Axel Gross

Axel Gross
Ulm University | UULM · Institute of Theoretical Chemistry

Prof. Dr.

About

339
Publications
41,536
Reads
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11,225
Citations
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
December 2004 - present
Ulm University
Position
  • Managing Director
September 1998 - September 2004
Technische Universität München
Position
  • Professor (Associate)
October 1993 - September 1998
Fritz Haber Institute of the Max Planck Society
Position
  • Researcher

Publications

Publications (339)
Article
Full-text available
Employing density functional theory (DFT) calculations and x-ray photoelectron spectroscopy (XPS), we identify products of the reaction of the ionic liquid N,N - butylmethylpyrrolidinum bis(triuoromethylsulfonyl)imide (BMP-TFSI) with lithium in order to model the initial chemical processes contributing to the formation of the solid electrolyte inte...
Preprint
Full-text available
Employing density functional theory (DFT) calculations and x-ray photoelectron spectroscopy (XPS), we identify products of the reaction of the ionic liquid N,N - butylmethylpyrrolidinum bis(trifluoromethylsulfonyl)imide (BMP-TFSI) with lithium in order to model the initial chemical processes contributing to the formation of the solid electrolyte in...
Preprint
In this review, a discussion on renewable sources of energy with clear focus on solar cell applications is presented. Especially, possible future directions for development of dye-sensitized solar cells (DSSCs) are discussed. Dye-sensitized solar cells have become an important topic of research due to its high importance in energy conversion. Curre...
Article
This article reviews recent forays in theoretical modeling of the double layer structure at electrode/electrolyte interfaces by current atomistic and continuum approaches. We will briefly discuss progress in both approaches and present a perspective on how to better describe the electric double layer by combining the unique advantages of each metho...
Article
The Cover Feature illustrates properties of the potential energy surface for charge carriers in spinel solid electrolyte and electrode materials that yield a descriptor for the ion mobility. The descriptor is based on the energetic difference between the two symmetrically different intercalation sites in these materials. This allows to predict the...
Article
While the Mo 6 S 8 chevrel phase is frequently used as cathode material in Mg–ion batteries, theoretical studies on this material are comparatively scarce. The particular structure of the Mo 6 S 8 phase, with rather loosely connected cluster entities, points to the important role of dispersion forces in this material. However, so far this aspect ha...
Article
Bimetallic surfaces allow tailoring their catalytic activity by modifying their composition and/or structure. However, under operating conditions, catalytically active bimetallic structures are often not stable and change their morphology which might reduce their functionality. Still, catalytically active structures do not necessarily need to be th...
Article
Full-text available
Ion mobility is a critical performance parameter not only in electrochemical energy storage and conversion but also in other electrochemical devices. On the basis of first-principles electronic structure calculations, we have derived a descriptor for the ion mobility in battery electrodes and solid electrolytes. This descriptor is entirely composed...
Article
Full-text available
Structures and processes at water/metal interfaces play an important technological role in electrochemical energy conversion and storage, photoconversion, sensors, and corrosion, just to name a few. However, they are also of fundamental significance as a model system for the study of solid−liquid interfaces, which requires combining concepts from t...
Preprint
Full-text available
It is a paradigm in chemistry that chemical reaction are mainly governed by thermodynamics. Within this assumption, reaction rates can be derived from transition state theory which requires a quasi-equilibrium between reactants and activated transition state complexes that is achieved through friction. However, to reach thermal equilibrium through...
Preprint
Full-text available
Density functional theory calculations together with ab initio molecular dynamics (AIMD) simulations have been used to study the solvation, diffusion and transformation of Li+ and LiO2 upon O2 reduction in three organic electrolytes. These processes are critical for the performance of Li-air batteries. Apart from studying the structure of the solva...
Preprint
Full-text available
Alkali metal ion batteries, and in particular Li-ion batteries, have become a key technology for current and future energy storage, already nowadays powering many devices of our daily lives. Due to the inherent complexity of batteries and their components, the use of computational approaches on all length and time scales has been largely evolving w...
