2023 • Energy & Environmental Science
J Alberto Blázquez, Rudi R Maça, Olatz Leonet, Eneko Azaceta, Ayan Mukherjee, Zhirong Zhao-Karger, Zhenyou Li, Aleksey Kovalevsky, Ana Fernández-Barquín, Aroa R Mainar, Piotr Jankowski, Laurin Rademacher, Sunita Dey, Siân E Dutton, Clare P Grey, Janina Drews, Joachim Häcker, Timo Danner, Arnulf Latz, Dane Sotta, M Rosa Palacin, Jean-Frédéric Martin, Juan Maria García Lastra, Maximilian Fichtner, Sumana Kundu, Alexander Kraytsberg, Yair Ein-Eli, Malachi Noked, Doron Aurbach
Emerging energy storage systems based on abundant and cost-effective materials are key to overcome the global energy and climate crisis of the 21st century. Rechargeable Magnesium Batteries (RMB), based on Earth-abundant magnesium, can provide a cheap and environmentally responsible alternative to the benchmark Li-ion technology, especially for large energy storage applications. Currently, RMB technology is the subject of intense research efforts at laboratory scale. However, these emerging approaches must be placed in a real-world perspective to ensure that they satisfy key technological requirements. In an attempt to bridge the gap between laboratory advancements and industrial development demands, herein, we report the first non-aqueous multilayer RMB pouch cell prototypes and propose a roadmap for a new advanced RMB chemistry. Through this work, we aim to show the great unrealized …
Show more2023 • Small
Sagi Hacmon, Shir R Liber, Lee Shool, Alexander V Butenko, Ayelet Atkins, Eli Sloutskin
Oil‐in‐water emulsion droplets spontaneously adopt, below some temperature Td, counterintuitive faceted and complex non‐spherical shapes while remaining liquid. This transition is driven by a crystalline monolayer formed at the droplets' surface. Here, we show that ppm‐level doping of the droplet's bulk by long‐chain alcohols allows tuning Td by >50 °C, implying formation of drastically different interfacial structures. It finds that “magic” alcohol chain lengths maximize Td. This is shown to arise from self‐assembly of mixed alcohol:alkane interfacial structures of stacked alkane layers, co‐crystallized with hydrogen‐bonded alcohol dimers. It accounts for these structures theoretically and resolve them by direct cryogenic transmission electron microscopy (cryoTEM), confirming the proposed structures. The discovered tunability of key properties of commonly‐used emulsions by minute concentrations of specific bulk …
Show more2023 • Materials Advances
Anagha Usha Vijayakumar, Jael George Mathew, Anya Muzikansky, Hannah-Noa Barad, David Zitoun
A sustainable future based on hydrogen fuel rests its faith on the rapid advancement of non-precious metal catalysts for the oxygen evolution reaction (OER). We demonstrate the efficient utilisation in the analysis of a large compositional space of binary NiFe and ternary NiFeV alloys for OER using a combinatorial method. We fabricated a gradient library of these multi metal alloys using physical vapor deposition and characterised them using high-throughput techniques. The electrocatalytic OER activity was studied using an automated electrochemical scanning droplet cell (SDC) set up designed in our lab. From the overpotential (@10mA/cm2) heatmaps of the libraries, the compositional regime of interest is funnelled down to 10-15% of Fe and 85-90 % of Ni for the NiFe alloy and 1-3% V, 10-15% Fe, and 80-90% Ni for the NiFeV alloy with their overpotential values falling between 320 – 330 mV. Due to its oxidation …
Show more2023 • Nanoscale 15 (17), 7625-7639, 2023
Vijay Bhooshan Kumar, Aharon Gedanken, I Porat Ze'ev
Ultrasonic irradiation of molten metals in liquid media causes dispersion of the metals into suspensions of micro- and nanoparticles that can be separated. This is applicable mainly to low-mp elemental metals or alloys, but higher mp elemental metals or alloys were also reported. Among metals, mercury and gallium exhibit especially-low melting points and are thus considered as liquid metals (LMs). Sonication of mercury in aqueous solutions of certain metal ions can cause simultaneous reduction of the ions and reactions between the metals. Gallium can be melted and sonicated in warm water, as well as in aqueous solutions of various solutes such as metal ions and organic compounds, which opened a wide window of interactions between the gallium particles and the solutes. Sonication of molten metals in organic liquids, such as polyethylene glycol (PEG) 400, forms carbon dots (C-dots) doped with …
Show more2023 • Materials Advances
Maximilian Mellin, Zhili Liang, Hadar Sclar, Sandipan Maiti, Igor Píš, Silvia Nappini, Elena Magnano, Federica Bondino, Ilargi Napal, Robert Winkler, Réne Hausbrand, Jan P Hofmann, Lambert Alff, Boris Markovsky, Doron Aurbach, Wolfram Jaegermann, Gennady Cherkashinin
