Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB))

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Computational Study of a Copper-Catalyzed Synthesis of Fluoroalcohols from Alkylboranes and Ketones
(American Chemical Society, 2025-09-03) Gómez-Mudarra, Francisco A.; Aullón López, Gabriel; Jover Modrego, Jesús
Fluoroalcohols are a class of organic compounds containing one or more fluorine atoms together with an alcohol group in their molecular structure. These fluorinated species have a wide range of applications due to their unique properties and are used in medicine and electronics. Herein, we propose a new synthetic procedure, promoted by a copper(I) catalyst, for preparing fluoroalcohols from alkylboranes and symmetric ketones. The reaction has been computationally explored to propose a plausible mechanism, which allows identifying the rate-limiting step and quantitatively evaluating the electronic effects of each substrate on the overall reactivity. These DFT calculations suggest that the combination of electron-poor ketones with electron-rich alkylboranes produce the most efficient catalytic systems for preparing fluoroalcohols. Microkinetic modeling of the studied systems allow the prediction of the activation barrier limit to achieve fully functional reactions and multilinear regression techniques provide a methodology to estimate the overall reaction barriers in a simple manner, opening the way for proposing new catalytic systems.
Kinetico-mechanistic insights into the photodynamic process of AuI complexes with the CNC6H4NNC6H5 (iso-Ph) azobenzene ligand
(Royal Society of Chemistry, 2025-01) Raïch Panisello, Ot; Jover Modrego, Jesús; Puigjaner, Cristina; Ferrer García, Montserrat; Martínez López, Manuel, 1957-
A family of neutral isocyanide monoazo AuI complexes [AuCl(iso-Ph)], [Au(C6F5)(iso-Ph)] and [Au(C[triple bond, length as m-dash]Cpy)(iso-Ph)] (iso-Ph being CN–C6H4–N[double bond, length as m-dash]N–Ph) and a closely related cationic bisazo symmetrical derivative, [Au(iso-Ph)2](OTf), have been prepared. All the compounds have been structurally characterized using the conventional techniques HRMS, NMR, UV-Vis and IR spectroscopy. Moreover, the structure of the [AuCl(iso-Ph)] compound has been determined by XRD. These compounds undergo more efficient trans-to-cis photoisomerisation upon irradiation at 365 nm than that of the free iso-Ph ligand. The reverse cis-to-trans thermal process has been investigated using different solvents, temperatures and pressures to determine the values of the activation parameters and thus, the corresponding isomerisation mechanism. A change in the operating mechanism (from charge-separated rotational to inversional) has been observed upon going from the monoazo to the bisazo compounds. This effect has been attributed to the difference in the electronic density at the AuI centre in the transition state between the unsymmetrical and the symmetrical species.
A versatile luminescent probe for sensing and monitoring amyloid proteins
(Elsevier B.V., 2024-12-01) Vázquez Bigas, Guillem; Espargaró Colomé, Alba; Caballero Hernández, Ana Belén; Di Pede Mattatelli, Ania; Busquets i Viñas, Ma. Antonia; Nawrot, Daria; Sabaté Lagunas, Raimon; Nicolás Galindo, Ernesto; Juárez Jiménez, Jordi; Gámez Enamorado, Patrick
A modified lysine residue containing an environment-sensitive moiety was prepared through a straightforward synthesis, and its fluorescent properties were examined. The new fluorescent sensor, DMN-BocK, can monitor amyloid aggregation processes associated with neurodegenerative diseases such as Alzheimer’s or Parkinson’s. DMN-BocK offers advantages over classical amyloid-specific dyes like Thioflavins or Congo Red because it is (1) available to detect a broader range of amyloid structures; (2) useful both in vitro and in cellulo; (3) capable of differentiating amyloid structures, providing information on the binding site microenvironment; and (4) a synthon than can be incorporated into protein sequences to gain further structural information. Our findings suggest that DMN-based amino-acid probes have a strong potential to become a sensor of choice for in vitro and in cellulo studies of amyloid aggregation in drug discovery assays.
