
Javier CarrascoCIC Energigune · Electrochemical Energy Storage
Javier Carrasco
PhD
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154
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Introduction
Dr. Javier Carrasco obtained his PhD in 2006 from the Universitat de Barcelona. His Ph.D thesis was devoted to the theoretical description of point defects in metal oxides using ab initio quantum chemistry methods. In 2007 he joined the Theory Department of the Fritz Haber Institute of the Max Planck Society, Berlin, as an Alexander von Humboldt fellow, working in the area of water-metal interfaces using density functional theory. In 2009 he moved to University College London, London, as a Newton International fellow. During this time he focused his research on the molecular-level understanding of ice formation on metal surfaces. Following this, in 2011 he moved to Instituto de Catálisis y Petroleoquímica del Consejo Superior de Investigaciones Científicas, Madrid, as a Ramón y Cajal fellow. Much of his work during this time was centred upon theoretical catalysis for hydrogen production and hydrogenation of hydrocarbons, as well as the application of van de Waals density functionals to molecular adsorption on metal and oxide surfaces. Since September 2013 he leads the Computational Studies group at the CIC Energigune.
Publications
Publications (154)
Manganese (Mn) substitution is a widely explored strategy aimed at sustainably enhancing the energy density of iron (Fe)-based electrode materials by taking advantage of the higher redox potential of the former. However, excessive Mn content can lead to detrimental effects, offsetting the expected improvements. In experimental studies, triphylite N...
Recent advancements in battery technology emphasize the critical role of solid electrolytes in enhancing the performance and safety of next-generation batteries. In this study, we investigate the interface stability and reaction mechanisms of Li3YCl5Br, a promising halide-based solid electrolyte, in contact with high-voltage Ni–Mn–Co (NMC) cathodes...
FullProfAPP is a software tool for data processing, refinement and visualization of large collections of powder diffraction patterns. Featuring an intuitive graphical user interface, it seamlessly facilitates a variety of tasks. These include conducting full-profile phase searches, sequential and high-throughput Rietveld refinements, and managing b...
Solid-state ionic conductors find application across various domains in materials science, particularly showcasing their significance in energy storage and conversion technologies. To effectively utilize these materials in high-performance electrochemical devices, a comprehensive understanding and precise control of charge carriers’ distribution an...
Climate Change and Materials Criticality challenges are driving urgent responses from global governments. These global responses drive policy to achieve sustainable, resilient, clean solutions with Advanced Materials (AdMats) for industrial supply chains and economic prosperity. The research landscape comprising industry, academe, and government id...
Halides are potential electrolytes for Li metal solid state batteries owing to their combination of high ionic conductivity, ductility and electrochemical stability against oxidation. However, their reactivity with the Li metal electrode may result in the formation of secondary compounds hindering their practical utility in terms of cycling perform...
Over the last decades, Density Functional Theory (DFT) has been the standard quantum mechanical method for the atomistic modelling of solids, giving an insight into the functional properties of applied materials. However, current materials innovation requires the screening of increasingly large and complex chemical spaces for both disordered and me...
This study presents novel computational methods applied to the technologically significant solid electrolyte materials, Li 6.55+y Ga 0.15 La 3 Zr 2-x O 12 ( Ga 0.15 /Sc y -LLZO), in order to investigate the effect of the distribution of Ga ⁺³ on Li-ion...
The growing requirements for electrified applications entail exploring alternative battery systems. Lithium‐sulfur batteries (LSBs) have emerged as a promising, cost‐effective, and sustainable solution; however, their practical commercialization is impeded by several intrinsic challenges. With the aim of surpassing these challenges, the implementat...
Model validation of a well-known class of solid polymer electrolyte (SPE) is utilized to predict the ionic structure and ion dynamics of alternative alkali metal ions, leading to advancements in Na-, K-, and Cs-based SPEs for solid-state alkali metal batteries. A comprehensive study based on molecular dynamics (MD) is conducted to simulate ion coor...
The development of high-energy-dense, sustainable all-solid-state batteries faces a major challenge in achieving compatibility between the anode and electrolyte. A promising solution lies in the use of highly ion-conductive solid electrolytes, such as those from the argyrodite family. Previous studies have shown that the ionic conductivity of the a...
Sulfonimide salts are of great interest for battery use thanks to their special properties including sufficient superior chemical/thermal stabilities, structural flexibility, etc. In particular, the hydrogen-containing sulfonimide (difluoromethanesulfonyl)(trifluoromethanesulfonyl)imide anion {[N(SO2CF2H) (SO2CF3)]⁻, DFTFSI⁻}, stands out owing to i...
The successful development of all-solid-state batteries will provide solutions for many problems facing current Li-ion batteries, such as high flammability, limited energy density, poor cyclability and low cation transference number. In this quest, the development of high-performance solid-state electrolytes is critical. Composite polymer electroly...
