
Axel GrossUlm University | UULM · Institute of Theoretical Chemistry
Axel Gross
Prof. Dr.
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Introduction
Axel Gross currently works at the Institute of Theoretical Chemistry, Ulm University, and at the Helmholtz-Institute Ulm. Axel does research in Theoretical Chemistry, Surface Chemistry and Electrochemistry. Their current projects are related to (electro-)chemical energy conversion and storage at interfaces and in bulk materials. Axel is one of the three spokespersons of the Cluster of Excellence POLiS (Post-Li Energy Storage) funded by the German Science Foundation.
Additional affiliations
October 1993 - September 1998
September 1998 - September 2004
December 2004 - present
Publications
Publications (439)
Continuing our investigation of electronic metal−support interactions (EMSIs) in heterogeneous catalysis, we have investigated the influence of the position and the number of O-vacancies on their stabilization by the Ru nanorod, on the charge transfer from the support to the metal, and on CO adsorption on the Ru nanorod. Employing density functiona...
In this work, the origin of Na ⁺ /vacancy orderings in P2-type Na x Ni y Mn 1− y O 2 is investigated. A general guideline to suppress Na ⁺ /vacancy orderings in P2-type Na x MO 2 cathode active materials is postulated.
Chlorinated trityl radicals functionalized with electron-donating groups are promising red-emitting materials for optoelectronic and spintronic applications, overcoming the spin-statistical limit of conventional emitters. Donor functionalization induces charge transfer character, enhancing photoluminescence quantum yield, which depends on the donor...
Chlorinated trityl radicals functionalized with electron-donating groups are promising red-emitting materials for optoelectronic and spintronic applications, overcoming the spin-statistical limit of conventional emitters. Donor functionalization induces charge transfer character, enhancing photoluminescence quantum yield, which depends on the donor...
Sodium-ion batteries are emerging as a cost-effective and sustainable alternative to lithium-ion technology. Prussian blue compounds are demonstrating considerable potential as cathode materials, offering exceptional structural stability and rapid sodium-ion diffusion capabilities. However, in spite of the importance of Prussian Blue for the emergi...
Batteries using multivalent charge carriers present a promising alternative to traditional Li-ion technology, offering the potential for higher energy densities and often relying on more abundant elements. However, their ion mobility within the electrolyte and cathode is generally lower than that of monovalent carriers due to stronger electrostatic...
By preventing water decomposition on the electrode surface, the solid-electrolyte interphase (SEI) plays a crucial role in enhancing the electrochemical stability of water-in-salt electrolytes, thereby facilitating their commercialization. In this study, we employ density functional theory calculations to explore the initial stages of SEI formation...
Sustainable batteries are key for powering electronic devices of the future, with aqueous zinc-ion batteries (AZIBs) standing out for their use of abundant, readily available elements, and safer production processes. Among the various electrode materials studied for AZIBs, the Chevrel Phase, Mo6S8 has shown promise due to its open framework, but is...
Chloride–ion batteries (CIBs) offer a compelling alternative to conventional battery systems, particularly in applications demanding cost‐effectiveness and resource sustainability. However, the development of tailored electrode materials remains a critical bottleneck for CIB advancement. In this study, an untapped class of perovskite‐based material...
The magnesium chalcogenide spinel MgSc2Se4 with high Mg‐ion room‐temperature conductivity has recently attracted interest as solid electrolyte for magnesium ion batteries. Its ionic/electronic mixed‐conducting nature and the influence of the spinel composition on the conductivity and Mg²⁺ migration barrier are yet not well understood. Here, results...
Sodium‐ion batteries (SIBs) show promise for the next generation of energy storage technology but face significant challenges in regards to stability due in part to uncontrolled degradation of the solid electrolyte interphase (SEI). Kinetic Monte Carlo (kMC) modeling is uniquely suited to provide molecular‐scale insight on the phenomena that influe...
Chloride ion batteries (CIBs) offer a compelling alternative to lithium-ion systems, particularly in applications demanding cost-effectiveness and resource sustainability. However, the development of tailored electrode materials remains a critical bottleneck for CIB advancement. In this study, we synthesized an untapped class of perovskite-based ma...
The magnesium chalcogenide spinel MgSc2Se4 with high Mg-ion room-temperature conductivity has recently attracted interest as solid electrolyte for magnesium ion batteries. Its ionic/electronic mixed-conducting nature and the influence of the spinel composition on the conductivity and Mg2+ migration barrier are yet not well understood. Here, results...
