jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Cristiana Cesari | Marco Bortoluzzi | Tiziana Funaioli | Cristina Femoni | Maria Carmela Iapalucci | Stefano Zacchini
Source: Inorganic Chemistry (article, 2023-08-30)
Field: Chemistry — Organic Chemistry

Highly Reduced Ruthenium Carbide Carbonyl Clusters: Synthesis, Molecular Structure, Reactivity, Electrochemistry, and Computational Investigation of [Ru<sub>6</sub>C(CO)<sub>15</sub>]<sup>4–</sup> The reaction of [Ru<sub>6</sub>C(CO)<sub>16</sub>]<sup>2-</sup> (<b>1</b>) with NaOH in DMSO resulted in the formation of a highly reduced [Ru<sub>6</sub>C(CO)<sub>15</sub>]<sup>4-</sup> (<b>2</b>), which was readily protonated by acids, such as HBF<sub>4</sub>·Et<sub>2</sub>O, to [HRu<sub>6</sub>C(CO)<sub>15</sub>]<sup>3-</sup> (<b>3</b>). Oxidation of <b>2</b> with [Cp<sub>2</sub>Fe][PF<sub>6</sub>] or [C<sub>7</sub>H<sub>7</sub>][BF<sub>4</sub>] in CH<sub>3</sub>CN resulted in [Ru<sub>6</sub>C(CO)<sub>15</sub>(CH<sub>3</sub>CN)]<sup>2-</sup> (<b>5</b>), which was quantitatively converted into <b>1</b> after exposure to CO atmosphere. The reaction of <b>2</b> with a mild methylating agent such as CH<sub>3,</sub>I afforded the purported [Ru<sub>6</sub>C(CO)<sub>14</sub>(COCH<sub>3</sub>)]<sup>3-</sup> (<b>6</b>). By employing a stronger reagent, that is, CF<sub>3</sub>SO<sub>3</sub>CH<sub>3</sub>, a mixture of [HRu<sub>6</sub>C(CO)<sub>16</sub>]<sup>-</sup> (<b>4</b>), [H<sub>3</sub>Ru<sub>6</sub>C(CO)<sub>15</sub>]<sup>-</sup> (<b>7</b>), and [Ru<sub>6</sub>C(CO)<sub>15</sub>(CH<sub>3</sub>CNCH<sub>3</sub>)]<sup>-</sup> (<b>8</b>) was obtained. The molecular structures of <b>2-5</b>, <b>7</b>, and <b>8</b> were determined by single-crystal X-ray diffraction as their [NEt<sub>4</sub>]<sub>4</sub>[<b>2</b>]·CH<sub>3</sub>CN, [NEt<sub>4</sub>]<sub>3</sub>[<b>3</b>], [NEt<sub>4</sub>][<b>4</b>], [NEt<sub>4</sub>]<sub>2</sub>[<b>5</b>], [NEt<sub>4</sub>][<b>7</b>], and [NEt<sub>4</sub>][<b>8</b>]·solv salts. The carbyne-carbide cluster <b>6</b> was partially characterized by IR spectroscopy and ESI-MS, and its structure was computationally predicted using DFT methods. The redox behavior of <b>2</b> and <b>3</b> was investigated by electrochemical and IR spectroelectrochemical methods. Computational studies were performed in order to unravel structural and thermodynamic aspects of these octahedral Ru-carbide carbonyl clusters displaying miscellaneous ligands and charges in comparison with related iron derivatives. Chemistry ; Ruthenium ; Reactivity (psychology) ; Electrochemistry ; Reagent ; Carbide ; Cluster (spacecraft) ; Rhenium ; Cyclic voltammetry ; Protonation ; Redox ; Crystallography ; Medicinal chemistry ; Inorganic chemistry ; Physical chemistry ; Catalysis ; Organic chemistry ; Electrode Organometallic Complex Synthesis and Catalysis ; Asymmetric Hydrogenation and Catalysis ; Metal complexes synthesis and properties
Authors: Yasmine Bouchentouf Idriss | B. Bouadjemi | M. Matougui | M. Houari | T. Lantri | S. Haid | S. Bentata
Source: Revista Mexicana de Física (article, 2023-09-01)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Hubbard's parameter influence on Ba2GdReO6 properties, a promising ferromagnetic double Pérovskite oxide for thermoelectric applications In this paper, an exhaustive investigation was carried out on the compound double Perovskite Ba2GdReO6 including its structural, electronic, magnetic and thermoelectric properties. This study is based on the density functional theory (DFT) and more explicitly on the full potential linearized augmented plane wave (FP-LAPW), in the context of different approximations as exchange and correlation potential such as: The generalized gradient approximation (GGA) and its corollary the Becke – Johnson approach modified by Trans-Blaha (TB - mBJ) for a better approximation of the gap, and the GGA + U approach (where U is the Hubbard correction term). After an analysis of the results obtained, it turns out that the double perovskite material Ba2GdReO6 is a ferromagnetic material and has a half-metallic character, moreover, this compound has an integral magnetic moment of 9µB, which is in accordance with the rule of Slater-Pauling. From the study of the thermoelectric properties consisting in plotting curves of different parameters such as: the Seebeck coefficient (S), electrical conductivity per relaxation time (σ/τ), the electronic thermal conductivity per relaxation time ( /τ) and the merit factor (ZT) as a function of temperature, based on the GGA+U approximation, which is most suitable for the study of this compound, it emerges that the double pérovskite Ba2GdReO6 presents thermoelectric performances in medium to high temperature ranges, in view of the high values ​​of the Seebeck coefficient and those of the electrical conductivity as well as a value close to unity for the merit factor, therefore, this compound can be used for thermoelectric applications in this range of temperatures (medium to high). Condensed matter physics ; Thermoelectric effect ; Seebeck coefficient ; Materials science ; Ferromagnetism ; Electrical resistivity and conductivity ; Figure of merit ; Thermal conductivity ; Magnetic moment ; Physics ; Thermodynamics ; Quantum mechanics Heusler alloys: electronic and magnetic properties ; Advanced Thermoelectric Materials and Devices ; Magnetic and transport properties of perovskites and related materials
Authors: Alexey Fedorov | Andrey V. Bukhtiyarov | Maxim A. Panafidin | Igor P. Prosvirin | Yan V. Zubavichus | V. I. Bukhtiyarov
Source: Nanomaterials (article, 2023-12-25)
Field: Materials Science — Materials Chemistry