The advent of Li-metal batteries has seen progress toward studies focused on the chemical modification of solid polymer electrolytes, involving tuning either polymer or Li salt properties to enhance the overall cell performance. This study encompasses chemically modifying simultaneously both polymer matrix and lithium salt by assessing ion coordina...
Atomistic-level understanding of ion migration mechanisms holds the key to design high-performance solid-state ion conductors for a breadth of electrochemical devices. First-principles simulations play an important role in this quest. Yet, these methods are generally computationally-intensive, with limited access to complex, low-symmetry structures...
Atomistic-level understanding of ion migration mechanisms holds the key to design high-performance solid-state ion conductors for a breadth of electrochemical devices. First-principles simulations play an important role in this quest. Yet, these methods are generally computationally-intensive, with limited access to complex, low-symmetry structures...
Polymer electrolytes (PEs) with excellent flexibility, processability, and good contact with lithium metal (Li°) anodes have attracted substantial attention in both academic and industrial settings. However, conventional poly(ethylene oxide) (PEO)-based PEs suffer from a low lithium-ion transference number (TLi+), leading to a notorious concentrati...
A better molecular-level understanding of Li⁺ diffusion through ceramic/polymer interfaces is key to design high-performance composite solid-state electrolytes for all-solid-state batteries. By considering as a case study a composite electrolyte constituted by Li⁺ conductive Ga³⁺ doped-Li7La3Zr2O12 (LLZO) garnet fillers embedded within a poly(ethyl...
Magnesium has attracted a growing interest for its use in various applications, primarily due to its, abundance, lightweight properties and relatively low-cost. However, one major drawback to its widespread use remains its reactivity in aqueous environments, which is poorly understood at the atomistic level. Ab initio density functional theory meth...
High-throughput approaches in computational materials discovery often yields a combinatorial explosion that makes the exhaustive rendering of complete structural and chemical spaces impractical. A common bottleneck when screening new compounds with archetypal crystal structures is the lack of fast and reliable decision-making schemes to quantitativ...
P2-Na2/3[Fe1/2Mn1/2]O2 layered oxide is a promising high energy density cathode material for sodium-ion batteries. However, one of its drawbacks is the poor long-term stability in the operating voltage window of 1.5–4.25 V vs Na+/Na that prevents its commercialization. In this work, additional light is shed on the origin of capacity fading, which h...
Accelerating materials discovery is the cornerstone of modern technological competitiveness. Yet, the inorganic synthesis of new compounds is often an important bottleneck in this quest. Well-established quantum chemistry and experimental synthesis methods combined with consolidated network science approaches might provide revolutionary knowledge t...
The use of two types of bulky cations, tetrabutylammonium (TBA⁺) and Cs⁺, as electrolyte additives in Na‐O2 batteries is investigated. These cations facilitate the stabilization of sodium superoxide in the electrolyte, promoting the solution‐mediated pathway. Both the addition of TBA⁺ and Cs⁺ favor the growth of larger NaO2 cubes than in the case o...
Largely inspired by nature, hierarchical porous materials are attractive for a wide range of applications as they provide a unique combination of transport and interfacial properties. Hierarchical macro-nanoporous metals (HMNPM) are of particular interest due to their high thermal and electrical conductivities, high volumetric macroporosity as well...
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...
Sulfide glasses, with high room-temperature Li-ion conductivities, are a promising class of solid-state electrolytes for all-solid-state batteries. Yet, when in contact with Li metal, our current understanding of important interfacial phenomena such as electrolyte reduction and Li-ion transport is still quite limited, especially at the atomic scale...
Solid solutions of transition metal oxides are interesting for a diverse range of applications such as energy storage, catalysis, or microelectronics. Often, a key aspect to tailor the functioning of these materials is to control non-stoichiometry, i.e., the formation and mobility of oxygen vacancies. However, an accurate description of oxygen vaca...
CoxMn1−x)3O4 is a promising candidate material for solar thermochemical energy storage. A high-temperature model for this system would provide a valuable tool for evaluating its potential. However, predicting phase diagrams of complex systems with ab initio calculations is challenging due to the varied sources affecting the free energy, and with th...
(CoxMn1-x)3O4 is a promising candidate material for solar thermochemical energy storage. A high-temperature model for this system would provide a valuable tool for evaluating its potential. However, predicting phase diagrams of complex systems with ab initio calculations is challenging due to the varied sources affecting the free energy, and with t...
Accurate knowledge of phase coexistence regions, i.e., solubility gaps (SGs), is key to the development of mixed transition metal oxides for various applications, such as thermochemical energy storage, or catalysis. However, predicting a SG from first principles in these materials is particularly challenging due to the complex interplay between sev...
