Malachi Noked

Bar-Ilan University

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Yair Ein‐Eli

Technion – Israel Institute of Technology

Ayan Mukherjee

Institute of Minerals and Materials Technology

Jean‐Frédéric Martin

CEA LITEN

A. A. Kovalevsky

Technion – Israel Institute of Technology

Dane Sotta

Commissariat à l'Énergie Atomique et aux Énergies Alternatives

Aroa R. Mainar

Centre for Electrochemical Technologies

Ruhong Li

Institute of Biophysics

Xiulin Fan

Zhejiang University

J. Alberto Blázquez

Centre for Electrochemical Technologies

Eneko Azaceta

Centre for Electrochemical Technologies

Cooperative Institutions

Bar-Ilan University

Zhejiang University

Chinese Academy of Sciences

Institute of Nanotechnology

Alzheimer's Association of Israel

Ben-Gurion University of the Negev

Centre National de la Recherche Scientifique

The Technological College of Beer Sheva

Technion – Israel Institute of Technology

University of Chinese Academy of Sciences

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Improved Electrochemical Properties of Nickel-Rich, Low-Cobalt Layered Oxide Cathodes Using Dual-Functional Di-tert-butylmethyl Adamantoyl Silane Additives

ACS Applied Energy Materials (2024)

Sri Harsha Akella Mamta Sham Lal Yogendra Kumar Melina Zysler Dmitry Bravo‐Zhivotovskii

With an increasing demand for high-energy-density lithium-ion batteries (LIBs), nickel-rich cathodes such as LiNi0.9Mn0.05Co0.05O2 (NMC90) have gained significant interest due to their relatively low cobalt and high specific energy. However, cycling stability is compromised due to parasitic reactions at the electrode–electrolyte interfaces of NMC90. Herein, we demonstrate improved electrochemical properties of NMC90 using di-tert-butylmethyl adamantoyl silane (RSiCOAd: R is tBu(CH3)2 and Ad is 1-Ad) as an additive in a commercial electrolyte. Upon detailed electrochemical and spectroscopic analysis, we demonstrate that the RSiCOAd additive undergoes in situ decomposition to form a fluorinated organosiloxane passivation layer on the NMC90 surface and enhanced fluorination on the lithium anode surface. This phenomenon could significantly mitigate the parasitic reactions at the cathode–electrolyte interface while improving the electrochemical performances. Furthermore, the practical viability of the RSiCOAd additive is evaluated by full-cell studies with the graphite anode. After prolonged 200 cycles, full cells containing RSiCOAd with the incorporation of just 1% additive demonstrate an impressive ∼10% higher capacity retention, outperforming pristine NMC90 full cells.

Cobalt oxide

Nickel oxide

10.1021/acsaem.3c03273

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Citations (1)

Ultrathin Surface Coating Enables the Stable Sodium Metal Anode

Advanced Energy Materials (2016)

Wei Luo Chuan‐Fu Lin Oliver Zhao Malachi Noked Ying Zhang

A stable Na metal anodeis is reported by forming an artificial solid electrolyte interphase via a low-temperature plasma-enhanced atomic layer deposition technology. It is discovered that an ultrathin layer of Al2O3 layer (2.8 nm) can protect Na metal from electrolyte decomposition, prevent 3D dendrite formation, and significantly enhance its cycle stability in a carbonate-based electrolyte.

Interphase

Dendrite (mathematics)

Deposition

10.1002/aenm.201601526

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Citations (346)

A Rechargeable Zn–Air Battery with High Energy Efficiency Enabled by a Hydrogen Peroxide Bifunctional Catalyst (Adv. Energy Mater. 47/2024)

Advanced Energy Materials (2024)

Alagar Raja Kottaichamy Jonathan Tzadikov Angus Pedersen Jesús Barrio Gabriel Mark

Bifunctional catalyst

10.1002/aenm.202470208

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Multifunctional solvent molecule design enables high-voltage Li-ion batteries

Nature Communications (2023)

