Sofia Calero

Eindhoven University of Technology | TUE · Department of Applied Physics

Entropies for alkane isomers longer than C10 are computed using our recently developed linear regression model for thermochemical properties which is based on second-order group contributions. The computed entropies show excellent agreement with experimental data and data from Scott’s tables which are obtained from a statistical mechanics-based cor...

Phonons in chiral crystal structures can acquire a circular polarization, becoming chiral themselves. Chiral phonons carry a spin angular momentum, which is observable in heat currents, and, via coupling to the electron spin, in spin currents. Two-dimensional (2D) hybrid halide perovskites comprise a class of direct band gap semiconductors that can...

The ability to efficiently predict adsorption properties of zeolites can be of large benefit in accelerating the design process of novel materials. The existing configuration space for these materials is wide, while existing molecular simulation methods are computationally expensive. In this work, we propose a model which is 4 to 5 orders of magnit...

Linear regression (LR) is used to predict thermochemical properties of alkanes at temperatures (0–1000) K to study chemical reaction equilibria inside zeolites. The thermochemical properties of C1 until C10 isomers reported by Scott are used as training data sets in the LR model which is used to predict these properties for alkanes longer than C10...

We present RASPA3, a molecular simulation code for computing adsorption and diffusion in nanoporous materials and thermodynamic and transport properties of fluids. It implements force field based classical Monte Carlo/molecular dynamics in various ensembles. In this article, we introduce the new additions and changes compared to RASPA2. RASPA3 is r...

The energy storage capability of supercapacitors (SCs) strongly depend on the operating cell voltage of the electrolytes of choice. In this regard, the inherent distinct electrochemical stability of cations and anions is a factor of relevance for the operating cell voltage. The use of double salts sharing one ion has been described as an approach t...

The confinement effect of porous materials on the thermodynamical equilibrium of the CO2 hydrogenation reaction presents a cost-effective alternative to transition metal catalysts. In metal–organic frameworks, the type of metal center has a greater impact on the enhancement of formic acid production than the scale of confinement resulting from the...

With the use of chiral organic cations in two-dimensional metal halide perovskites, chirality can be induced in the metal halide layers, which results in semiconductors with intriguing chiral optical and spin-selective transport properties. The chiral properties strongly depend upon the temperature, despite the basic crystal symmetry not changing f...

Lead halide perovskites are well known for their exceptional photophysical and electronic properties, which have placed them at the forefront of challenging optoelectronic applications and solar‐to‐fuel conversion. However, their air/water instability, combined with their toxicity, is still a critical problem that has slowed down their commercializ...

Using chiral organic cations in two-dimensional metal halide perovskites, chirality can be induced in the metal halide layers, which results in semiconductors with intriguing chiral optical and spin-selective transport properties. The chiral properties strongly depend on temperature, despite the basic crystal symmetry not changing fundamentally. We...

Efficiently predicting properties of porous crystalline materials has great potential to accelerate the high throughput screening process for developing new materials, as simulations carried out using first principles models are often computationally expensive. To effectively make use of Deep Learning methods to model these materials, we need to ut...

Correction for ‘How fast do defects migrate in halide perovskites: insights from on-the-fly machine-learned force fields’ by Mike Pols et al. , Chem. Commun. , 2023, 59 , 4660–4663, https://doi.org/10.1039/D3CC00953J.

All-inorganic halide perovskites have received a great deal of attention as attractive alternatives to overcome the stability issues of hybrid halide perovskites that are commonly associated with organic cations. To find a compromise between the optoelectronic properties of CsPbI3 and CsPbBr3, perovskites with CsPb(BrxI1–x)3 mixed compositions are...

The building climate industry and its influence on energy consumption have consequences on the environment due to the emission of greenhouse gasses. Improving the efficiency of this sector is essential...

For industrial applications, materials used in water treatment must be stable in moist conditions for easy handling and cost-effectiveness. UiO-66 has been identified as a promising material for this purpose....

The adsorption performance of ZIF-71 towards two common volatile organic compounds such as chlorobenzene and phenol has been evaluated using a number of experimental techniques and gran canonical Monte Carlo...

The building climate industry and its influence on energy consumption have consequences on the environment due to the emission of greenhouse gasses. Improving the efficiency of this sector is essential to reduce the effect on climate change. In recent years, the interest in porous materials in applications such as heat pumps has increased for their...