Article
Full-text available
Magnesium Batteries Ion mobility is a critical parameter contributing to the performance of batteries. In article number 2100113 by Axel Groß and co-workers, the site preference of ions in battery electrodes and solid electrolytes is determined as a function of volume by quantum chemical calculations. The results reveal that an analysis purely base...
Preprint
Full-text available
While the Mo6S8 chevrel phase is frequently used as cathode material in Mg--ion batteries, theoretical studies on this material are comparatively scarce. The particular structure of the Mo6S8 phase, with rather loosely connected cluster entities, points to the important role of dispersion forces in this material. However, so far this aspect has bee...
Preprint
Full-text available
The surface structures of promising cathode materials for zinc-air batteries, Mn3O4 and Co3O4, have been systematically studied under operating conditions by density functional theory calculations. The environment has been taken into account using grand-canonical schemes both for gas-phase and electrochemical conditions. By analysing the structures...
Preprint
Full-text available
The theoretical modeling of the double layer structure at electrode/electrolyte interfaces by current atomistic and continuum approaches is reviewed. We will briefly discuss recent progress in both approaches and present a perspective on how to better describe the electric double layer by exchanging the unique advantages of each method. First-princ...
Article
Full-text available
Conductive polymers represent a promising alternative to semiconducting oxide electrodes typically used in dye-sensitized cathodes as they more easily allow a tuning of the physicochemical properties. This can then also be very beneficial for using them in light-driven catalysis. In this computational study, we address the coupling of Ru-based phot...
Preprint
Full-text available
Bimetallic surfaces allow tailoring their catalytic activity by modifying their composition and/or structure. However, under operating conditions, catalytically active bimetallic structures are often not stable and change their morphology which might reduce their functionality. Still, catalytically active structures do not necessarily need to be th...
Preprint
Bimetallic surfaces allow tailoring their catalytic activity by modifying their composition and/or structure. However, under operating conditions, catalytically active bimetallic structures are often not stable and change their morphology which might reduce their functionality. Still, catalytically active structures do not necessarily need to be th...
Chapter
Electrochemistry is concerned with processes at the interface between an electron conductor and an ion conductor. The reorganisation of electronic and ionic charge leads to the formation of two oppositely charged layers forming the so-called electric double layer (EDL). This chapter presents the results of molecular dynamics simulations that are ba...
Article
Full-text available
The influence of electrolyte ions on the catalytic activity of electrode/electrolyte interfaces is a controversial topic for many electrocatalytic reactions. Herein, we focus on an effect that is usually neglected, namely, how the local reaction conditions are shaped by nonspecifically adsorbed cations. We scrutinize the oxygen evolution reaction (...
Article
Full-text available
Nickel-based oxides are highly active, cost effective materials for the oxygen evolution reaction in alkaline conditions. Recent experimental studies have revealed the importance of surface deprotonation and alkali metal cation adsorption on the activity of Ni oxide surfaces, in contact with aqueous alkaline electrolyte. As a first step to elucidat...
Preprint
Full-text available
Structures and processes at water/metal interfaces play an important technological role in electro-chemical energy conversion and storage, photoconversion, sensors or corrosion, just to name a few. However, they are also of fundamental significance as a model system for the study of solid-liquid interfaces which requires to combine concepts from ch...
Article
Full-text available
Batteries based on multivalent ions such as magnesium have been attracting considerable attention due to their potential for high energy densities, but their low ion mobility remains an obstacle. Herein, ionic conductivity in spinel host materials, which represent a promising class of cathode and solid‐electrolyte materials in batteries, is address...
Preprint
Full-text available
Conductive polymers represent a promising alternative to semiconducting oxide electrodes typically used in dye-sensitized cathodes as they more easily allow a tuning of the physicochemical properties. This can then also be very beneficial for using them in light-driven catalysis. In this computational study, we address the coupling of Ru-based phot...
Preprint
Conductive polymers represent a promising alternative to semiconducting oxide electrodes typically used in dye-sensitized cathodes as they more easily allow a tuning of the physicochemical properties. This can then also be very beneficial for using them in light-driven catalysis. In this computational study, we address the coupling of Ru-based phot...
