Alexis Grimaud

Alexis Grimaud
Collège de France · Solid State Chemistry and Energy

Doctor of Philosophy
CNRS researcher - Collège de France

About

122
Publications
36,594
Reads
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10,291
Citations
Additional affiliations
October 2014 - present
French National Centre for Scientific Research
Position
  • Researcher
January 2012 - September 2014
Massachusetts Institute of Technology
Position
  • PostDoc Position
Education
November 2008 - December 2011

Publications

Publications (122)
Article
Battery 2030+ This Special Issue provides an overview of the scientific ambition for the European roadmap for future battery technologies “Battery 2030+”. It includes both the roadmap itself with its long term perspective as well as state of the art descriptions and deep‐dive articles outlining key themes of the roadmap. The overall purpose of “Bat...
Article
The sodium‐air battery offers a sustainable, high‐energy alternative to lithium‐ion batteries. Discharge in the cell containing glyme‐based electrolytes can lead to formation of large cubic NaO 2 particles via a solution‐precipitation mechanism. While promising, high rates result in sudden death. The exact nature of the discharge product has been a...
Article
Highly concentrated electrolytes offer enhanced energy-density for aqueous batteries, but the high salt concentration presents formidable challenges for practical implementation. Now, an electrolyte has been designed that has a substantially reduced salt concentration while still enabling high-performance batteries.
Article
This roadmap presents the transformational research ideas proposed by “BATTERY 2030+,” the European large-scale research initiative for future battery chemistries. A “chemistry-neutral” roadmap to advance battery research, particularly at low technology readiness levels, is outlined, with a time horizon of more than ten years. The roadmap is center...
Article
Driven by the continuous search for improving performances, understanding the phenomena at the electrode/electrolyte interfaces has become an overriding factor for the success of sustainable and efficient battery technologies for mobile and stationary applications. Toward this goal, rapid advances have been made regarding simulations/modeling techn...
Article
Li-ion batteries are the essential energy-storage building blocks of modern society. However, producing ultra-high electrochemical performance in safe and sustainable batteries for example, e-mobility, and portable and stationary applications, demands overcoming major technological challenges. Materials engineering and new chemistries are key aspec...
Preprint
Full-text available
Understanding the interfacial reactivity of aqueous electrolytes is crucial for their use in future batteries. We investigate the reactivity of the bis(trifluoromethane)sulfonimide (TFSI) anion when exposed to a strong alkaline medium, by means of ab initio molecular dynamics and enhanced sampling techniques. In particular, we study the nucleophili...
Article
Full-text available
The development of new batteries has historically been achieved through discovery and development cycles based on the intuition of the researcher, followed by experimental trial and error—often helped along by serendipitous breakthroughs. Meanwhile, it is evident that new strategies are needed to master the ever-growing complexity in the developmen...
Article
Full-text available
Insertion compounds provide the fundamental basis of today’s commercialized Li-ion batteries. Throughout history, intense research has focused on the design of stellar electrodes mainly relying on layered oxides or sulfides, and leaving aside the corresponding halides because of solubility issues. This is no longer true. In this work, we show the f...
Article
Today development of efficient catalytic systems for selective oxidation of alcohols to aldehydes remains not only a major concern in basic chemistry research but also a significant challenge for the chemical industry. One promising green and sustainable approach to increase the selectivity as well as waste reduction and to minimize the use of toxi...
Article
Full-text available
This is a critical review of artificial intelligence/machine learning (AI/ML) methods applied to battery research. It aims at providing a comprehensive, authoritative, and critical, yet easily understandable, review of general interest to the battery community. It addresses the concepts, approaches, tools, outcomes, and challenges of using AI/ML as...
Article
Full-text available
Open access to research data is increasingly important for accelerating research. Grant authorities therefore request detailed plans for how data is managed in the projects they finance. We have recently developed such a plan for the EU‐H2020 BIG‐MAP project – a cross‐disciplinary project targeting disruptive battery‐material discoveries. Essential...
Article
Highly concentrated electrolytes were recently proposed to improve the performances of aqueous electrochemical systems by delaying the water splitting and increasing the operating voltage for battery applications. While advances were made regarding their implementation in practical devices, debate exists regarding the physical origin for the delaye...