Metal–water interfaces are central to many electrochemical, (electro)catalytic, and materials science processes and systems. However, our current understanding of their thermodynamic properties is limited by the scarcity of accurate experimental and computational data and procedures. In this work, thermodynamic quantities for metal–water interface...
Structures formed by dense CO adsorption layers can provide information about the balance between molecule–surface and molecule–molecule interactions. However, in many cases, the structure models are not clear. Using density functional theory (DFT) and scanning tunneling microscopy (STM), we have investigated the high-coverage CO layer on the Ru(00...
Metal–water interfaces are central to many electrochemical, (electro)catalytic, and materials science processes and systems. However, our current understanding of their thermodynamic properties is limited by the scarcity of accurate experimental and computational data and procedures. In this work, thermodynamic quantities for metal–water interface...
Using periodic density functional theory calculations we have investigated the stability, electronic properties and CO adsorption properties of bimetallic Pt Ag surfaces, including pseudomorphic Ag film covered Pt(111) surfaces and...
Improving electrochemical ion intercalation capacity and kinetics in layered host materials is a critical challenge to further develop lithium-ion batteries, as well as emerging cell chemistries based on ions beyond lithium. Modification of the nanoconfined interlayer space within host materials by synthetic pillaring approaches has emerged as a pr...
The nanoscale form of the Chevrel phase, Mo6S8, is demonstrated to be a highly efficient zinc-free anode in aqueous zinc ion hybrid supercapacitors (ZIHSCs). The unique morphological characteristics of the...
Offering a compelling combination of safety and cost-effectiveness, water-in-salt (WiS) electrolytes have emerged as promising frontiers in energy storage technology. Still, there is a strong demand for research and development efforts to make these electrolytes ripe for commercialization. Here, we present a first-principles-based molecular dynamic...
Metal–water interfaces are central to many electrochemical, (electro)catalytic, and materials science processes and systems. However, our current understanding of their thermodynamic properties is limited by the scarcity of accurate experimental and computational data and procedures. In this work, thermodynamic quantities for metal–water interface...
Using periodic density functional theory calculations we have investigated the stability, electronic properties and CO adsorption properties of bimetallic Pt Ag surfaces, including pseudomorphic Ag film covered Pt(111) surfaces and PtxAg1-x/Pt(111) monolayer surface alloys. The data provide detailed insights into the relative stabilities of differe...
As an example for bimetallic surfaces in general, we have systematically investigated the thermodynamic surface properties of bimetallic Ag/Pt(111) and Ag/Pd(111) surfaces, including pseudomorphic Ag film covered surfaces and M1Ag3/M(111) (M = Pt, Pd) monolayer surface alloys, by periodic density functional theory calculations. Employing larger, sy...
The research of new electrode materials such as sodium intercalation compounds is key to meet the challenges of future demands of sustainable energy storage. For these batteries, the intercalation behavior on the micro-scale is governed by a complex interplay of chemical, electrical and mechanical forces strongly influencing the overall cell perfor...
Conversion of CO2 to hard carbon is an interesting technology for the removal of carbon dioxide from the atmosphere. Recently, it was shown that CeO2 can selectively catalyze this reaction, but we still lack information regarding the reaction mechanism. Using density functional theory modeling, we explore possible reaction mechanisms that allow for...
Due to its negligible capacity with respect to sodium intercalation, graphite is not suited as anode material for sodium ion batteries. Hard carbon materials, on the other hand, provide reasonably high capacities at low insertion potential, making them a promising anode materials for sodium (and potassium) ion batteries. The particular nanostructur...
We report the synergistic combination of Pd(OAc)2 and Ag2O for the oxidative C–H arylation of (poly)fluoroarenes with aryl pinacol boronates (Ar‐Bpin) in DMF as the solvent. This procedure can be conducted easily in air, and without using additional ligands, to afford the fluorinated unsymmetrical biaryl products in up to 98% yield. Experimental st...
Ion mobility in electrolytes and electrodes is a critical factor influencing the performance of batteries. Low ion mobility is for example one of the major factors reducing the range of battery-electric vehicles in winter time. On the other hand, with respect to the ion mobility in battery cathode materials there are scaling relations linking large...
Offering a compelling combination of safety and cost-effectiveness, Water-in-Salt (WiS) electrolytes have emerged as promising frontiers in energy storage technology. Still, there is a strong demand for research and development efforts to make these electrolytes ripe for commercialization. Here we present a first-principles based molecular dynamics...