New series of mononuclear β-diketonate cerium(iii) field induced single-molecule magnets
(Royal Society of Chemistry, 2024-05-08) Tubau Ribot, Ànnia; Gómez Coca, Silvia; Speed Castro, Saskia; Font Bardia, Ma. Mercedes; Vicente Castillo, Ramón
Five new β-diketonate Ce3+ mononuclear complexes, [Ce(Btfa)3(H2O)2] (1), [Ce(Btfa)3(phen)] (2), [Ce (Btfa)3(bipy)] (3), [Ce(Btfa)3(terpy)] (4) and [Ce(Btfa)3(bathophen)(DMF)] (5), where Btfa− = 4,4,4-trifluoro-1- phenyl-1,3-butanedionate, phen = 1,10-phenanthroline, bipy = 2,2’-bipyridyl, terpy = 2,2’:6’,2’’-terpyridine and bathophen = 4,7-diphenyl-1,10-phenanthroline, have been synthesized and structurally characterized through X-ray diffraction of single crystals. The central Ce3+ atom displays a coordination number of 8 for 1, 2 and 3 and of 9 for 4 and 5. Under a 0 T external magnetic field, none of the given compounds exhibits single molecule magnet (SMM) behaviour. However, a small magnetic field, between 0.02 and 0.1 T, is enough for all the compounds to exhibit slow relaxation of the magnetization. A comprehensive magnetic analysis, with experimental magnetic data and ab initio calculations, was undertaken for all the complexes, and the study highlights the significance of the different spin relaxation mechanisms that must be considered for a Ce3+ lanthanide ion.
A Leap from Diradicals to Tetraradicals by Topological Control of π-Conjugation.
(American Chemical Society, 2024-09-20) Betkhoshvili, Sergi; Poater i Teixidor, Jordi; Moreira, Ibério de Pinho Ribeiro; Bofill i Villà, Josep M.
In this work, we explore the series of diradical(oid)s based on 2,2′-(5,11-dihydroindolo[3,2-b]carbazole-3,9-diyl)-dimalononitrile (further referred to as PH). Hydrogen atoms in the central benzenoid (CB) ring of PH are substituted by the seriesof substituents with various lengths of π-conjugated chain and electron-donating or electron-withdrawing properties to study howthey modulate the diradical character of the parent compound. The diradical character of molecules increases up to 88−89% by twogroups doubly bonded to both sides of the CB ring of PH in para relative positions. This breaks the direct π-conjugation betweenunpaired electrons that gives rise to two radical centers and restricts the minimal polyradical identity of the compound todiradical. We show that diradicals and tetraradicals can be designed, and their polyradical character can be modulated by controlling the topology of π-conjugation as long as there is sufficient aromatic stabilization. Henceforth, the bridge between diradicals and tetraradicals is established, leading to the tetraradical(oid) molecule, which has been predicted to have narrow low-spin to high-spin energy gaps in our recent Letter.
Ferrofluid-based bioink for 3d printed skeletal muscle tissues with enhanced force and magnetic response
(John Wiley & Sons, 2025-06-25) Fuentes Llanos, Judith; Guix Noguera, Maria; Cenev, Zoran M.; Bakenecker, Anna; Ruiz González, Noelia; Beaune, Grégory; Timonen, Jaakko V. I.; Sánchez Ordóñez, Samuel; Magdanz, Veronika
3D printing has emerged as a transformative technology in several manufacturing processes, being of particular interest in biomedical research for allowing the creation of 3D structures that mimic native tissues. The process of tissue 3D printing entails the construction of functional, 3D tissue structures. In this article, the integration of ferrofluid consisting of iron oxide nanoparticles into muscle cell-laden bioink is presented to obtain a 3D printed magnetically responsive muscle tissue, i.e., the ferromuscle. Using extrusion-based methods, the seamless integration of biocompatible ferrofluids are achieved to cell-laden hydrogels. The resulting ferromuscle tissue exhibits improved tissue differentiation demonstrated by the increased force output upon electrical stimulation compared to muscle tissue prepared without ferrofluid. Moreover, the magnetic component originating from the iron oxide nanoparticles allows magnetic guidance, as well as good cytocompatibility and biodegradability in cell culture. These findings offer a new versatile fabrication approach to integrate magnetic components into living constructs, with potential applications as bioactuators and for future integration in smart, functional muscle implants.