Article
Two-dimensional (2D) layered magnetic materials are generating a great amount of interest for the next generation of electronic devices thanks to their remarkable properties associated with spin dynamics. The recently discovered layered VI3 ferromagnetic phase belongs to this family, although a full understanding of its properties is limited by the...
Article
Full-text available
Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to manipulate the spin ordering of ferromagnetic OER catalysts (e.g., by magnetization) can reduce the kinetic barrier. However, most active OER catalysts are not...
Preprint
Full-text available
Open access to research data is increasingly important for accelerating research. Grant authorities therefore request detailed plans for how data is managed in the projects they finance. We have recently developed such a plan for the EU-H2020 BIG-MAP project - a cross-disciplinary project targeting disruptive battery-material discoveries. Essential...
Preprint
Highly concentrated electrolytes were recently proposed to improve the performances of aqueous electrochemical systems by delaying the water splitting and increasing the operating voltage for battery applications. While advances were made regarding their implementation in practical devices, debate exists regarding the physical origin for the delaye...
Preprint
Full-text available
Two-dimensional (2D) layered magnetic materials are generating a great amount of interest for the next generation of electronic devices thanks to their remarkable properties associated to spin dynamics. The recently discovered layered VI$_3$ ferromagnetic phase belongs to this family, although a full understanding of its properties is limited by an...
Article
Invited for this month's cover picture is an effort run by the group of Alejandro A. Franco and made in collaboration with Mathieu Morcrette, Patrik Johansson, Patrice Simon and Alexis Grimaud. The Front Cover illustrates an ideal scientific literature, in which all the data are systematically disclosed and available for researchers, together with...
Article
The Front Cover illustrates an ideal scientific literature, in which all the data are systematically disclosed and available for researchers, together with artificial intelligence algorithms aiming to bring new light on the next generation of batteries. More information can be found in the Concept by A. A. Franco and co‐workers.
Preprint
Insertion compounds provide the fundamental basis of today’s commercialized Li-ion batteries. Throughout history, intense research has focus on the design of stellar electrodes mainly relying on layered oxides or sulfides, and leaving aside the corresponding halides because of solubility issues. This is no longer true. In this work, we show for the...
Preprint
Full-text available
The production of hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. As spin-dependent kinetics exist in OER, the spin alignment in active OER catalysts is critical for reducing the kinetic barriers in OER. It is effective to facilitate the spin polarization in...
Preprint
p>Aqueous biphasic systems (ABS) can form when mixing water with two compounds such as polymers, ionic-liquids or simple salts. While this phenomenon has been known for decades and found applications in various fields such as biology, recycling or even more recently electrochemistry, the physics behind the formation of ABSs remains ill-understood....
Article
Full-text available
In this study, the effect of flow of the electrolyte on an electrolysis cell and a zinc cell is investigated. The gain of energy brought by the flow is discussed and compared to the viscous losses in the cells. We point out that the balance between the gained electrical power and the viscous loss power is positive only if the hydrodynamic resistanc...
Article
Full-text available
The recent discovery of “water-in-salt” electrolytes has spurred a rebirth of research on aqueous batteries. Most of the attention has been focused on the formulation of salts enabling the electrochemical window to be expanded as much as possible, well beyond the 1.23 V allowed by thermodynamics in water. This approach has led to critical successes...
Article
Full-text available
Artificial Intelligence (AI) has the promise of providing a paradigm shift in battery R&D by significantly accelerating the discovery and optimization of materials, interfaces, phenomena, and processes. However, the efficiency of any AI approach ultimately relies on rapid access to high‐quality and interpretable large datasets. Scientific publicati...
Article
CoCr2O4 activated at 1.7 V for 1.5 h (Act‐CoCr2O4) exhibits better OER activity compared to IrO2 in alkaline solutions. Pristine CoCr2O4 is originally inactive; activation (>1.56 V) promotes Cr leaching and lattice oxygen losses in CoCr2O4, leaving the highly defective surface for Co species to reconstruct into octahedrally coordinated Co3+–4+ oxyh...