Metal-organic frameworks (MOFs) have become promising materials for multiple applications due to their controlled dimensionality and tunable properties. The incorporation of chirality into their frameworks opens new strategies for chiral separation, a key technology in the pharmaceutical industry as each enantiomer of a racemic drug must be isolate...

This work aimed to investigate the adsorption of toluene in UiO-66 materials. Toluene is a volatile, aromatic organic molecule that is recognized as the main component of VOCs. These compounds are harmful to the environment as well as to living organisms. One of the materials that allows the capture of toluene is the UiO-66. A satisfactory represen...

In this work, two industrial dual-step pressure swing adsorption (PSA) processes were designed and simulated to obtain high-purity methane, CO2, and syngas from a gas effluent of a CO2 electroreduction reactor using different design configurations. Among the set of zeolites that was investigated using Monte Carlo and molecular dynamics simulations,...

We present the RUPTURA code (https://github.com/iraspa/ruptura) as a free and open-source software package (MIT license) for (1) the simulation of gas adsorption breakthrough curves, (2) mixture prediction using methods like the Ideal Adsorption Solution Theory (IAST), segregated-IAST and explicit isotherm models, and (3) fitting of isotherm models...

The main challenge of the position is to create a methodological framework to build in silico DNA for materials, where materials are identified by their ‘genome’ and their properties. To achieve this, we use simulation of materials based on first principle (molecular simulation) and scaled by generative machine learning (ML). There is a PhD positio...

Efficiently predicting properties of porous crystalline materials has great potential to accelerate the high throughput screening process for developing new materials, as simulations carried out using first principles model are often computationally expensive. To effectively make use of Deep Learning methods to model these materials, we need to uti...

The migration of defects plays an important role in the stability of halide perovskites. It is challenging to study defect migration with experiments or conventional computer simulations. The former lacks an atomic-scale resolution and the latter suffers from short simulation times or a lack of accuracy. Here, we demonstrate that machine-learned fo...

Ideal Adsorbed Solution Theory (IAST) is a common method for modelling mixture adsorption isotherms based on pure component isotherms. When the adsorbent has distinct adsorption sites, the segregated version of IAST (SIAST) provides improved adsorbed loadings compared to IAST. We have adopted the concept of SIAST and applied it to an explicit isoth...

Reducing carbon dioxide emissions has become a must in society, making it crucial to find alternatives to supply the energy demand. Adsorption-based cooling and heating technologies are receiving attention for thermal energy storage applications. In this paper, we study the adsorption of polar working fluids in hydrophobic and hydrophilic zeolites...

Metal-Organic Frameworks (MOFs) offer considerable potential for applications in adsorption due to their large pore volumes and surface areas. Studies on mechanical stability of MOFs are scarce. Seminal experimental work has shed a new light on the role that elastic constants play in establishing the structural stability of the prototypical ZIF-8 M...

There is a growing interest in the development of routes to produce formic acid from CO2, such as the electrochemical reduction of CO2 to formic acid. The solubility of CO2 in the electrolyte influences the production rate of formic acid. Here, the dependence of the CO2 solubility in aqueous HCOOH solutions with electrolytes on the composition and...

We have investigated MOR, MFI, and FAU zeolites to acquire a better understanding of the aluminum T-position effect on the heat of adsorption of ammonia and water at a microscopic level. We performed Monte Carlo simulations using RASPA code to obtain the heats of adsorption of water and ammonia in zeolites with one Al-substitution. We show that the...

Structural defects in metal–organic frameworks can be exploited to tune material properties. In the case of UiO-66 material, they may change its nature from hydrophobic to hydrophilic and therefore affect the mechanism of adsorption of polar and non-polar molecules. In this work, we focused on understanding this mechanism during adsorption of molec...

Ordered Nanoporous Metals (ONMs) form a new family of nanoporous materials composed only of pure metals. The expected impact is considerable from combining the ordered nanopore structure of MOFs, zeolites and carbon schwartzites with the robustness and electronic conductivity of metals. Little is known about their stability and structural features....

The commercialization of perovskite solar cells is hindered by the poor long-term stability of the metal halide perovskite (MHP) light-absorbing layer. Solution processing, the common fabrication method for MHPs, produces polycrystalline films with a wide variety of defects, such as point defects, surfaces, and grain boundaries. Although the optoel...