High energy density Li-rich 0.33Li2MnO3·0.67LiNi0.4Co0.2Mn0.4O2 (HE-NCM) layered structure cathodes for Li-ion batteries provide higher capacity gain via incorporation of an excess of lithium into the host. As a serious drawback, these cathodes suffer from continuous voltage fade upon cycling. Recently, high capacity retention, rate capability and low voltage hysteresis were achieved for HE-NCM by new thermal double gases SO2 and NH3 treatment. However, so far a fundamental understanding of the mechanisms responsible for this improved stability is missing. Herein, a comprehensive study of the chemical composition and electronic structure modifications of a series of HE-NCM (untreated, treated, carbon- and binder- free) is performed using advanced electron spectroscopy techniques supported by theoretical calculations. We demonstrate that the double gases treatment process leads to a partial …
Show more2023 • The Journal of Physical Chemistry C
Oria Holin, Yosef Gofer, Dan Thomas Major, Doron Aurbach
A unique thermodynamic behavior was observed for solutions of magnesium bis(trifluoromethanesulfonyl) imide in 1,2-dimethoxyethane (DME), highly promising solutions for rechargeable Mg batteries: between 287 and 373 K, the solution exists as two immiscible phases, each with a different salt concentration, volume, and density. These characteristics depend strongly on temperature. To study this dependence, a phase diagram was constructed. In addition, partial phase volumes and densities were measured as a function of temperature. We observed that the temperature–molar fraction phase diagram exhibits closed-loop behavior, which is circumscribed by 287 and 373 K, with 333 K as an inversion locus. Below 287 K, the solution exists as a single homogeneous phase. At 287 K and above, the solution separates into two immiscible phases: a concentrated and dense lower phase and a dilute upper phase …
Show more2023 • bioRxiv
Andrew M Collins, Mats Ohlin, Martin Corcoran, James M Heather, Duncan Ralph, Mansun Law, Jesus Martinez-Barnetche, Jian Ye, Eve Richardson, William S Gibson, Oscar L Rodriguez, Ayelet Peres, Gur Yaari, Corey T Watson, William D Lees
Analysis of an individual's immunoglobulin (IG) gene repertoire requires the use of high-quality germline gene Reference Sets. The Adaptive Immune Receptor Repertoire-Community (AIRR-C) Reference Sets have been developed to include only human IG heavy and light chain alleles that have been confirmed by evidence from multiple high-quality sources. By including only those alleles with a high level of support, including some new sequences that currently lack official names, AIRR-seq analysis will have greater accuracy and studies of the evolution of immunoglobulin genes, their allelic variants and the expressed immune repertoire will be facilitated. Although containing less than half the previously recognised IG alleles (e.g. just 198 IGHV sequences), the Reference Sets eliminated erroneous calls and provided excellent coverage when tested on a set of repertoires from 99 individuals comprising over 4 million V(D)J rearrangements. To improve AIRR-seq analysis, some alleles have been extended to deal with short 3' or 5' truncations that can lead them to be overlooked by alignment utilities. To avoid other challenges for analysis programs, exact paralogs (e.g. IGHV1-69*01 and IGHV1-69D*01) are only represented once in each set, though alternative sequence names are noted in accompanying metadata. The Reference Sets also include novel alleles: 8 IGHV alleles, 2 IGKV alleles and 5 IGLV alleles. The version-tracked AIRR-C Reference Sets are freely available at the OGRDB website (https://ogrdb.airr-community.org/germline_sets/Human) and will be regularly updated to include newly-observed and previously-reported …
Show more2023 • bioRxiv
Thomas Konstantinovsky, Gur Yaari
T-cell diversity is crucial for producing effective receptors that can recognize the pathogens encountered throughout life. A stochastic biological process known as VDJ recombination accounts for the high diversity of these receptors, making their analysis challenging. We present a new approach to sequence encoding and analysis, based on the Lempel-Ziv 76 algorithm (LZ-76). By creating a graph-like model, we identify specific sequence features and produce a new encoding approach to an individual's repertoire. We demonstrate that this repertoire representation allows for various applications, such as generation probability inference, informative feature vector derivation, sequence generation, and a new measure for diversity estimation.