Article
A rational design on oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Numerous works have been devoted to understanding the cation leaching and surface reconstruction of some very active electrocatalysts, while few have been on intentionally promoting the surface in a controlled fashion. In this...
Article
In Science, Oener, Foster, and Boettcher demonstrate that combining acidic and basic oxides as water dissociation catalysts allows for reducing the overpotential induced by the use of bipolar membranes close to zero under practical conditions. Furthermore, they demonstrate that design principles are shared across water dissociation catalysts and wa...
Article
Green hydrogen production using renewables-powered, low-temperature water electrolysers is crucial for rapidly decarbonizing the industrial sector and with it many chemical transformation processes. However, despite decades of research, advances at laboratory scale in terms of catalyst design and insights into underlying processes have not resulted...
Article
The sustainability of battery components is becoming a key parameter for storing renewable energy at large scale. Toward that goal, several strategies are currently being explored. Great hopes are placed in the use of superconcentrated aqueous electrolytes, which enlarge the electrochemical stability window well beyond 1.2 V. Although fundamentally...
Article
Full-text available
The growing hydrogen economy requires accelerating the hydrogen evolution reaction. The water dissociation step (Volmer step) has been proposed as a main kinetic limitation, but the mechanisms at play in the electrochemical double-layer are poorly understood. This is due to the dual role of water: it acts both as a reactant and as a solvent. Here w...
Article
This report investigates how the microstructures and chemical properties of carbon cathodes influence on the discharge capacity of aprotic Li-O2 batteries. For that, electrospun carbon fibers (CFs), Multi-wall carbon nanotubes (MWCNTs), carbon Super P and gas diffusion layer (GDL) were fully discharged at various applied current densities (0.05 - 0...
Article
Full-text available
The race for developing Li-ion batteries positive electrodes with always greater energy density has recently renewed interest towards understanding the formation of the so-called cathode electrolyte interface (CEI) forming upon cycling at high potential. In this work, we used an approach combining electrochemical measurements with physical characte...
Article
Full-text available
Water electrolysis is considered as a promising way to store and convert excess renewable energies into hydrogen, which is of high value for many chemical transformation processes such as the Haber-Bosch process. However, to allow for the wide-spread of the polymer electrolyte membrane water electrolysis (PEMWE) technology, the main challenge lies...
Article
Full-text available
The production of hydrogen at a large scale by the environmentally-friendly electrolysis process is currently hampered by the slow kinetics of the oxygen evolution reaction (OER). We report a solid electrocatalyst α-Li2IrO3 which upon oxidation/delithiation chemically reacts with water to form a hydrated birnessite phase, the OER activity of which...
Article
Recent studies have revealed the critical role played by the electrolyte composition on the oxygen evolution reaction (OER) kinetics on the surface of highly active catalysts. While numerous works were devoted to understand the effect of the electrolyte composition on the physical properties of catalysts’ surface, very little is known yet about its...
Article
Full-text available
High-energy-density lithium-rich materials are of significant interest for advanced lithium-ion batteries, provided that several roadblocks, such as voltage fade and poor energy efficiency are removed. However, this remains challenging as their functioning mechanisms during first cycle are not fully understood. Here we enlarge the cycling potential...
Preprint
p>The growing hydrogen-economy requires accelerating the hydrogen evolution reaction. The water dissociation step (Volmer step) has been proposed as a main kinetic limitation, but the mechanisms at play in the electrochemical double-layer are poorly understood. This is due to the ambivalent role of water: it acts both as a reactant and as a solvent...
Article
Full-text available
The production of sustainable hydrogen with water electrolyzers is envisaged as one of the most promising way to match the continuously growing demand for renewable electricity storage. While so far regarded as fast when compared to the oxygen evolution reaction (OER), the hydrogen evolution reaction (HER) regained interests in the last few years o...
Article
Full-text available
The development of efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is critical for improving the efficiency of water electrolysis. Here, we report a strategy using Fe substitution to enable the inactive spinel CoAl2O4 to become highly active and superior to the benchmark IrO2. The Fe substitution is revealed to facil...
Article
Hydrogen production technologies have attracted intensive attention for their potential to cope with future challenges related to renewable energy storage and conversion. However, the significant kinetic barriers associated with the oxygen evolution reac-tion (OER), one of the two half reactions at the heart of water electrolysis, greatly hinder th...
