Sofia Calero

• Professor
• Professor (Full) at Eindhoven University of Technology

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...

UiO-66, reported in 2008, inspired the ongoing chemistry of the group 4 metal-organic frameworks and it is still one of the most studied MOFs due to its exceptional stability. The...

Stability of metal-organic frameworks is a key factor for many applications in some fields that require working at harsh conditions. It is known that a large number of MOFs are vulnerable to humid air. It means that when they are exposed to water, a structural collapse of the crystal happens. In this work, Molecular Dynamics simulations using a Rea...

In this work, we analyze the influence of small adsorbates on the vibrational spectra of Mg- and Zn-metal-organic framework MOF-74 by means of first-principles calculations. In particular, we consider the adsorption of four representative species of different interaction strengths: Ar, CO2, H2O, and NH3. Apart from a comprehensive characterization...

We compare the industrial viability of two emerging technologies for CO2 capture from flue gases, i.e., adsorption in porous commercial zeolites and biomass production by microalgae. Our study is organized in two steps: first, the best system is selected (either zeolite type or microalgae strain). Second, their performance is quantified and their a...

Computational methods to calculate the properties of zeolites in gas adsorption and separation have proven to be a valuable complement to experimental work. Molecular simulation provides a molecular understanding of the mechanisms involved in the adsorption, desorption, and transport. The accuracy and reliability of the predictions depend on the mo...

High‐performance energy‐storage devices are receiving great interest in sustainable terms as a required complement to renewable energy sources to level out the imbalances between supply and demand. Besides electrode optimization, a primary objective is also the judicious design of high‐performance electrolytes combining novel ionic liquids (ILs) an...

January 11, 2021 (online) Registration (free but compulsory) via: www.iraspa.org Contact: raspaworkshop2021@gmail.com This workshop/school focuses on a practical understanding of visualization and molecular simulation of nanoporous materials and fluids, using iRASPA and RASPA. RASPA is well known for force field-based molecular simulation of adsor...

Aqueous dilutions of deep eutectic solvents (DESs) have lately allowed exploring new and more demanding applications where neat DESs are not capable to perform well. However, the use of DES dilutions with non-aqueous hydrogen-bond-forming solvents remains basically unexplored. It is worth noting the obvious interest of using organic solvents in tho...

Competitive adsorption of water is an important issue in the adsorption-based industrial processes of bio- and flue gases separation. The dehumidification of gases prior to separation would increase process complexity and lower its economic interest. In this work, large-scale computational screening was applied to identify Metal-Organic Frameworks...

Metal halide perovskites (MHPs) are nowadays one of the most studied semiconductors due to their exceptional performance as active layers in solar cells. Although MHPs are excellent solid-state semiconductors, they are also ionic compounds, where ion migration plays a decisive role in their formation, their photovoltaic performance and their long-t...

Ammonia is an important chemical compound used in a wide range of applications. This makes its capture, purification and recovery necessary. We combine experimental and molecular simulation techniques to identify the molecular mechanisms ruling the adsorption of ammonia in pure and high silica zeolites. To reproduce accurately the interaction betwe...

Separation of benzene and cyclohexane is one of the greatest challenges in industry. Their close boiling points and similar properties make them difficult compounds to separate. In this context, adsorption-based separation using zeolites or aluminosilicates is a promising technology. In the present work, we combine experimental measurements, densit...

Syngas is traditionally used in industry for production of fuels in the kerosene, gasoline and diesel range via Fischer-Tropsch, for the manufacture of bulk chemicals like ammonia, methanol and dimethyl ether and for synthesis of a whole array of fine chemicals. The carbon monoxide/hydrogen ratio of the syngas is an important design variable to max...

Metal halide perovskites (MHPs) are nowadays one of the most studied semiconductors due to their exceptional performance as active layers in solar cells. Although MHPs are excellent solid-state semiconductors, they are also ionic compounds, where ion migration plays a decisive role in their formation, their photovoltaic performance and their long-t...

In this work we propose the OCEAN-algorithm, a method for the analysis and selection of the best performing material and working conditions for an efficient separation of carbon dioxide and methane from biogas. Molecular simulation and intelligent computational techniques joint forces to generate a reliable database of adsorption values with an opt...

Adsorption of n-alkanes from pentane to decane (C5–C10) in zeolites LTA (ITQ-29 and 5A) and FAU (dealuminated high-silica Na-FAU, NaY, and NaX) as well as branched hexane isomers in FAU was investigated by means of experimental quasi-equilibrated temperature programmed desorption and adsorption (QE-TPDA) and theoretical Monte Carlo molecular simula...

Deep eutectic solvents (DESs) are lately expanding their use to more demanding applications upon aqueous dilution thanks to the preservation of the most appealing properties of the original DESs while overcoming some of their most important drawbacks limiting their performance, like viscosity. Both experimental and theoretical works have studied th...

Water adsorption within zeolites of the Linde Type A (LTA) structure plays an important role in processes of water removal from solvents. For this purpose, knowing in which adsorption sites water is preferably found is of interest. In this paper, the distribution of water within LTA is investigated in several aluminum-substituted frameworks ranging...