Show more2023 • EPJ Web of Conferences
Ilya Olevsko-Arad, Moshe Feldberg, Martin Oheim, Adi Salomon
Total internal reflection fluorescence (TIRF) has come of age, but a reliable and easy-to-use tool for calibrating evanescent-wave penetration depths is missing. We provide a test-sample for TIRF and other axial super-resolution microscopies for emitter axial calibration. Our originality is that nanometer(nm) distances along the microscope’s optical axis are color-encoded in the form of a multi-layered multi-colored transparent sandwich. Emitter layers are excited by the same laser but they emit in different colors. Layers are deposited in a controlled manner onto a glass substrate and protected with a non-fluorescent polymer. Decoding the penetration depth of the exciting evanescent field, by spectrally unmixing of multi-colored samples is presented as well. Our slide can serve as a test sample for quantifying TIRF, but also as an axial ruler for nm-axial distance measurements in single-molecule localization …
Show more2023 • ACS Energy Letters
Pallavi Singh, Yahel Soffer, Davide Raffaele Ceratti, Michael Elbaum, Dan Oron, Gary Hodes, David Cahen
In terms of sustainable use, halide perovskite (HaP) semiconductors have a strong advantage over most other classes of materials for (opto)electronics, as they can self-heal (SH) from photodamage. While there is considerable literature on SH in devices, where it may not be clear exactly where damage and SH occur, there is much less on the HaP material itself. Here we perform “fluorescence recovery after photobleaching” (FRAP) measurements to study SH on polycrystalline thin films for which encapsulation is critical to achieving complete and fast self-healing. We compare SH in three photoactive APbI3 perovskite films by varying the A-site cation ranging from (relatively) small inorganic Cs through medium-sized MA to large FA (the last two are organic cations). While the A cation is often considered electronically relatively inactive, it significantly affects both SH kinetics and the threshold for photodamage. The …
Show more2023 • Sustainable Energy & Fuels
Hari Krishna Sadhanala, Akanksha Gupta, Aharon Gedanken
Electrolysis of sea water is regarded as the most appealing and promising approach for the generation of hydrogen green energy, and even it lowers the cost of hydrogen production. However, for seawater electrolysis, highly efficient and robust electrocatalysts that can withstand chloride corrosion on the electrodes, particularly the anode, are required. Here, we present the synthesis of nickel molybdenum phosphide engineered with ruthenium supported on nickel foam (Ru22NiMoP2/NF) by a hydrothermal technique followed by reactions under autogenic pressure at elevated temperatures (RAPET) in a Swagelok, which demonstrated excellent electrocatalytic activity in alkaline sea water. For the hydrogen evolution reaction (HER), Ru22NiMoP2/NF requires low overpotentials of 60 and 52 mV to achieve a current density of 10 mA cm−2 compared to commercial Pt/C/NF (65 & 130 mV) in alkaline and alkaline sea …
Show more2023 • Advanced Therapeutics
Ella Itzhaki, Eva Chausky‐Barzakh, Ayelet Atkins, Avital Bareket‐Samish, Salomon M Stemmer, Shlomo Margel, Neta Moskovits
The arginine‐glycine‐glutamic acid (RGD) sequence, an αvβ3 integrin recognition site, is overexpressed in malignancies and neovasculature, making it a potential therapeutic target. Here, we assess efficacy/safety of tumor‐targeted RGD‐based proteinoid nanocapsules (NCs) entrapping a synergistic combination of two drugs – palbociclib (Pal), a CDK4/6 inhibitor, and alpelisib (Alp), a P13K inhibitor, as a cancer treatment. P(RGD) proteinoid polymers are produced by thermal step‐growth polymerization of R, G and D under inert atmosphere. P(RGD) NCs, hollow and encapsulating 25 w% each of Pal and Alp, are formed by self‐assembly of the proteinoid polymer. The encapsulation yields of Pal and Alp were 72% and 95%, respectively. Long‐term stability, controlled release, cellular uptake, and synergistic cytotoxicity and induced cell death are evident from in‐vitro experiments. Findings from in‐vivo breast …