Article
Operando Liquid-electrochemical TEM for Monitoring Growth and Dissolution Steps of NaO2 Cubes in Na-O2 Battery - Volume 25 Supplement - Walid Dachraoui, Lukas Lutz, Lee. R. Johnson, Peter G. Bruce, Jean-Marie Tarascon, Alexis Grimaud, Arnaud Demortière
Article
The development of efficient water splitting heterogeneous catalysts in acidic media is largely hampered by both the slow kinet-ics of the oxygen evolution reaction (OER) and the limited stability of the electrocatalyst under these harsh working conditions. At the origin of both the activity and the instability of iridium oxides currently considere...
Article
Full-text available
Developing highly active electrocatalysts for oxygen evolution reaction (OER) is critical for the effectiveness of water splitting. Low‐cost spinel oxides have attracted increasing interest as alternatives to noble metal–based OER catalysts. A rational design of spinel catalysts can be guided by studying the structural/elemental properties that det...
Article
Aqueous biphasic systems (ABSs), in which two aqueous phases with different compositions coexist as separate liquids, were first reported more than a century ago with polymer solutions. Recent observations of ABS forming from concentrated mixtures of inorganic salts and ionic liquids raise the fundamental question of how "different" the components...
Article
Recently, Ir(V)‐based perovskite‐like materials were proposed as oxygen evolution reaction (OER) catalysts in acidic media with promising performance. However, iridium dissolution and surface reconstruction were observed, questioning the real active sites on the surface of these catalysts. In this work, Sr2MIr(V)O6 (M = Fe, Co) and Sr2Fe0.5Ir0.5(V)...
Article
Recently, Ir(V)‐based perovskite‐like materials were proposed as oxygen evolution reaction (OER) catalysts in acidic media with promising performance. However, iridium dissolution and surface reconstruction were observed, questioning the real active sites on the surface of these catalysts. In this work, Sr2MIr(V)O6 (M = Fe, Co) and Sr2Fe0.5Ir0.5(V)...
Preprint
Full-text available
i>Aqueous Biphasic Systems (ABS), in which two aqueous phases with different compositions coexist as separate liquids, have first been reported over a century ago with polymer solutions. Recent observations of ABS forming from concentrated mixtures of inorganic salts and ionic liquids raise the fundamental question of how "different" the components...
Article
The water reduction which produces hydrogen is one key reaction for electrochemical energy storage. While it has been widely studied in traditional aqueous electrolytes for water splitting (electrolyzers), it also plays an important role for batteries. Indeed, the reduction of water at relatively high potential prevents the practical realization of...
Article
Multiple electrochemical processes are involved at the catalyst/electrolyte interface during the oxygen evolution reaction (OER). With the purpose of elucidating the complexity of surface dynamics upon OER, we systematically studied two Ni-based crystalline oxides (LaNiO3-δ and La2Li0.5Ni0.5O4) and compared them with the state-of-the-art Ni-Fe (oxy...
Article
Aqueous Li-ion batteries have long been envisioned as safe and green energy storage technology, but have never commercially realized owing to the limited electrochemical stability window of water, which drastically hampers their energy density. Recently, Water-in-Salt electrolytes (WiSEs) in which a large amount of organic salts is dissolved into w...
Preprint
The water reduction which produces hydrogen is one key reaction for electrochemical energy storage. While it has been widely studied in traditional aqueous electrolytes for water splitting (electrolyzers), it also plays an important role for batteries. Indeed, the reduction of water at relatively high potential prevents the practical realization of...
Article
While quantitative models exist for measuring rate constants for electron exchange at the surface of semiconductors to or from redox couples in solution, their use is very limited for studying transition metal oxide electrodes. Taking advantage of the possibility of tuning the doping level of WO3 by thermal treatment, we measured the rate constants...
Article
The finding that triggering the redox activity of oxygen ions within the lattice of transition metal oxides can boost the performances of materials used in energy storage and conversion devices such as Li-ion batteries or oxygen evolution electrocatalysts has recently spurred intensive and innovative researches in the field of energy. While experim...