The development of competitive rechargeable Mg batteries is hindered by the poor mobility of divalent Mg ions in cathode host materials. In this work, we explore the dual cation co-intercalation strategy to mitigate the sluggishness of Mg²⁺ in model TiS2 material. The strategy involves pairing Mg²⁺ with Li⁺ or Na⁺ in dual-salt electrolytes in order...
We present a density functional theory study of the initial steps of chlorine deposition on the Mg(0001) surface. Such processes occur in chloride-ion batteries in which lithium and magnesium are used as anode materials. In addition, it is also of fundamental interest, as halide adsorption on metal electrodes is an important process in interfacial...
In the pursuit of more affordable battery technologies, potassium-ion batteries (KIBs) have emerged as a promising alternative to lithium-ion systems, owing to the abundance and wide distribution of potassium resources....
Conversion of CO2 to hard carbon is an interesting technology for the removal of carbon dioxide from the atmosphere. Recently, it was shown that CeO2 can selectively catalyse this reaction but we still lack information regarding the reaction mechanism. Using density functional theory (DFT) modelling we explore possible reaction mechanisms that allo...
The field of sustainable energy storage and conversion has witnessed increasing interest in ionic conductors due to their potential applications in electrochemical devices such as electrodes and solid electrolytes. In this study, we employed a combination of density functional theory investigations and artificial intelligence techniques to develop...
The reduction of CO 2 is a promising route for the synthesis of renewable energy carriers and the removal of CO 2 from the atmosphere to limit global warming. These negative emission technologies (NETs) require the conversion of carbon dioxide into a stable and easily storable form[1]. However, despite its potential, the development of suitable CO...
At the interface between two conducting phases, an electric double layer (EDL) forms. In interfacial electrochemistry, such an EDL is present at the interface between the electrode and the electrolyte. The structure of the EDL can be crucial for all processes that occur at such interfaces, for example in electrochemical energy conversion and storag...
Ion mobility in electrolytes and electrodes is an important performance parameter in electrochemical devices, particularly in batteries. In this review, the authors concentrate on the charge carrier mobility in crystalline battery materials where the diffusion basically corresponds to hopping processes between lattice sites. However, in spite of th...
The electrification of the transportation sector exacerbates all issues concerning the use of critical materials in state‐of‐the‐art batteries and, therefore, urges the development of new technologies based on potentially greener and more abundant materials. One research trend is the substitution of Li as shuttle ion with other elements such as Na,...
Zinc‐based batteries offer good volumetric energy densities and are compatible with environmentally friendly aqueous electrolytes. Zinc‐ion batteries (ZIBs) rely on a lithium‐ion‐like Zn²⁺‐shuttle, which enables higher roundtrip efficiencies and better cycle life than zinc‐air batteries. Manganese‐oxide cathodes in near‐neutral zinc sulfate electro...
The increasing need for electrochemical energy storage drives the development of post‐lithium battery systems. Among the most promising new battery types are sodium‐based battery systems. However, like its lithium predecessor, sodium batteries suffer from various issues like parasitic side reactions, which lead to a loss of active sodium inventory,...
Based on quantum chemical calculations, we predict strong solvatochromism in a light‐driven molecular photocatalyst for hydrogen generation, that is we show that the electronic and optical properties of the photocatalyst strongly depend on the solvent it is dissolved in. Our calculations in particular indicate a solvent‐dependent relocation of the...
In order to obtain atomistic insights into the initial stages of the formation of the solid electrolyte interphase (SEI) in Na ion or Na metal batteries, we employ surface chemistry experiments and DFT calculations to study the interactions and reactions between a Na surface and the ionic liquid (IL) 1‐butyl‐1‐methylpyrrolidinium bis(trifluoromethy...
Prussian Whites (PW) have gained attention for their potential application as high energy density cathodes in Na‐ion batteries. However, the rhombohedral phase of this compound still remains elusive. This study addresses the electronic and structural properties of the rhombohedral host material, as well as its ionic conductivity. Using periodic den...
Secondary batteries using multivalent cations as ionic charge carriers have attracted increasing attention in recent years due to the high theoretical energy density provided by multi‐electron redox reactions. However, the high charge density of these cations inevitably leads to sluggish kinetics of ion migration at room temperature, which poses a...