Show more2023 • Laser & Photonics Reviews
Chenni Xu, Li‐Gang Wang, Patrick Sebbah
Chaos, namely exponential sensitivity to initial conditions, is generally considered a nuisance, inasmuch as it prevents long‐term predictions in physical systems. Here, an easily accessible approach to undo deterministic chaos and tailor ray trajectories in arbitrary 2D optical billiards by introducing spatially varying refractive index therein is presented. A new refractive index landscape is obtained by a conformal mapping, which makes the trajectories of the chaotic billiard fully predictable and the billiard fully integrable. Moreover, trajectory rectification can be pushed a step further by relating chaotic billiards with non‐Euclidean geometries. Two examples are illustrated by projecting billiards built on a sphere as well as the deformed spacetime outside a Schwarzschild black hole, which respectively lead to all periodic orbits and spiraling trajectories remaining away from the boundaries of the transformed 2D billiards …
Show more2023 • Energy & Fuels
Sengodan Prabhu, Moorthy Maruthapandi, Arulappan Durairaj, John HT Luong, Aharon Gedanken
Capsule-like CuO/CDs (CuO@CDs) with a surface area of 33.12 m2 g–1 were synthesized by the hydrothermal treatment, compared to 19.02 m2 g–1 for pristine CuO. An anode was then fabricated from capsule-like CuO@CDs to form a hybrid solid-state supercapacitor (HSSC) with the activated carbon (AC) cathode and PVA/1M KOH as an electrolyte. Three electrode system offered 1208.88 F/g (specific capacitance at 2 A/g current density) and unveiled a remarkable life cycle (retention) and Coulombic efficiency (CF): 93 and 98% after 5000 charge–discharge cycles at 10 A/g. In terms of performance, the HSSC delivered 1.5 V and 102.60 F/g (50.74 C/g) at 2 A/g, 8437.50 W/kg (power density), and 36.90 Wh/kg (energy density). The HSSC still retained 92% of cyclic stability and 83% of CF after 10,000 cycles.
Show more2023 • Batteries & Supercaps
Nabil El Halya, Mohamed Aqil, Karim El Ouardi, Amreen Bano, Ayoub El Bendali, Loubna Hdidou, Rachid Amine, Seoung‐Bum Son, Fouad Ghamouss, Dan Thomas Major, Khalil Amine, Jones Alami, Mouad Dahbi
TiO2 material has gained significant attention for large‐scale energy storage due to its abundant, low‐cost, and environmentally friendly properties, as well as the availability of various nanostructures. Phosphorus doping has been established as an effective technique for improving electronic conductivity and managing the slow ionic diffusion kinetics of TiO2. In this study, non‐doped and phosphorus doped TiO2 materials were synthesized using sodium alginate biopolymer as chelating agent. The prepared materials were evaluated as anode materials for lithium‐ion batteries (LIBs). The electrodes exhibit remarkable electrochemical performance, including a high reversible capacity of 235 mAh g−1 at 0.1 C and excellent first coulombic efficiency of 99 %. An integrated approach, combining operando XRD and ex‐situ XAS, comprehensively investigates the relationship between phosphorus doping, material …
Show more2023 • Chemical Communications
Roman R Kapaev, Malachi Noked
Although non-alkaline rechargeable Zn–air batteries (RZABs) are promising for energy storage, their chemistry is still underdeveloped and unclear. It was suggested that using Zn(OAc)2 or Zn(OTf)2 aqueous solutions as electrolytes enables reversible, corrosion-free charge–discharge processes, but the anodic stability of carbon in these cells has remained poorly studied. We report that CO2 evolution is manifested during the oxygen evolution reaction in non-alkaline RZABs, which is associated with the corrosion of carbon scaffolds. This corrosion is observed for different electrolyte compositions, such as Zn(OAc)2, ZnSO4 and Zn(OTf)2 solutions of various concentrations. The corrosion rate decreases when the overpotentials during the oxygen evolution reaction are lower. This study underlines the importance of addressing the anodic instability of carbon in non-alkaline RZABs.