Development of efficient strategies for the rational design of materials involved in the production and storage of renewable energy is essential for accelerating the transition to a low-carbon economy. To contribute to this goal, we propose a novel workflow for the assessment and optimization of battery materials. The approach effectively combines...
Rechargeable solid-state batteries (SSBs) are of prime importance for developing the necessary safe and efficient energy infrastructures of the future. With several inherent advantages such as cost-effectiveness, superior flexibility, good processability, polymer electrolytes (PEs) have emerged as one of the most promising solid-state electrolytes...
Transition metal layered oxides (TMLOs) of general formula LiTMO 2 are the cornerstone of the present Li-ion technology as these cathode active materials allow the highest energy density thanks to the large capacity they offer. This is due to the high concentration of alkali metal their structure includes in the form of Li layers between TMO 2 meta...
Solid polymer electrolytes (SPEs) have been playing a crucial role in the development of high-performance solid-state lithium metal battery. The safety and the easy tailoring of the polymers designate these materials as promising candidates to be implemented as electrolytes. Poly(ethylene oxide) (PEO) has been widely employed during the past four d...
With the blooming of energy storage systems in e-mobility applications, the research activities of rechargeable lithium metal (Li°) batteries (LMBs) using solid-state electrolytes have been rekindled in recent years in light of stringent demands in terms of safety and energy density which are far beyond the capability of the contemporary lithium-io...
A novel single lithium‐ion conducting (SLIC) polymer electrolyte containing a weakly coordinating fluorine‐free polysalt is presented. The polysalt, lithium poly(4‐styrenesulfonyl)(dicyano)methide (LiPSDM), is conceived on the basis of a fluorine‐free green chemistry, and motivated by the highly performing non‐fluorinated lithium tricyanomethanide...
Polyanionic compounds stand out as attractive candidates for electrode materials in Na-ion and Li-ion batteries due to their stable 3D framework. ¹ Furthermore, according to theoretical calculations, N-substituted polyanionic compounds should enable the use of more than one redox couple of transition metals due to the lowering their working voltage...
Solid‐state lithium metal (Li°) batteries (SSLMBs) are believed to be the most promising technologies to tackle the safety concerns and the insufficient energy density encountered in conventional Li‐ion batteries. Solid polymer electrolytes (SPEs) inherently own good processability and flexibility, enabling large‐scale preparation of SSLMBs. To min...
In this work we report a framework to understand the role of solvent-salt interactions and how they mediate the performance of sodium-air/O2 batteries. The utilization of suitable electrolyte materials remains a point of major concern within the research community, as their stability and decomposition pathways during cycling are intimately connecte...
Heat-storage technologies are well suited to improve the energy efficiency of power plants and the recovery of process heat. A good option for high storage capacities, especially at high temperatures, is storing thermal energy by reversible thermochemical reactions. In particular, the Co3O4/CoO and Mn2O3/Mn3O4 redox-active couples are known to be v...
The search for sodium ion battery cathodes has led to considerable interest in sodium layered oxides due to their attractive properties - e.g. flexibility, versatility, and intrinsically fast Na ion structural diffusion (leading to enhanced rate capability). Based upon our rational approach to material selection (i.e. doping a Mn-rich structure wit...
Electrolytes with high ionic conductivity and intrinsic safety are key to achieving practical high-performance batteries and supercapacitors. Water-in-salt electrolytes (WiSE) render the performance of an aqueous lithium-ion battery well comparable to non-aqueous systems owing to the wide electrochemical windows and non-flammability. Critically, Wi...
Suppressing the mobility of anionic species in polymer electrolytes (PEs) is essential for mitigating the concentration gradient and internal cell polarization, and thereby improving the stability and cycle life of rechargeable alkali metal batteries. Now, an ether‐functionalized anion (EFA) is used as a counter‐charge in a lithium salt. As the sal...
Der Einfang negativer Ladungen in Polymerelektrolyten mit einem froschförmigen, Ether‐funktionalisierten Anion (EFA) wird von H. Zhang, J. Carrasco, M. Armand et al. in ihrer Zuschrift (DOI: 10.1002/ange.201905794) vorgestellt. Das Bis(trifluormethansulfonyl)imid‐Anion (TFSI), hier als Kaulquappe gezeigt, ist in einer Poly(ethylenoxid)‐Matrix (PEO)...
Trapping negative charges in polymer electrolytes using a frog‐shaped, ether‐functionalized anion (EFA) is presented by H. Zhang, J. Carrasco, M. Armand and co‐workers in their Communication (DOI: 10.1002/anie.201905794). The bis(trifluoromethanesulfonyl)imide anion (TFSI), shown as a slippery tadpole, is highly mobile in poly(ethylene oxide) (PEO)...