Field-Induced Slow Relaxation of the Magnetization in Two Families of [MIILnIII] Complexes
(American Chemical Society, 2024-07-03) Costa Villén, Ernesto; Font Bardia, Ma. Mercedes; Mayans Ayats, Júlia; Escuer Fité, Albert
A family of discrete dinuclear complexes [MIILnIII] (M = Cu, Ni and Ln = Ce, Gd, Tb, Dy, Er, Yb) has been synthesized from the use of the compartmental Schiff base ligand H4L (3,3′-((1E,1′E)-(ethane-1,2-diylbis- (azaneylylidene)) bis(methaneylylidene))bis(benzene-1,2-diol)), obtained from the condensation of ethylenediamine and 2,3-dihydroxybenzaldehyde. All of the complexes have been structurally and magnetically characterized. The dynamic magnetic measurements show that the [CuIILnIII] and [NiIILnIII] derivatives exhibit ac response as a function of the d-cation. Noteworthily, the isotropic GdIII complexes exhibit a slow relaxation of magnetization.
Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
(American Chemical Society, 2024-08-06) Recio-Poo, Miguel; Morales García, Ángel; Illas i Riera, Francesc; Bromley, Stefan Thomas
Ab initio atomistic thermodynamics (AIAT) has become an indispensable tool to estimate Gibbs free energy changes for solid surfaces interacting with gaseous species relative to pressure (p) and temperature (T). For such systems, AIAT assumes that solid vibrational contributions to Gibbs free energy differences cancel out. However, the validity of this assumption is unclear for nanoscale systems. Using hydrated titania nanoparticles (NPs) as an example, we estimate the vibrational contributions to the Gibbs free energy of hydration (ΔGhyd(T,p)) for arbitrary NP size and degree of hydration. Comparing ΔGhyd(T,p) phase diagrams for NPs when considering these contributions (AIATnano) relative to a standard AIAT approach reveals significant qualitative and quantitative differences, which only become negligible for large systems. By constructing a size-dependent ΔGhyd(T,p) phase diagram, we illustrate how our approach can provide deeper insights into how nanosytems interact with their environments, with many potential applications (e.g., catalytic nanoparticles, biological colloids, nanoparticulate pollutants).
Comprehensive Density Functional and Kinetic Monte Carlo Study of CO2 Hydrogenation on a Well-Defined Ni/CeO2 Model Catalyst: Role of Eley-Rideal Reactions
(American Chemical Society, 2024-02-16) Lozano-Reis, Pablo; Gamallo Belmonte, Pablo; Sayós Ortega, Ramón; Illas i Riera, Francesc
A detailed multiscale study of the mechanism of CO2 hydrogenation on a well-defined Ni/CeO2 model catalyst is reported that couples periodic density functional theory (DFT) calculations with kinetic Monte Carlo (kMC) simulations. The study includes an analysis of the role of Eley–Rideal elementary steps for the water formation step, which are usually neglected on the overall picture of the mechanism, catalytic activity, and selectivity. The DFT calculations for the chosen model consisting of a Ni4 cluster supported on CeO2 (111) show large enough adsorption energies along with low energy barriers that suggest this catalyst to be a good option for high selective CO2 methanation. The kMC simulations results show a synergic effect between the two 3-fold hollow sites of the supported Ni4 cluster with some elementary reactions dominant in one site, while other reactions prefer the another, nearly equivalent site. This effect is even more evident for the simulations explicitly including Eley–Rideal steps. The kMC simulations reveal that CO is formed via the dissociative pathway of the reverse water–gas shift reaction, while methane is formed via a CO2 → CO → HCO → CH → CH2 → CH3 → CH4 mechanism. Overall, our results show the importance of including the Eley–Rideal reactions and point to small Ni clusters supported on the CeO2 (111) surface as potential good catalysts for high selective CO2 methanation under mild conditions, while very active and selective toward CO formation at higher temperatures.
Theoretical Prediction of Core-Level Binding Energies: Analysis of Unexpected Errors
(American Chemical Society, 2024-02-08) Sousa Romero, Carmen; Bagus, Paul S.; Illas i Riera, Francesc
The analysis of the C(1s) and O(1s) core-level binding energies (CLBEs) of selected molecules computed by means of total energy Hartree–Fock (ΔSCF-HF) differences shows that in some cases, the calculated values for the C(1s) are larger than the experiment, which is unexpected. The origin of these unexpected errors of the Hartree–Fock ΔSCF BEs is shown to arise from static, nondynamical, electron correlation effects which are larger for the ion than for the neutral system. Once these static correlation effects are included by using complete active space self-consistent field (CASSCF) wave functions that include internal correlation terms, the resulting ΔSCF BEs are, as expected, smaller than measured values.
