Publications
27 results found
Pedretti E, Restuccia P, Righi MC, 2023, Xsorb: A software for identifying the most stable adsorption configuration and energy of a molecule on a crystal surface, Computer Physics Communications, Vol: 291, ISSN: 0010-4655
Molecular adsorption is the first important step of many surface-mediated chemical processes, from catalysis to lubrication. This phenomenon is controlled by physical/chemical interactions, which can be accurately described by first-principles calculations. Several computational tools have been developed to study molecular adsorption based on high throughput/automatized approaches in recent years. However, these tools can sometimes be over-sophisticated for non-expert users. Here we present Xsorb, a Python-based program for identifying the accurate adsorption energy and geometry of complex molecules on crystalline (reconstructed) surfaces. The program automatically samples the potential energy surface (PES) that describes the molecule-surface interaction by generating several adsorption configurations through symmetry operations. The set of the most representative ones is automatically identified through a fast pre-optimization scheme. Finally, the PES global minimum is identified through a full structural optimization process. We show the program capabilities through an example consisting of a hydrocarbon molecule, 1-hexene, adsorbed over the (110) surface of iron and the reconstructed (001) surface of diamond. This program, despite its conceptual simplicity, is very effective in reducing the computational workload usually associated with the creation and optimization of several adsorption configurations. Program summary: Program title: Xsorb CPC Library link to program files: https://doi.org/10.17632/kv97tgybx8.1 Developer's repository link: https://gitlab.com/triboteam/xsorbed/ Licensing provisions: CC by 4.0 Programming language: Python (version 3.7 and above) and Quantum ESPRESSO (for the ab initio calculations). Nature of problem: Identifying the most stable adsorption configuration of a molecule over a substrate and compute its adsorption energy. Solution method: Creating a Python-based code that generates many adsorption configurations with different molecul
Benini F, Bassoli N, Restuccia P, et al., 2023, Interaction of Water and Oxygen Molecules with Phosphorene: An Ab Initio Study., Molecules, Vol: 28
Phosphorene, the 2D form of black phosphorus, has recently attracted interest for optoelectronic and tribological applications. However, its promising properties are affected by the strong tendency of the layers to oxidize in ambient conditions. A significant effort has been made to identify the role of oxygen and water in the oxidation process. In this work, we introduce a first-principles study of the phosphorene phase diagram and provide a quantitative estimate of the interaction of pristine and fully oxidized phosphorene layers with oxygen and water molecules. Specifically, we study oxidized layers with oxygen coverages of 25% and 50% that keep the typical anisotropic structure of the layers. We found that hydroxilated and hydrogenated phosphorene layers are both energetically unfavorable, leading to structural distortions. We also studied the water physisorption on both pristine and oxidized layers, finding that the adsorption energy gain doubled on the oxidized layers, whereas dissociative chemisorption was always energetically unfavorable. At the same time, further oxidation (i.e., the dissociative chemisorption of O2) was always favorable, even on oxidized layers. Ab initio molecular dynamics simulations of water intercalated between sliding phosphorene layers showed that even under harsh tribological conditions water dissociation was not activated, thus further strengthening the results obtained from our static calculations. Overall, our results provide a quantitative description of the interaction of phosphorene with chemical species that are commonly found in ambient conditions at different concentrations. The phase diagram that we introduced confirms the tendency of phosphorene layers to fully oxidize due to the presence of O2, resulting in a material with improved hydrophilicity, a piece of information that is relevant for the application of phosphorene, e.g., as a solid lubricant. At the same time, the structural deformations found for the H- and OH- t
Restuccia P, Losi G, Chehaimi O, et al., 2023, High-Throughput First-Principles Prediction of Interfacial Adhesion Energies in Metal-on-Metal Contacts., ACS Appl Mater Interfaces, Vol: 15, Pages: 19624-19633
Adhesion energy, a measure of the strength by which two surfaces bind together, ultimately dictates the mechanical behavior and failure of interfaces. As natural and artificial solid interfaces are ubiquitous, adhesion energy represents a key quantity in a variety of fields ranging from geology to nanotechnology. Because of intrinsic difficulties in the simulation of systems where two different lattices are matched, and despite their importance, no systematic, accurate first-principles determination of heterostructure adhesion energy is available. We have developed robust, automatic high-throughput workflow able to fill this gap by systematically searching for the optimal interface geometry and accurately determining adhesion energies. We apply it here for the first time to perform the screening of around a hundred metallic heterostructures relevant for technological applications. This allows us to populate a database of accurate values, which can be used as input parameters for macroscopic models. Moreover, it allows us to benchmark commonly used, empirical relations that link adhesion energies to the surface energies of its constituent and to improve their predictivity employing only quantities that are easily measurable or computable.