Show more2023 • Physical Chemistry Chemical Physics
Yehuda Ben-Shabo, Adeliya Kurbanov, Claus Dieter Schröter, Robert Moshammer, Holger Kreckel, Yoni Toker
Velocity map imaging (VMI) is a powerful technique to deduce the kinetic energy of ions or electrons that are produced from a large volume in space with good resolution. The size of the acceptance volume is determined by the spherical aberrations of the ion optical system. Here we present an analytical derivation for velocity map imaging with no spherical aberrations. We will discuss a particular example for the implementation of the technique that allows using the reaction microscope recently installed in the cryogenic storage ring (CSR) in a VMI mode. SIMION simulations confirm that a beam of electrons produced almost over the entire volume of the source region, with a width of 8 cm, can be focused to a spot of 0.1 mm on the detector. The use of the same formalism for position imaging, as well as in a mixed mode where position imaging is in one axis and velocity map imaging is in a different axis, is also …
Show more2023 • Chemical Communications
Yulia Shenberger, Lada Gevorkyan-Airapetov, Melanie Hirsch, Lukas Hofmann, Sharon Ruthstein
EPR in-cell spin-labeling was applied to CueR in E. coli. The methodology employed a Cu(II)-NTA complexed with dHis. High resolved in-cell distance distributions were obtained revealing minor differences between in vitro and in-cell data. This methodology allows study of structural changes of any protein in-cell, independent of size or cellular system.
Show more2023 • Journal of Materials Chemistry A
Sri Harsha Akella, Muniyandi Bagavathi, Daniel Sharon, Capraz Ozgur, Malachi Noked
The realization of lithium–oxygen (Li–O2) batteries has been impeded by parasitic reactions that cause cell component degradation, often accompanied by the release of CO2 gas during oxidation reactions. The use of halide-based redox mediators (RMs) like LiBr and LiI has been proposed as a strategy to reduce overpotentials during oxygen evolution reactions and thus suppress the subsequent evolution of CO2. However, there is a scarcity of research examining the effectiveness of these RMs in the direct mitigation of parasitic reactions. In this study, we investigated the evolution of CO2 during the oxidation processes using an online electrochemical mass spectrometer. The results show that cells without RMs exhibited high overpotentials and significant CO2 evolution from the first charging cycle. In contrast, the addition of 50 mM LiI to the electrolyte resulted in a delay in CO2 evolution, observed only after …
Show more2023 • Industrial Chemistry & Materials
Lior Elbaz, Minhua Shao, Jianglan Shui, Carlo Santoro
Climate change calls for a change in the way we use and produce energy, and carbon-free has become the future direction of energy production and utilization. To obtain this, we must rely on sustainable energy sources such as wind and sun, but their intermittence limits the production of clean energy to only a few hours a day. To overcome this issue, energy storage and production technologies must be developed. Although several technologies have been proposed, the only viable scheme that could allow short-to-long-term storage and efficient energy transportation at-scale is the hydrogen economy, which relies on three pillars of technology: electrolyzers, hydrogen storage and fuel cells. In recent years, there have been rapid technological advances in hydrogen production, new hydrogen storage materials, and high-performance hydrogen fuel cells, etc. However, there are still numerous technological difficulties …
Show more2023 • Journal of Materials Chemistry A
Francis Amalraj Susai, Amreen Bano, Sandipan Maiti, Judith Grinblat, Arup Chakraborty, Hadar Sclar, Tatyana Kravchuk, Aleksandr Kondrakov, Maria Tkachev, Michael Talianker, Dan Thomas Major, Boris Markovsky, Doron Aurbach
Lithiated oxides like Li[NixCoyMnz]O2 (x + y + z = 1) with high nickel content (x ≥ 0.8) can possess high specific capacity ≥200 mA h g−1 and have attracted extensive attention as perspective cathode materials for advanced lithium-ion batteries. In this work, we synthesized LiNi0.9Co0.1O2 (NC90) materials and studied their structural characteristics, electrochemical performance, and thermal behavior in Li-cells. We developed modified cationic-doped NC90 samples with greatly improved properties due to doping with Mo6+ and B3+ and dual doping via simultaneous modification with these dopants. The main results of the current study are significantly higher capacity retention, greatly reduced voltage hysteresis, and considerably decreased charge-transfer resistance of the Mo and Mo–B doped electrodes compared to the undoped ones upon prolonged cycling. We also revealed remarkable microstructural …
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