grafting to the polymeric building blocks by exploiting the prior surface functionalization of the flakes4. The conductivity of the hydrogels was increased with the further incorporation of in-situ polyaniline (PANI), which is a widely used material in biomedical applications as a biocompatible conductive polymer5. The as-obtained hydrogels are characterized through a combination of techniques, whereas their electromechanical properties are investigated via a home-made setup to prove that compression causes an increase in current due to the piezoresistive properties introduced with the incorporation of 2D MoS2 and PANI.
[1] Xie, J. et al. J Electrochem Soc
2020,167, 037541.
[2] Zhang, D. et al. J Mater Chem B
2020, 8, 3171–3191.
[3] Acerce, M. et al. Nat Nanotechnol
2015, 10, 313–318.
[4] Knirsch, K. C. et al. ACS Nano
2015, 9, 6018–6030.
[5] Humpolicek, P. et al. J. Synth Met
2012, 162, 722–727.
Phase Field Damage Framework for Modeling Thin-Film Silicon Anodes in All-Solid-State Batteries
Authors: Pyo Jaechan , Di Leo Claudio V. 
Published: August 2024

Recent advancements in solid electrolyte research have revived interest in the concept of silicon anodes for All-Solid-State Batteries (aSSBs). Tan et al. have recently proposed stable cyclic performance of micro-grain size pure silicon anodes paired with sulfide-based solid electrolytes [1]. This development has opened pathways toward potential aSSBs without encountering dendrite growth issues. This rediscovery of the thin-film a-silicon anodes concept has sparked computational interest in simulating the fracture-chemo-mechanical silicon lithiation mechanism. Understanding chemical reactions during lithiation and crack evolution during de-lithiation processes are intriguing topics. Especially, elastic-plastic deformation coupled with phase-field continuous fracture is crucial in comprehending the underlying physics and enhancing performance of battery cell through reverse engineering approaches.
In this work, we develop a thermodynamically consistent deformation-diffusion-damage coupled framework to model the evolution of dense, thin-film-like a-silicon anodes during lithiation and delithiation. During delithiation, tensile stress develops inside the film as the lithiated film overcomes the initial stack pressure and compressive stress prevalent during lithiation. As tensile stress and strain evolve, randomly distributed weak spots lead to crack nucleation. This fracture occurs throughout the silicon film, forming sharp vertical cracks, and depending on surface conditions along the solid-state electrolyte, some interfacial cracks may emerge, leading to permanent contact loss and resulting in capacity reduction.
From the model, we observed “mud crack” like phenomena, where crack distribution is not controlled by particle’s property, but entire cluster’s thickness matters. While flat model suggests that one that nucleate the crack was weak spots where they make stress concentration over entire body, whether they can evolve into big vertical crack mostly governed by connectivity of such weak spot maps. However, from our interface roughness model, what governs the crack evolution most was not the randomly distributed weak spot, but its geometric relative thickness difference between one another. Due to manufacturing process, perfect interface is hard to be achieved and such geometric irregularity always exist, thus, additive and binder studies along the silicon anode and its interface between sse would be key to achieve long and stable life span for a-silicon based aSSBs.

Reference

[1] Tan, Darren HS, et al. "Carbon-free high-loading silicon anodes enabled by sulfide solid electrolytes." Science 373.6562 (2021): 1494-1499.
Studies on Dual Sputtered CuGaO2 Thin Films
Authors: Bharath Akash Hari , Sundaram Kalpathy B. 
Published: August 2024

There has been extensive research conducted on n-type transparent conducting oxide (TCO) films like Sn-doped In2O3 (ITO) [1], Al-doped ZnO (AZO) [2], etc. P-type transparent conducting oxides are yet to be researched extensively. Active devices such as p-n junction devices and transistors are required to make progress in the development of transparent electronics. In this effort, research in p-Type TCOs is important. Most of the p-Type TCOs are copper-based ternary oxides [3].
In this work, CuGaO2 thin films were prepared using the dual-target RF magnetron sputtering technique. Cu2O and Ga2O3 targets were simultaneously sputtered on quartz substrates. The sputtering power of Cu2O was kept constant at 50 W and the sputtering power of Ga2O3 was varied. The films were deposited at room temperature and were subsequently annealed in nitrogen ambiance at 900 °C. The X-ray diffraction and optical studies were performed to analyze the films to optimize their properties.
[1] Fallah, H.; Ghasemi, M.; Hassanzadeh, A.; Steki, H. The effect of annealing on structural, electrical and optical properties of nanostructured ITO films prepared by e-beam evaporation. Mater. Res. Bull. 2007, 42, 487–496
[2] Shantheyanda, B.P.; Todi, V.O.; Sundaram, K.B.; Vijayakumar, A.; Oladeji, I. Compositional study of vacuum annealed Al doped ZnO thin films obtained by RF magnetron sputtering. J. Vac. Sci. Technol. A 2011, 29, 051514.
[3] Sundaresh, S.; Bharath, A.H.; Sundaram, K.B. Effect of Cu2O Sputtering Power Variation on the Characteristics of Radio Frequency Sputtered p-Type Delafossite CuCrO2 Thin Films. Coatings 2023, 13, 395.