de Tomas C, Alabidun S, Chater L, et al., 2023, Doping carbon electrodes with sulfur achieves reversible sodium ion storage, JPhys Energy, Vol: 5
We present a combination of experiments and theory to study the effect of sulfur doping in hard carbons anodes for sodium-ion batteries. Hard carbons are synthesised through a two step process: hydrothermal carbonisation followed by pyrolysis of a biomass-derived carbon precursor. Subsequent sulfur doping is introduced via chemical-vapour deposition. The resulting sulfur-doped hard carbon shows enhanced sodium storage capacity with respect to the pristine material, with significantly improved cycling reversibility. Atomistic first principles simulations give insight into this behaviour, revealing that sulfur chemisorbed onto the hard carbon increases the sodium adsorption energies and facilitates sodium desorption. This mechanism would increase reversible Na storage, confirming our experimental observations and opening a pathway towards more efficient Na-ion batteries.
Peeters S, Losi G, Restuccia P, et al., 2022, Unraveling the mechanism to form MoS2 lubricant layers from MoDTC by ab initio simulations, APPLIED SURFACE SCIENCE, Vol: 606, ISSN: 0169-4332
Antonov P, Restuccia P, Righi MC, et al., 2022, Attractive curves: the role of deformations in adhesion and friction on graphene, NANOSCALE ADVANCES, Vol: 4, Pages: 4175-4184, ISSN: 2516-0230
Restuccia P, Ahmad EA, Harrison NM, 2022, A transferable prediction model of molecular adsorption on metals based on adsorbate and substrate properties, PHYSICAL CHEMISTRY CHEMICAL PHYSICS, Vol: 24, Pages: 16545-16555, ISSN: 1463-9076
- Author Web Link
- Cite
- Citations: 2
Losi G, Cutini M, Restuccia P, et al., 2022, Modeling phosphorene and MoS2 interacting with iron: lubricating effects compared to graphene, JOURNAL OF NANOSTRUCTURE IN CHEMISTRY, ISSN: 2008-9244
Kousar K, Dowhyj M, Walczak MS, et al., 2022, Corrosion inhibition in acidic environments: key interfacial insights with photoelectron spectroscopy, FARADAY DISCUSSIONS, Vol: 236, Pages: 374-388, ISSN: 1359-6640
- Author Web Link
- Cite
- Citations: 1
Restuccia P, 2021, First-Principles Simulation-Nano-Theory, CRYSTALS, Vol: 11
Kousar K, Walczak MS, Ljungdahl T, et al., 2021, Corrosion inhibition of carbon steel in hydrochloric acid: Elucidating the performance of an imidazoline-based surfactant, Corrosion Engineering Science and Technology, Vol: 180, Pages: 1-8, ISSN: 0007-0599
A combination of electrochemical measurement and interface analysis have been applied to characterise the interaction of OMID, an exemplar imidazoline-based corrosion inhibitor, with carbon steel in 1 M hydrochloric acid. Corrosion inhibition efficiency data indicate that excellent performance is achieved well below the critical micelle concentration. High resolution X-ray photoelectron spectra demonstrate that, as the corrosion rate decreases, the interface evolves towards one comprising OMID bound to film-free carbon steel. This latter result provides key input for those researchers attempting to predict corrosion inhibitor functionality through atomic scale interfacial modelling, and so identify next generation chemistries.