Junbo Zhang Haikuo Zhang Suting Weng Ruhong Li Di Lu

Elevating the charging cut-off voltage is one of the efficient approaches to boost the energy density of Li-ion batteries (LIBs). However, this method is limited by the occurrence of severe parasitic reactions at the electrolyte/electrode interfaces. Herein, to address this issue, we design a non-flammable fluorinated sulfonate electrolyte by multifunctional solvent molecule design, which enables the formation of an inorganic-rich cathode electrolyte interphase (CEI) on high-voltage cathodes and a hybrid organic/inorganic solid electrolyte interphase (SEI) on the graphite anode. The electrolyte, consisting of 1.9 M LiFSI in a 1:2 v/v mixture of 2,2,2-trifluoroethyl trifluoromethanesulfonate and 2,2,2-trifluoroethyl methanesulfonate, endows 4.55 V-charged graphite||LiCoO2 and 4.6 V-charged graphite||NCM811 batteries with capacity retentions of 89% over 5329 cycles and 85% over 2002 cycles, respectively, thus resulting in energy density increases of 33% and 16% compared to those charged to 4.3 V. This work demonstrates a practical strategy for upgrading the commercial LIBs.

Trifluoromethanesulfonate

Interphase

10.1038/s41467-023-37999-4

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A Rechargeable Zn–Air Battery with High Energy Efficiency Enabled by a Hydrogen Peroxide Bifunctional Catalyst

Advanced Energy Materials (2024)

Alagar Raja Kottaichamy Jonathan Tzadikov Angus Pedersen Jesús Barrio Gabriel Mark

Abstract Rechargeable alkaline zinc–air batteries (ZAB) hold great promise as a viable, sustainable, and safe alternative energy storage system to the lithium‐ion battery. However, the practical realization of ZABs is limited by their intrinsically low energy trip efficiency, stemming from a large charge and discharge potential gap. This overpotential is attributed to the four‐electron oxygen evolution and reduction reactions and their sluggish kinetics. Here, a new concept based on two‐electron generation and consumption of hydrogen peroxide at the air electrode is introduced. The O 2 /peroxide chemistry, facilitated by a newly developed Ni‐based bifunctional electrocatalyst, enables fast peroxide generation/consumption, exceptional energy efficiency, high durability, and high capacity. Hence, this new design offers substantial progress toward the commercialization of high energy density metal–air batteries.

Bifunctional catalyst

10.1002/aenm.202403817

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AZ31 Magnesium Alloy Foils as Thin Anodes for Rechargeable Magnesium Batteries

ChemSusChem (2021)

Ananya Maddegalla Ayan Mukherjee J. Alberto Blázquez Eneko Azaceta Olatz Leonet

In recent decades, rechargeable Mg batteries (RMBs) technologies have attracted much attention because the use of thin Mg foil anodes may enable development of high-energy-density batteries. One of the most critical challenges for RMBs is finding suitable electrolyte solutions that enable efficient and reversible Mg cells operation. Most RMB studies concentrate on the development of novel electrolyte systems, while only few studies have focused on the practical feasibility of using pure metallic Mg as the anode material. Pure Mg metal anodes have been demonstrated to be useful in studying the fundamentals of nonaqueous Mg electrochemistry. However, pure Mg metal may not be suitable for mass production of ultrathin foils (<100 microns) due to its limited ductility. The metals industry overcomes this problem by using ductile Mg alloys. Herein, the feasibility of processing ultrathin Mg anodes in electrochemical cells was demonstrated by using AZ31 Mg alloys (3 % Al; 1 % Zn). Thin-film Mg AZ31 anodes presented reversible Mg dissolution and deposition behavior in complex ethereal Mg electrolytes solutions that was comparable to that of pure Mg foils. Moreover, it was demonstrated that secondary Mg battery prototypes comprising ultrathin AZ31 Mg alloy anodes (≈25 μm thick) and Mgx Mo6 S8 Chevrel-phase cathodes exhibited cycling performance equal to that of similar cells containing thicker pure Mg foil anodes. The possibility of using ultrathin processable Mg metal anodes is an important step in the realization of rechargeable Mg batteries.