We present a density functional theory study of the initial steps of chlorine deposition on the Mg(0001) surface. Such processes occur in chloride-ion batteries in which lithium and magnesium are used as anode materials. In addition, it is also of fundamental interest, as halide adsorption on metal electrodes is an important process in interfacial...
The electrification of the transportation sector exacerbates all issues concerning the use of critical materials in state-of-the-art batteries and, therefore, urges the development of new technologies based on potentially greener and more abundant materials. One research trend is the substitution of Li as shuttle ion with other elements such as Na,...
Zinc-based batteries offer good volumetric energy densities and are compatible with environmentally friendly aqueous electrolytes. Zinc-ion batteries (ZIBs) rely on a lithium-ion-like Zn$^{2+}$-shuttle, which enables higher roundtrip efficiencies and better cycle life than zinc-air batteries. Manganese-oxide cathodes in near-neutral zinc sulfate el...
Ion mobility in electrolytes and electrodes is an important performance parameter in electrochemical devices, particularly in batteries. In this review, we concentrate on the charge carrier mobility in crystalline battery materials where the diffusion basically corresponds to hopping processes between lattice sites. However, in spite of the seem- i...
The high ionic conductivity and good oxidation stability of halide-based solid electrolytes evoke strong interest in this class of materials. Nonetheless, the superior oxidative stability compared to sulfides comes at the expense of limited stability toward reduction and instability against metallic lithium anodes, which hinders their practical use...
Accurate modeling of highly concentrated aqueous solutions, such as water-in-salt (WiS) electrolytes in battery applications, requires proper consideration of polarization contributions to atomic interactions. Within the force field molecular dynamics (MD) simulations, the atomic polarization can be accounted for at various levels. Nonpolarizable f...
The increasing need for electrochemical energy storage drives the development of post-lithium battery systems. Among the most promising new battery types are sodium-based battery systems. However, like its lithium predecessor, sodium batteries suffer from various issues like parasitic side reactions, which lead to a loss of active sodium inventory,...
Conversion of CO2 to hard carbon is an interesting technology for the removal of carbon dioxide from the atmosphere. Recently, it was shown that CeO2 can selectively catalyse this reaction but we still lack information regarding the reaction mechanism. Using density functional theory (DFT) modelling we explore possible reaction mechanisms that allo...
The research of new electrode materials such as sodium intercalation compounds is key to meet the challenges of future demands of sustainable energy storage. For these batteries, the intercalation behaviour on the micro-scale is governed by a complex interplay of chemical, electrical and mechanical forces strongly influencing the overall cell perfo...
The transition from lithium‐based energy storage to post lithium systems plays a crucial part in achieving an environmentally sustainable energy infrastructure. Prime candidates for the replacement of lithium are sodium and potassium batteries. Despite being critical to battery performance, the solid electrolyte interphase (SEI) formation process f...
The modelling of electrochemical interfaces between a liquid electrolyte and an electrode from a quantum chemical perspective is typically done by performing ab initio molecular dynamics simulations. Thus the statistically nature of the electrolyte structure can be taken into account by performing the proper averages. However, in order to obtain re...
The diffusion of adsorbed O atoms on a CO-covered Ru(0001) surface has recently been explained by a “door-opening” mechanism which is driven by fluctuations in the CO layer. Here, we analyze how this mechanism changes at a higher CO coverage than the 0.33 monolayers applied in the previous study and, therefore, lower concentrations of empty sites....
The transition from lithium-based energy storage to post lithium systems plays a crucial part in achieving an environmentally sustainable energy infrastructure. Prime candidates for the replacement of lithium are sodium and potassium batteries. Despite being critical to battery performance, the solid electrolyte interphase (SEI) formation process f...
Mg batteries with oxide cathodes have the potential to significantly surpass existing Li-ion technologies in terms of sustainability, abundance, and energy density. However, Mg intercalation at the cathode is often severely hampered by the sluggish kinetics of Mg$^{2+}$ migration within oxides. Here we report a combined theoretical and experimental...
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The cathode material Na$_x$FePO$_4$ of sodium-ion batteries exhibits complex phase segregation thermodynamics with the existence of an intermediate phase, and large volume change during (dis)charging. A virtual multiscale modeling chain is established to construct a 3D anisotrop...
To model a NaOTF Water-in-Salt (WiS) electrolyte using classical Molecular Dynamics (MD) simulations, we explore various force fields where atomic polarization is accounted for at three different levels: a non-polarizable all-atom force field where polarization is only implicitly included in its Van der Waals interaction parameters, the same force...