Die richtige Gegenladung: Ein Ether‐funktionalisiertes Anion (EFA) als Gegenladung zu einem Lithiumion erreicht ein niedriges anionisches Diffusionsvermögen, aber ausreichende Li‐Ionen‐Leitfähigkeit in einem Polymer‐Elektrolyten. Diese Eigenschaft ist sehr begehrt für Hochleistungs‐Festkörper‐Lithiumbatterien.
Abstract
Suppressing the mobility of...
Garnet Li7La3Zr2O12 (LLZO) is a promising solid electrolyte candidate for solid-state Li-ion batteries, but at room temperature it crystallizes in a poorly Li-ion conductive tetragonal phase. To this end, partial substitution of Li⁺ by Al³⁺ ions is an effective way to stabilize the highly conductive cubic phase at room temperature. Yet, fundamental...
Amongst post‐Li‐ion battery technologies, lithium–sulfur (Li–S) batteries have captured an immense interest as one of the most appealing devices from both the industrial and academia sectors. The replacement of conventional liquid electrolytes with solid polymer electrolytes (SPEs) enables not only a safer use of Li metal (Li°) anodes but also a fl...
The many advantages of Na-ion batteries (NIBs) in terms of availability and cost of raw materials if compared with Li-ion batteries (LIBs) are hindered by the stability of the Na-based electrodes. The most promising NIB positive electrodes are Co- and Ni-free sodium manganese rich layered oxides with general formula NaxMn1-yTMy-zT’MzO2 (y < 0.33, T...
With an extremely high theoretical energy density, solid-state lithium-sulfur (Li-S) batteries (SSLSBs) are emerging as one of the most feasible chemistries; however, their energy efficiency and long-term cyclability are severely hampered by the lithium metal (Li°) dendrite formation during repeated discharge/charge cycles and the shuttling of aggr...
Research into new energy storage technologies, for both portable and stationary applications, has become an urgent necessity. Rechargeable metal-air (oxygen) batteries are receiving intense interest as possible alternatives to lithium-ion batteries, because of their potential to provide higher gravimetric energies. While much attention has been foc...
Among high-capacity, low-cost cathode contenders for Na-ion batteries, layered transition metal oxides are particularly promising materials. Yet there is a strong need to improve their long-term stability and capacity retention due to unwanted phase transitions occurring during sodium insertion and extraction cycles. Here, using density functional...
The anion chemistry of lithium salts plays a pivotal role in dictating the physicochemical and electrochemical performance of solid polymer electrolytes (SPEs), thus affecting the cyclability of all‐solid‐state lithium metal batteries (ASSLMBs). The bis(trifluoromethanesulfonyl)imide anion (TFSI⁻) has long been studied as the most promising candida...
Progress in energy-related technologies demands new and improved materials with high ionic conductivities. Na- and Li-based compounds have high priority in this regard owing to their importance for batteries. This work presents a high-throughput exploration of the chemical space for such compounds. The results suggest that there are significantly f...
A salient aspect of research in batteries is the discovery of new materials or novel properties of existing compounds. In this quest, the traditional approach is to focus on archetype compounds in which a desirable property was first observed, stimulating further investigations. This has been the innovation pathway of many battery materials (e.g.,...
The anion chemistry of lithium salts plays a pivotal role in dictating the physicochemical and electrochemical performance of solid polymer electrolytes (SPEs), thus affecting the cyclability of all solid‐state lithium metal batteries (ASSLMBs). Bis(trifluoromethanesulfonyl)imide anion (TFSI−) has long been studied as the most promising candidate f...
Solid polymer electrolytes (SPEs) with high cationic conductivity are highly desired for enhancing the power performance of all‐solid‐state alkali metal batteries (ASSAMBs). In this work, a new sulfonimide anion, (difluoromethanesulfonyl)(trifluoromethanesulfonyl)imide (DFTFSI−), is proposed as a possible alternative to the most widely used bis(tri...
Garnet-structured Li7La3Zr2O12 is a promising solid electrolyte for next-generation solid-state Li batteries. However, sufficiently fast Li-ion mobility required for battery applications only emerges at high temperatures, upon a phase transition to cubic structure. A well-known strategy to stabilize the cubic phase at room temperature relies on ali...
During the past two decades, the demand for the Electrical Energy Storage systems has increased for both portable and stationary applications, predominantly in the form of batteries [1]. In this sense, lithium-ion batteries have dominated the market as they offer the highest gravimetric capacity. However, owing to concerns over lithium cost and sus...
The delicate balance between hydrogen bonding and van der Waals interactions determines the stability, structure, and chirality of many molecular and supramolecular aggregates weakly adsorbed on solid surfaces. Yet the inherent complexity of these systems makes their experimental study at the molecular level very challenging. In this quest, small a...