Javier Carrasco

Javier Carrasco
CIC Energigune · Electrochemical Energy Storage

PhD

About

123
Publications
23,553
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6,114
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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 (123)
Preprint
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...
Article
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...
Article
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...
Article
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...
Article
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...
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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...
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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...
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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...
Article
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...
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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...
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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...
Article
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...
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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...
Preprint
Full-text available
(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...
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Full-text available
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...
Chapter
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...
Article
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...
Article
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...
Article
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...
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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...
Article
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...
Article
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...
Article
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...
Article
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...
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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...
Article
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)...
Article
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)...
Article
Full-text available
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. Herein, we propose an ether‐functionalized anion (EFA−) as novel counter‐charge in a lithium salt....
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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...
Article
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...
Article
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...
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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...
Article
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...
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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...
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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...
Article
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...
Article
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...
Article
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...
Article
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...
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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...
Preprint
Full-text available
The delicate balance between H-bonding and van der Waals interactions determine 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.Small alcohols adsorbed on metal s...
Article
With a remarkably higher theoretical energy density compared to lithium-ion batteries (LIBs) and abundance of elemental sulfur, lithium sulfur (Li-S) batteries have emerged as one of the most promising alternatives among all the post LIB technologies. In particular, the coupling of solid polymer electrolytes (SPEs) with the cell chemistry of Li-S b...
Article
Lithium salts based on perfluorinated sulfonimide anions (PSAs) are promising new electrolyte components for application in next-generation lithium batteries. Several typical symmetric ([(n-CmF2m+1SO2)2N]⁻, m = 0, 1, 2, 3, and 4) and asymmetric ([(FSO2) (n-CmF2m+1SO2)N], m = 1, 2, 4, 6, and 8) PSAs have been extensively investigated in recent years...
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Magnetic properties of maricite (m) and triphlyte (t) polymorphs of NaFePO4 are investigated by combining ab-initio density functional theory with a model Hamiltonian approach, where a realistic Hubbard-type model for magnetic Fe 3d states in NaFePO4 is constructed entirely from first-principles calculations. For these purposes, we perform a compar...
Article
Olivine NaFePO4 is a promising cathode material for Na-ion batteries. Intermediate phases such as Na0.66FePO4 govern phase stability during intercalation-deintercalation processes, yet little is known about Na+ diffusion in NaxFePO4 (0 < x < 1). Here we use an advanced simulation technique, Randomized Shell Mass Generalized Shadow Hybrid Monte Carl...
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Metal–organic frameworks (MOFs) are promising materials for batteries and supercapacitors. However, random crystal orientations and low conductivity can result in poor performance. Designing a convenient method to address these issues is therefore an important challenge. Here we describe an efficient strategy to fabricate self-supported MOF wall-li...
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The search for Si-based anodes capable of undergoing low volume changes during electrochemical operation in rechargeable batteries is ample and active. Here we focus on crystalline Si24, a recently discovered open-cage allotrope of silicon, to thoroughly investigate its electrochemical performance using density functional theory calculations. In pa...
Article
We report the preparation and electrochemical properties of Na3V(PO3)3N made by ammonolysis. Na3V(PO3)3N is reversibly oxidized to Na2V(PO3)3N at high voltage (4.0 V vs. Na⁺/Na⁰ and 4.1 V vs. Li⁺/Li⁰) with an unusually small difference in the insertion/extraction voltage between both alkali metal reference electrodes. In both cases, the voltage hys...
Article
Alkali-metal superoxides are gaining increasing interest as 2p magnetic materials for information and energy storage. Despite significant research efforts on bulk materials, gaps in our knowledge of the electronic and magnetic properties at the nanoscale still remain. Here, we focused on the role that structural details play in determining stabilit...
Article
Cobalt hydroxide is a promising electrode material for supercapacitors due to the high capacitance and long cyclability. However, the energy storage/conversion mechanism of cobalt hydroxide is still vague at the atomic level. Here we shed light on how cobalt hydroxide functions as a supercapacitor electrode at operando conditions. We find that the...
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Supplementary Figures and Supplementary Tables
Article
The discovery of computationally driven materials requires efficient and accurate methods. Density functional theory (DFT) meets these two requirements for many classes of materials. However, DFT-based methods have limitations. One significant shortcoming is the inadequate treatment of weak van der Waals (vdW) interactions, which are crucial for la...
Article
The study of ion transport in electrochem-ically active materials for energy storage systems requires simulations on quantum-atomistic-and meso-scales. The methods accessing these scales not only have to be effective but also well compatible to provide a full description of the underlying processes. We propose to adapt the Generalized Shadow Hybrid...
Article
Full-text available
Solid state electrolytes could address the current safety concerns of lithium-ion batteries as well as provide higher electrochemical stability and energy density. Amongst solid electrolytes contenders, garnet-structured Li7La3Zr2O12 appears as a particularly promising material owing to its wide electrochemical stability window; however its ionic c...
Article
The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K producing adsorbed CHx and COx (x= 2-3) groups. Calculations based on density-functional theory predict a relatively low activation energy of 0.6-0.7 eV for the cleavage of the first C-H bond in...
Article
Transition metal layered oxides are promising cathode materials for sodium-ion batteries. Phase transitions involving different stacking sequences of the oxide layers often plague the electrochemistry of these materials during cycling, which strongly impacts in their electrochemical performance. However, the underlying mechanisms of these processes...
Article
The quest for new sustainable iron-based positive electrode materials for lithium-ion batteries recently led to the discovery of a new family of compounds with the general formula Li2M(SO4)2 with M = transition metal, which presents monoclinic and orthorhombic polymorphs. In terms of electrochemical performances, although both Li2Fe(SO4)2 polymorph...
Article
Ni-CeO2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO2 at temperatures as low as 3...
Article
Ni-CeO2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO2 at temperatures as low as 3...
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Full-text available
Olivine NaFePO4 has recently attracted the attention of the scientific community as promising cathode material for Na-ion batteries. In this work we combine density functional theory (DFT) calculations and high resolution synchrotron X-ray diffraction (HRXRD) experiments to study the phase stability of NaxFePO4 along the whole range of sodium compo...
Article
Rechargeable metal-oxygen batteries are receiving significant interest as a possible alternative to current state of the art lithium ion batteries due to their potential to provide higher gravimetric energies, giving significantly lighter or longer lasting batteries. Recent advances suggest that the Na-O2 battery, in many ways analogous to Li-O2 ye...