Peeters S, Restuccia P, Loehle S, et al., 2020, Tribochemical Reactions of MoDTC Lubricant Additives with Iron by Quantum Mechanics/Molecular Mechanics Simulations, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 124, Pages: 13688-13694, ISSN: 1932-7447
- Author Web Link
- Cite
- Citations: 15
Losi G, Restuccia P, Righi MC, 2020, Superlubricity in phosphorene identified by means of ab initio calculations, 2D MATERIALS, Vol: 7, ISSN: 2053-1583
- Author Web Link
- Cite
- Citations: 23
Restuccia P, Ferrario M, Righi MC, 2020, Quantum Mechanics/Molecular Mechanics (QM/MM) applied to tribology: Real-time monitoring of tribochemical reactions of water at graphene edges, COMPUTATIONAL MATERIALS SCIENCE, Vol: 173, ISSN: 0927-0256
- Author Web Link
- Cite
- Citations: 6
Restuccia P, Ferrario M, Righi MC, 2020, Monitoring water and oxygen splitting at graphene edges and folds: Insights into the lubricity of graphitic materials, CARBON, Vol: 156, Pages: 93-103, ISSN: 0008-6223
- Author Web Link
- Cite
- Citations: 27
Peeters S, Restuccia P, Loehle S, et al., 2019, Characterization of Molybdenum Dithiocarbamates by First-Principles Calculations, JOURNAL OF PHYSICAL CHEMISTRY A, Vol: 123, Pages: 7007-7015, ISSN: 1089-5639
- Author Web Link
- Cite
- Citations: 14
Schulzendorf M, Hinaut A, Kisiel M, et al., 2019, Altering the properties of graphene on Cu(111) by intercalation of potassium bromide, ACS Nano, Vol: 13, Pages: 5485-5492, ISSN: 1936-0851
The catalytic growth on transition metal surfaces provides a clean and controllable route to obtain defect-free, monocrystalline graphene. However, graphene's optical and electronic properties are diminished by the interaction with the metal substrate. One way to overcome this obstacle is the intercalation of atoms and molecules decoupling the graphene and restoring its electronic structure. We applied noncontact atomic force microscopy to study the structural and electric properties of graphene on clean Cu(111) and after the adsorption of KBr or NaCl. By means of Kelvin probe force microscopy, a change in graphene's work function has been observed after the deposition of KBr, indicating a changed graphene-substrate interaction. Further measurements of single-electron charging events as well as X-ray photoelectron spectroscopy confirmed an electronic decoupling of the graphene islands by KBr intercalation. The results have been compared with density functional theory calculations, supporting our experimental findings.
Restuccia P, Righi MC, 2019, Tribochemistry of graphene on iron and its possible role in lubrication of steel (vol 106, pg 118, 2016), CARBON, Vol: 141, Pages: 794-794, ISSN: 0008-6223
Fatti G, Restuccia P, Calandra C, et al., 2018, Phosphorus Adsorption on Fe(110): An ab Initio Comparative Study of Iron Passivation by Different Adsorbates, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 122, Pages: 28105-28112, ISSN: 1932-7447
Restuccia P, Levita G, Wolloch M, et al., 2018, Ideal adhesive and shear strengths of solid interfaces: A high throughput ab initio approach, COMPUTATIONAL MATERIALS SCIENCE, Vol: 154, Pages: 517-529, ISSN: 0927-0256
Wolloch M, Levita G, Restuccia P, et al., 2018, Interfacial Charge Density and Its Connection to Adhesion and Frictional Forces, PHYSICAL REVIEW LETTERS, Vol: 121, ISSN: 0031-9007
Righi MC, Restuccia P, Fatti G, 2018, High throughput and multi-scale quantum-mechanics / molecular-mechanics calculations applied to lubricants, 255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water, Publisher: AMER CHEMICAL SOC, ISSN: 0065-7727
Nicolini P, Capozza R, Restuccia P, et al., 2018, Structural Ordering of Molybdenum Disulfide Studied via Reactive Molecular Dynamics Simulations, ACS APPLIED MATERIALS & INTERFACES, Vol: 10, Pages: 8937-8946, ISSN: 1944-8244
Marchetto D, Restuccia P, Ballestrazzi A, et al., 2017, Surface passivation by graphene in the lubrication of iron: A comparison with bronze, CARBON, Vol: 116, Pages: 375-380, ISSN: 0008-6223
Restuccia P, Ferrario M, Silvestrelli PL, et al., 2016, Size-dependent commensurability and its possible role in determining the frictional behavior of adsorbed systems, PHYSICAL CHEMISTRY CHEMICAL PHYSICS, Vol: 18, Pages: 28997-29004, ISSN: 1463-9076
Levita G, Restuccia P, Righi MC, 2016, Graphene and MoS2 interacting with water: A comparison by ab initio calculations, CARBON, Vol: 107, Pages: 878-884, ISSN: 0008-6223
Restuccia P, Righi MC, 2016, Tribochemistry of graphene on iron and its possible role in lubrication of steel, CARBON, Vol: 106, Pages: 118-124, ISSN: 0008-6223
This data is extracted from the Web of Science and reproduced under a licence from Thomson Reuters. You may not copy or re-distribute this data in whole or in part without the written consent of the Science business of Thomson Reuters.