Reducing carbon dioxide emissions has become a must in society, being crucial to find alternatives to supply the energy demand. Adsorption-based cooling and heating technologies are receiving attention for thermal energy storage applications. In this paper, we study the adsorption of polar working fluids in hydrophobic and hydrophilic zeolites by m...

Separation of volatile organic compounds is one of the most studied processes in industry. TAMOF-1 is a homochiral metal–organic framework with a crystalline network of interconnected ≈1 nm channels and has high thermal and chemical stability. Thanks to these features, it can resolve racemic mixtures of chiral drugs as a chiral stationary phase in...

The metal-organic framework MOF-808 contains Zr6O8 nodes with a high density of vacancy sites, which can incorporate carboxylate-containing functional groups to tune chemical reactivity. Although the postsynthetic methods to modify the chemistry of the Zr6O8 nodes in MOFs are well known, tackling these alterations from a structural perspective is s...

The commercialization of perovskite solar cells is hindered by the poor long-term stability of the metal halide perovskite (MHP) light absorbing layer. Solution processing, the common fabrication method for MHPs, produces polycrystalline films with a wide variety of defects, such as point defects, surfaces, and grain boundaries. Although the optoel...

Understanding the water splitting mechanism in photocatalysis is a rewarding goal as it will allow producing clean fuel for a sustainable life in the future. However, identifying the photocatalytic mechanisms by modeling photoactive nanoparticles requires sophisticated computational techniques based on multiscale modeling. In this review, we will s...

In this paper, we investigate the thermostructural properties of a type of silicon-based nanomaterials, which we refer to as SiC@Si nanocomposites, formed by SiC crystalline nanoparticles (with the cubic phase), embedded within an amorphous Si matrix. We have followed an in silico approach to characterize the mechanical and thermal behaviour of the...

We combine experiments and simulations to study the adsorption of water in several UiO-66 frameworks (ideal and defect-containing structures). We propose a new set of charges for the frameworks that accurately provides the water-structure interaction at the molecular level. The new set is suitable for predicting water adsorption in the ideal UiO-66...

The rapidly rising level of carbon dioxide in the atmosphere resulting from human activity is one of the greatest environmental problems facing our civilization today. Most technologies are not yet sufficiently developed to move existing infrastructure to cleaner alternatives. Therefore, techniques for capturing carbon dioxide from emission sources...

We present several new major features added to the Monte Carlo (MC) simulation code Brick-CFCMC for phase- and reaction equilibria calculations (https://gitlab.com/ETh_TU_Delft/Brick-CFCMC). The first one is thermodynamic integration for the computation of excess chemical potentials (μex). For this purpose, we implemented the computation of the ens...

Using a combination of molecular simulations techniques, we evaluate the structural tunability of the metal azolate framework with zeolitic RHO topology, MAF-6. Two mechanisms are explored to induce hydrophilicity to this hydrophobic material. The study at a molecular level of water adsorption takes place under a variety of conditions. On a first s...

The dehydration of bioalcohols is considered one of the major factors contributing to the cost of biofuel production. In this study, liquid phase separation of water from methanol and ethanol in a siliceous MFI pervaporation membrane was studied by performing concentration gradient driven molecular dynamic (CGD-MD) simulations. CGD-MD simulations w...

For many years, the performance of Li-ion batteries (LIBs) and supercapacitors (SCs) has relied mainly on two factors, (1) the optimization of electrodes composition and/or structure and (2) the selection of salts or ionic liquids (ILs) matching well with the compositional and/or structural features of electrodes. Solvents included in electrolyte c...

In this work we use classical methods to develop an accurate model able to describe the interactions between the molecule of water and the hematite surface. We study the variation of the interaction energy between the water molecule and the surface regarding some geometrical aspects such as the proximity to different parts of the surface, the molec...

p>The dehydration of bioalcohols is considered one of the major factors contributing to the cost of biofuel production. In this study, liquid phase separation of water from methanol and ethanol in a siliceous MFI pervaporation membrane was studied by performing concentration gradient driven molecular dynamic (CGD-MD) simulations. CGD-MD simulations...

According to the ISO 14687-2:2019 standard, the water content of H2 fuel for transportation and stationary applications should not exceed 5 ppm (molar). To achieve this water content, zeolites can be used as a selective adsorbent for water. In this work, a computational screening study is carried out for the first time to identify potential zeolite...