An Extension of the Stern–Volmer Equation for Thermally Activated Delayed Fluorescence (TADF) Photocatalysts
(American Chemical Society, 2024-10-11) Limburg, Bart
Fluorescence quenching experiments are essential mechanistic tools in photoredox catalysis, allowing one to elucidate the first step in the catalytic cycle that occurs after photon absorption. Thermally activated delayed fluorescence (TADF) photocatalysts, however, yield nonlinear Stern–Volmer plots, thus requiring an adjustment to this widely used method to determine the efficiency of excited state quenching. Here, we derive an extension of the Stern–Volmer equation for TADF fluorophores that considers quenching from both the singlet and triplet excited states and experimentally verify it with fluorescence quenching experiments using the commonly employed TADF-photocatalyst 4CzIPN, and multiple-resonance TADF-photocatalyst QAO with three different quenchers in four solvents. The experimental data are perfectly described by this new equation, which in addition to the Stern–Volmer quenching constants allows for the determination of the product of intersystem and reverse intersystem crossing quantum yields, a quantity that is independent of the quencher.
Unveiling the synergy between surface terminations and Boron configuration in Boron-based Ti3C2 MXenes electrocatalysts for Nitrogen reduction reaction
(American Chemical Society, 2024-10-03) Meng, Ling; Viñes Solana, Francesc; Illas i Riera, Francesc
The performance of B-containing Ti3C2 MXenes as catalysts for the nitrogen reduction reaction (NRR) is scrutinized using density functional theory methods on realistic models and accounting for working conditions. The present models include substituted and adsorbed boron along with various mixed surface terminations, primarily comprising −O and −OH groups, while considering the competitive hydrogen evolution reaction (HER) as well. The results highlight that substituted and low-coordinate adsorbed boron atoms exhibit a very high N2 adsorption capability. For NRR, adsorbed B atoms yield lower limiting potentials, especially for surfaces with mixed −O/–OH surface groups, where the latter participate in the reaction lowering the hydrogenation reaction energy costs. The NRR does also benefit of having B adsorbed on the surface which on moderate −OH terminated model displays the lowest limiting potential of −0.83 V, competitive to reference Ru and to HER. The insights derived from this comprehensive study provide guidance in formulating effective MXene-based electrocatalysts for NRR.
Pathway to Polyradicals: A Planar and Fully π-Conjugated Organic Tetraradical(oid)
(American Chemical Society, 2024-01-01) Betkhoshvili, Sergi; Moreira, Ibério de Pinho Ribeiro; Poater i Teixidor, Jordi; Bofill i Villà, Josep M.
In this work, we provide a general strategy to stabilize the ground state of polyradical(oid)s and make higher spin states thermally accessible. As a proof of concept, we propose to merge two planar fully π-conjugated diradical(oid)s to obtain a planar and cross-conjugated tetraradical(oid). Using multireference quantum chemistry methods, we show that the designed tetraradical(oid) is stabilized by aromaticity and delozalization in the π-system and has six thermally accessible spin states within 1.72 kcal/mol. Analysis of the electronic structure of these six states of the tetraradical(oid) shows that its frontier π-system consists of two weakly interacting subsystems: aromatic cycles and four unpaired electrons. Conjugation between unpaired electrons, which favors closed-shell structures, is mitigated by delocalization and the aromaticity of the bridging groups, leading to the synergistic cross-coupling between two diradical(oid) subunits to stabilize the tetraradical(oid) electronic structure.
Contrasting Metallic (Rh0) and Carbidic (2D-Mo2C MXene) Surfaces in Olefin Hydrogenation Provides Insights on the Origin of the Pairwise Hydrogen Addition
(American Chemical Society, 2024-08-06) Meng, Ling; Pokochueva, Ekaterina; Chen, Zixuan; Fedorov, Alexey; Viñes Solana, Francesc; Illas i Riera, Francesc; Koptyug, Igor V.