Article
Full-text available
Discrimination between electronic and structural effects in metal-support interactions (MSIs) is often hampered by contributions from either one. We report results of a combined experimental/theoretical study that directly demonstrate the action of electronic MSIs, while structural modifications like a partial overgrowth of metal nanoparticles by a...
Preprint
Full-text available
Nickel-based oxides are highly active, cost effective materials for the oxygen evolution reaction in alkaline conditions. Recent experimental studies have revealed the importance of surface deprotonation and alkali metal cation adsorption on the activity of Ni oxide surfaces, in contact with aqueous alkaline electrolyte. As a first step to elucidat...
Preprint
Nickel-based oxides are highly active, cost effective materials for the oxygen evolution reaction in alkaline conditions. Recent experimental studies have revealed the importance of surface deprotonation and alkali metal cation adsorption on the activity of Ni oxide surfaces, in contact with aqueous alkaline electrolyte. As a first step to elucidat...
Article
Tungsten-doped vanadia-based catalysts supported on anatase TiO2 are used to reduce hazardous NO emissions through the selective catalytic reduction of ammonia, but their exact atomistic structure is still largely unknown. In this computational study, the atomistic structure of mixed tungsta–vanadia monolayers on a TiO2 support under typical operat...
Presentation
Semi-tutorial talk about theoretical methods to describe electrode/electrolyte interfaces
Preprint
Full-text available
Tungsten-doped vanadia-based catalysts supported on anatase TiO<sub>2</sub> are used to reduce hazardous NO emissions through the selective catalytic reduction of ammonia, but their exact atomistic structure is still largely unknown. In this computational study, the atomistic structure of mixed tungsta-vanadia monolayers on TiO<sub>2</sub> support...
Preprint
Full-text available
In the area of sustainable energy storage, batteries based on multivalent ions such as magnesium have been attracting considerable attention due to their potential for high energy densities. Furthermore, they are typically also more abundant than, e.g., lithium. However, as a challenge their low ion mobility in electrode materials remains. This stu...
Preprint
Full-text available
In the area of sustainable energy storage, batteries based on multivalent ions such as magnesium have been attracting considerable attention due to their potential for high energy densities. Furthermore, they are typically also more abundant than, e.g., lithium. However, as a challenge their low ion mobility in electrode materials remains. This stu...
Preprint
Full-text available
Based on first-principles electronic structure calculations, we have derived an efficient physical descriptor for the ion mobility in battery electrodes and solid electrolytes which is a critical performance parameter in electrochemical energy storage and conversion. This descriptor is entirely composed of observables that are easily accessible: io...
Preprint
Full-text available
Ion mobility is a critical performance parameter in electrochemical energy storage and conversion, but also in other electrochemical devices. Based on first-principles electronic structure calculations, we have derived a descriptor for the ion mobility in battery electrodes and solid electrolytes. This descriptor is entirely composed of observables...
Article
One of the difficulties limiting the development of high capacity Li-O 2 batteries is the positive electrode passivation by the discharge product Li 2 O 2 which is deposited mostly due to the second electron transfer of oxygen reductionwhich requires the presence of Li ⁺ in the Stern layer. To suppress the passivation and shift the reaction zone of...
Article
The development of suitable electrode materials remains a great challenge for alternative battery technologies such as sodium-ion and potassium-ion batteries; especially with regard to the negative electrode. Herein, Fe-doped CeO2 (Ce0.9Fe0.1O2-δ), which has very recently been introduced as a new anode material for lithium-ion batteries, is investi...
Article
The Cover Feature illustrates that foreign atoms in single‐atom surface alloys can usually only migrate by vacancy‐mediated diffusion. Combining density functional theory calculations with kinetic Monte Carlo simulation, we show how the separation and recombination of the foreign atom and a surface vacancy influence structural changes of the bimeta...
Article
Full-text available
Electrochemical interfaces between an electrode and an electrolyte are often covered by ions from the solution. These adsorbed ions can strongly modify the properties of the interfaces. Furthermore, in electrocatalysis the reacting species typically have to get into contact with the surface of the electrocatalyst where then the reaction proceeds. H...
Article
Full-text available
The deposition of zinc from aqueous solutions is of great practical importance, and it also serves as a prototype for the deposition of divalent ions. Both experiment and theory agree, that it takes place in two steps. Previous theoretical work [1] had suggested that the step, Zn+++e-→Zn+ takes place in the outer sphere, but gave a prohibitively hi...