10.1002/cssc.202101323

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Solvent-Assisted Hopping Mechanism Enables Ultrafast Charging of Lithium-Ion Batteries

ACS Energy Letters (2022)

Xiaoteng Huang Ruhong Li Chuangchao Sun Haikuo Zhang Shuo‐Qing Zhang

Fast charging is regarded as one of the most coveted technologies for commercial Li-ion batteries (LIBs), but the lack of suitable electrolytes with sufficient ionic conductivity and effective passivation properties hinders its development. Herein, we designed a mixed-solvent electrolyte (1 M LiPF6 in fluoroethylene carbonate/acetonitrile, FEC/AN, 7/3 by vol.) to overcome these two limitations by achieving an FEC-dominated solvation structure and an AN-rich environment. The specific AN-assisted Li+ hopping transport behavior shortens the Li+ diffusion time, doubling the ionic conductivity to 12 mS cm–1, thus endowing the graphite anode with >300 mAh g–1 at 20C and reversible (de)intercalation over a wide temperature range (from −20 to +60 °C). Furthermore, the designed electrolyte triples the capacity of the 1 Ah graphite||LiNi0.8Mn0.1Co0.1O2 (NMC811) pouch cells at 8C in comparison with the commercial electrolyte. The solvent-assisted hopping mechanism maximizes the fast-charging capability of the electrolytes, which motivates further research toward viable next-generation high-energy LIBs.

Passivation

10.1021/acsenergylett.2c02240

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Citations (34)

A practical perspective on the potential of rechargeable Mg batteries

Energy & Environmental Science (2023)

J. Alberto Blázquez Rudi Ruben Maça Olatz Leonet Eneko Azaceta Ayan Mukherjee

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.

10.1039/d2ee04121a

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Citations (53)

Anion–Diluent Pairing for Stable High-Energy Li Metal Batteries

ACS Energy Letters (2022)

Chunnan Zhu Chuangchao Sun Ruhong Li Suting Weng Li‐Wu Fan

Rechargeable Li metal batteries (LMBs) have attracted wide attention as promising candidates for the next generation of energy-storage systems. However, limited Coulombic efficiency and unregulated dendrite growth restrict its application. Here, we report a kind of electrolyte by introducing fluorinated aromatic diluents into high-concentration electrolytes (HCEs). Unlike other localized HCEs, the fluorinated aromatic diluents pairing with anions promote the formation of a homogeneous and robust solid–electrolyte interphase (SEI), which endows Li metal with an ultrahigh Coulombic efficiency of ∼99.8%. The Li||LiNi0.8Co0.1Mn0.1O2 battery holds a capacity retention of >80% over 260 cycles even with a thin Li anode (20 μm) and a high cathode loading (3.5 mAh cm–2). A 1.8 Ah Li||NMC811 pouch cell with a lean electrolyte delivers an energy density of 340 Wh kg–1 and a stable cycling life over 200 cycles. The designed electrolytes, which benefit from the synergetic effects of anions and diluents on the SEI, pave the way for the next-generation LMBs.

Diluent

Potassium-ion battery

10.1021/acsenergylett.2c00232

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Citations (182)

Lithium Metal Anodes: Toward an Improved Understanding of Coupled Morphological, Electrochemical, and Mechanical Behavior

ACS Energy Letters (2017)

Kevin N. Wood Malachi Noked Neil P. Dasgupta

Li metal anodes are often considered a "holy grail" in the field of rechargeable batteries. Accordingly, the research community continuously seeks new strategies to improve their cyclability and reduce interfacial degradation. However, many recent reports focus on approaches that mitigate the symptoms of poor performance due to dendrites without addressing the underlying root cause of why they form and how they evolve. We propose that an emphasis on purely performance-based metrics has diluted the community's understanding of why a certain methodology is (un)successful. Furthermore, the lack of consistent protocols for reporting cell performance and inconsistent terminology for describing physical phenomena that occur at the Li anode make quantitative comparison difficult. The goal of this Perspective is to motivate the need for more consistent and fundamental research on the interfacial electrochemistry on Li metal anodes. Herein we provide an overview of: 1) recent advances in understanding the fundamental behavior of Li metal 2) the different "dendrite" morphologies (needle, mossy, fractal) often observed during cycling 3) the corresponding electrochemical and mechanical signatures of these various dendrites during cycling 4) the various failure modes of Li metal anodes and 5) how these failure modes are related to interactions at the electrode/electrolyte interface. As a result of these discussion points, five major questions are proposed that should be addressed through fundamental research in order to formulate design rules for mitigating deleterious performance of Li metal anodes, and standard experimental conditions are proposed that should be taken into account when reporting new strategies for Li stabilization.

10.1021/acsenergylett.6b00650

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Citations (489)