Kinetic studies are vital for gathering mechanistic insights into heterogeneously catalyzed hydrogenation of unsaturated organic compounds (olefins), where the Horiuti–Polanyi mechanism is ubiquitous on metal catalysts. While this mechanism envisions nonpairwise H2 addition due to the rapid scrambling of surface hydride (H*) species, a pairwise H2 addition is experimentally encountered, rationalized here based on density functional theory (DFT) simulations for the ethene (C2H4) hydrogenation catalyzed by two-dimensional (2D) MXene Mo2C(0001) surface and compared to Rh(111) surface. Results show that ethyl (C2H5*) hydrogenation is the rate-determining step (RDS) on Mo2C(0001), yet C2H5* formation is the RDS on Rh(111), which features a higher reaction rate and contribution from pairwise H2 addition compared to 2D-Mo2C(0001). This qualitatively agrees with the experimental results for propene hydrogenation with parahydrogen over 2D-Mo2C1–x MXene and Rh/TiO2. However, DFT results imply that pairwise selectivity should be negligible owing to the facile H* diffusion on both surfaces, not affected by H* nor C2H4* coverages. DFT results also rule out the Eley–Rideal mechanism appreciably contributing to pairwise addition. The measurable contribution of the pairwise hydrogenation pathway operating concurrently with the dominant nonpairwise one is proposed to be due to the dynamic site blocking at higher adsorbate coverages or another mechanism that would drastically limit the diffusion of H* adatoms.
An Unusual His/Asp Dyad Operates Catalysis in Agar-Degrading Glycosidases
(American Chemical Society, 2024-11-01) Sagiroglugil, Mert; Nin Hill, Alba; Ficko-Blean, Elizabeth; Rovira i Virgili, Carme
Agarose motifs, found in agars present in the cell walls of red algae, consist of alternating units of d-galactose (G) and α-3,6-anhydro-l-galactose (LA). Glycoside hydrolases from family 117 (GH117) cleave the terminal α-1,3-glycosidic bonds, releasing LA units. Structural studies have suggested that these enzymes use unconventional catalytic machinery, involving a histidine (His302) as a general acid rather than a carboxylic residue as in most glycosidases. By means of quantum mechanics/molecular mechanics metadynamics, we investigated the reaction mechanism of Phocaeicola plebeius GH117, confirming the catalytic role of His302. This residue shares a proton with a neighbor aspartate residue (Asp320), forming a His/Asp dyad. Our study also reveals that, even though the sugar unit at the –1 subsite (LA) can adopt two conformations, 4C1 and 1,4B, only the latter is catalytically competent, defining a 1,4B → [4E]‡ → 1,4B (→ 4C1) conformational itinerary. This mechanism may be applicable to similar enzymes with a His/Asp dyad in their active sites, such as GH3 β-N-acetylglucosaminidase and GH156 sialidase. These insights enhance our understanding of glycosidase catalytic strategies and could inform the engineering of enzymes for the more efficient processing of seaweed.
A Cartesian encoding graph neural network for crystal structure property prediction: application to thermal ellipsoid estimation
(Royal Society of Chemistry (RSC), 2025-12-01) Sole Gomez, Jaume Alexandre; Mosella-Montoro, Albert; Cardona, Joan; Gómez Coca, Silvia; Aravena Ponce, Daniel Alejandro; Ruiz Sabín, Eliseo; Ruiz-Hidalgo, Javier
In the diffraction resolution of crystal structures, thermal ellipsoids are a critical parameter that is usually more difficult to determine than atomic positions. These ellipsoids are quantified through Anisotropic Displacement Parameters (ADPs), which provide critical insights into atomic vibrations within crystalline structures. ADPs reflect the thermal behaviour and structural properties of crystal structures. However, traditional methods to compute ADPs are computationally intensive. This paper presents CartNet, a novel graph neural network (GNN) architecture designed to predict properties of crystal structures efficiently by encoding the atomic structural geometry to the Cartesian axes and the temperature of the crystal structure. Additionally, CartNet employs a neighbour equalization technique for message passing to help emphasise the covalent and contact interactions and a novel Cholesky-based head to ensure valid ADP predictions. Furthermore, a rotational SO(3) data augmentation technique has been proposed during the training phase to generalize unseen rotations. To corroborate this procedure, an ADP dataset with over 200 000 experimental crystal structures from the Cambridge Structural Database (CSD) has been curated. The model significantly reduces computational costs and outperforms existing previously reported methods for ADP prediction by 10.87%, while demonstrating a 34.77% improvement over the tested theoretical computation methods. Moreover, we have employed CartNet for other already known datasets that included different material properties, such as formation energy, band gap, total energy, energy above the convex hull, bulk moduli, and shear moduli. The proposed architecture outperformed previously reported methods by 7.71% in the JARVIS dataset and 13.16% in the Materials Project dataset, proving CarNet's capability to achieve state-of-the-art results in several tasks. The project website with online demo available at: https://www.ee.ub.edu/cartnet.