Article
Full-text available
In this work we aim towards the molecular understanding of the solid electrolyte interphase (SEI) formation at the electrode electrolyte interface (EEI). Herein, we investigated the interaction between the battery-relevant ionic liquid (IL) 1-butyl-1-methylpyrrolidinium bis(trifluoromethyl-sulfonyl)imide (BMP-TFSI), Li and a Co3O4(111) thin film mo...
Article
Full-text available
Ru(II)-bipyridine complexes connected with p-type semiconductors (p-SCs) are promising systems for photocatalytic applications such as in dye-sensitised solar cells (DSSCs). The photosensitizer-semiconductor interface governed by the anchoring group is of vital importance for the electronic properties of the systems as it determines the long-term s...
Article
We have performed density functional theory calculations to explore the possibility to overcome the linear scaling relations in the oxygen reduction reaction (ORR) using local inhomogeneities on Pt-based surface alloys, supported Pt monolayers, and Pt islands. We demonstrate that invoking inequivalent neighboring reaction sites allows overcoming th...
Article
Full-text available
Bimetallic surfaces can exhibit an improved catalytic activity through tailoring the concentration and/or the arrangement of the two metallic components. However, in order to be catalytically active, the active bimetallic surface structure has to be stable under operating conditions. Typically, structural changes in metals occur via vacancy diffusi...
Article
Full-text available
The combination of sulfur (S) as cathode with a Mg anode is a promising approach for batteries because of the high theoretical capacity (1,672 mAh g-1) as well as the abundance and relatively low cost of these elements. However, up to now Mg/S batteries face serious drawbacks like a large overpotential between charge/discharge cycles, rapid capacit...
Article
Full-text available
Periodic density functional theory calculations have been performed to study the migration of various charge carriers in spinel‐type MgSc2Se4. This compound exhibits low barriers for Mg ion diffusion, making it a potential candidate for solid electrolytes in Mg-ion batteries. In order to elucidate the decisive factors for the ion mobility in spinel...
Article
Full-text available
Vanadium oxides have been recognized to be among the most promising positive electrode materials for aqueous zinc metal batteries (AZMBs). However, their underlying intercalation mechanisms are still vigorously debated. To shed light on the intercalation mechanisms, high-performance δ-V2O5 is investigated as a model compound. Its structural and ele...
Article
Full-text available
The co-adsorption of sulfate, bisulfate and hydrogen on Pt(111) and Au(111) electrodes was studied based on periodic density functional calculations with the aqueous electrolyte represented by both explicit and implicit solvent models. The influence of the electrochemical control parameters such as the electrode potential and pH was taken into acco...
Article
In article number 2000783, Gabriele Giuli, Dominic Bresser and co‐workers report the use of Fe‐doped CeO2 as a new active material for lithium‐ion batteries, which combines an insertion‐type mechanism with the reduction of the Fe dopant at the atomic level. Such a fundamentally new mechanism allows for a tripling of the achievable capacity, accompa...
Article
Carbon-based anodes are technologically highly relevant for Li and post-Li ion batteries. While the storage mechanism of Li in graphite is essentially understood, the alkali metal intercalation in carbon derivatives has been strongly debated. Here, we present a combined computational and experimental study on the intercalation of Li and Na in hard...
Article
The Cover Feature shows a battery anode together with needle‐like dendrites under strain. Using density functional theory calculations, the influence of strain on the self‐diffusion and other properties of metal anodes is studied. Thus, the question is addressed whether strain can modify the harmful and hazardous growth of dendrites in batteries. M...
Data
A kMC trajectory simulated at 268 K with a parameter E_pair=0.08eV on Ru(0001) surface. The blue and red circles represent CO and O adatoms, respectively.
Article
Recently, a surprisingly fast diffusion of O atoms on a fully CO-covered Ru(0001) surface has been observed using video-rate scanning tunneling microscopy. This finding has been explained by a so-called door-opening mechanism in which intermittent diffusion pathways are created by local density fluctuations in the CO layer. Using input from density...