Atomic and Electronic Structures of Co-Doped In2O3 from Experiment and Theory
(American Chemical Society, 2024-05-29) Voccia, Maria; Kapse, Samadhan; Sayago-Carro, Rocío; Gómez-Cerezo, Natividad; Fernández-García, Marcos; Kubacka, Anna; Viñes Solana, Francesc; Illas i Riera, Francesc
The synthesis and properties of stoichiometric, reduced, and Co-doped In2O3 are described in the light of several experimental techniques, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), ultraviolet (UV)–visible spectroscopy, porosimetry, and density functional theory (DFT) methods on appropriate models. DFT-based calculations provide an accurate prediction of the atomic and electronic structure of these systems. The computed lattice parameter is linearly correlated with the experimental result in the Co concentration ranging from 1.0 to 5.0%. For higher Co concentrations, the theoretical-experimental analysis of the results indicates that the dopant is likely to be preferentially present at surface sites. The analysis of the electronic structure supports the experimental assignment of Co2+ for the doped material. Experiments and theory find that the presence of Co has a limited effect on the material band gap.
CO2 hydrogenation in Ru single atom catalyst encapsulated in silicalite: a DFT and microkinetic modelling study
(American Chemical Society, 2024-09-22) Cánovas Montes, Manuel Antonio; Gracia Gil, Alejandro; Sayós Ortega, Ramón; Gamallo Belmonte, Pablo
The critical levels of CO2 emissions reached in the past decade have encouraged researchers into finding techniques to reduce the amount of anthropogenic CO2 expelled to the atmosphere. One possibility is to capture the produced CO2 from the source of emission or even from air (i.e., direct air capture) by porous materials (e.g., zeolites and MOFs). Among the different usages of captured CO2, its conversion into light fuels such as methane, methanol, and formic acid is essential for ensuring the long-awaited circular economy. In the last years, single-atom catalysts encapsulated in zeolites have been considered to this purpose since they exhibit a high selectivity and activity with the minimum expression of catalytic species. In this study, a detailed mechanism composed by 47 elementary reactions, 42 of them in both forward and reverse directions and 5 of them that correspond to the desorption of gas products just forwardly studied), has been proposed for catalytic CO2 hydrogenation over Ru SAC encapsulated in silicate (Ru1@S-1). Periodic density functional theory (DFT) calculations along with microkinetic modeling simulations at different temperatures and pressures were performed to evaluate the evolution of species over time. The analysis of the results shows that carbon monoxide is the main gas produced, followed by formic acid and formaldehyde. The rate analysis shows that CO(g) is formed mainly through direct dissociation of CO2 (i.e., redox mechanism), whereas COOH formation is assisted by OH. Moreover, the Campbell’s degree of rate control analysis suggests that the determining steps for the formation of CO(g) and CH2O(g) gas species are their own desorption processes. The results obtained are in line with recent experimental and theoretical results showing that Ru1 SACs are highly selective to CO(g), whereas few atom clusters as Ru4 increase selectivity toward methane formation.
Determining the chemical ordering in nanoalloys by considering atomic coordination types
(American Institute of Physics (AIP), 2024-10-04) Farris, Riccardo; Neyman, Konstantin M.; Bruix Fusté, Albert
The energetically most favorable chemical ordering of bimetallic nanoparticles can be characterized by combining global optimization algorithms and surrogate energy models. The latter approximate the energy of nanoalloys relying on structural descriptors, training models, and data. Here, we systematically evaluate the performance of highly data-efficient topological descriptors [Kozlov et al., Chem. Sci. 6, 3868 (2015)] for predicting the energies of metal nanoalloys with different chemical orderings. We also introduce a new descriptor based on atomic coordination types, which results in a less data-efficient and interpretable approach, but improves the general accuracy and the quantification of orderings in the inner parts of nanoparticles. The capacity of both the original and new approaches in combination with a basin hopping algorithm is illustrated by generating convex hulls of PdZn nanoalloys and predicting the resulting active surface site distribution as a function of particle composition. Finally, we show how these approaches can be combined with machine-learning adsorption models in electrocatalysis studies for a fast evaluation of the reactivity landscape of targeted nanoalloys.
Mechanochemistry of degree two.
(Springer Verlag, 2024-12-05) Quapp, Wolfgang; Bofill i Villà, Josep M.
We simplify some proposed formulas for hydrostatic pressure on a molecule byG. Subramanian, N. Mathew and J. Leiding, J.Chem.Phys. 143, 134109 (2015). Weapply the formulas to an artificial triatom ABC whose potential energy surface isformed by a combination of Morse curves.

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