Thermally Induced Surface Structure and Morphology Evolution in Bimetallic Pt-Au/HOPG Nanoparticles as Probed Using XPS and STM Bimetallic nanoparticles expand the possibilities of catalyst design, providing an extra degree of freedom for tailoring the catalyst structure in comparison to purely monometallic systems. The distribution mode of two metal species defines the structure of surface catalytic sites, and current research efforts are focused on the development of methods for their controlled tuning. In light of this, a comprehensive investigation of the factors which influence the changes in the morphology of bimetallic nanoparticles, including the elemental redistribution, are mandatory for each particular bimetallic system. Here we present the combined XPS/STM study of the surface structure and morphology of bimetallic Pt-Au/HOPG nanoparticles prepared by thermal vacuum deposition and show that thermal annealing up to 350 °C induces the alloying process between the two bulk-immiscible metal components. Increasing the treatment temperature enhances the extent of Pt-Au alloying. However, the sintering of nanoparticles starts to occur above 500 °C. The approach implemented in this work includes the theoretical simulation of XPS signal intensities for a more meticulous analysis of the compositional distribution and can be helpful from a methodological perspective for other XPS/STM studies of bimetallic nanoparticles on planar supports. Bimetallic strip ; X-ray photoelectron spectroscopy ; Materials science ; Nanoparticle ; Catalysis ; Nanotechnology ; Chemical engineering ; Annealing (glass) ; Metal ; Metallurgy ; Chemistry ; Organic chemistry Catalytic Processes in Materials Science ; Electrocatalysts for Energy Conversion ; Copper-based nanomaterials and applications
Authors: Tianyu Yan | Huaizhong Zhang | Kristen A. Fichthorn
Source: ACS Nano (article, 2023-10-02)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Minimum Free-Energy Shapes of Ag Nanocrystals: Vacuum vs Solution We use two variants of replica-exchange molecular dynamics (MD) simulations, parallel tempering MD and partial replica exchange MD, to probe the minimum free-energy shapes of Ag nanocrystals containing 100-200 atoms in a vacuum, ethylene glycol (EG) solvent, and EG solvent with a PVP polymer containing 100 repeat units. Our simulations reveal a shape intermediate between a Dh and an Ih, a Dh-Ih, that has distinct structural signatures and magic sizes. We find several prominent features associated with entropy: pure FCC nanocrystals are less common than FCC crystals containing stacking faults, and crystals with the minimum potential energy are not always preferred over the range of relevant temperatures. The shapes of the nanocrystals in solution are influenced by the chemical identities of the solution-phase molecules. Comparing Ag nanocrystal shapes in EG to those in an EG+PVP solution, we find more icosahedra in EG and more decahedra in EG+PVP across all of the nanocrystal sizes probed in this study. At certain critical sizes, nanocrystal shapes can change dramatically with the addition and removal of a single atom or with a change in temperature at a fixed size. The information in our study could be useful in efforts to devise processing routes to achieve selective nanocrystal shapes. Nanocrystal ; Materials science ; Chemical physics ; Molecular dynamics ; Ethylene glycol ; Replica ; Polymer ; Solvent ; Nanotechnology ; Crystallography ; Chemical engineering ; Chemistry ; Computational chemistry Gold and Silver Nanoparticles Synthesis and Applications ; Nanocluster Synthesis and Applications ; nanoparticles nucleation surface interactions
Authors: Quentin Duez | Paul Tinnemans | Johannes A. A. W. Elemans | Jana Roithová
Source: Chemical Science (article, 2023-01-01)
Field: Chemistry — Spectroscopy

Kinetics of ligand exchange in solution: a quantitative mass spectrometry approach Complex speciation and exchange kinetics of labile ligands are critical parameters for understanding the reactivity of metal complexes in solution. We present a novel approach to determine ligand exchange parameters based on electrospray ionization mass spectrometry (ESI-MS). The introduction of isotopically labelled ligands to a solution of metal host and unlabelled ligands allows the quantitative investigation of the solution-phase equilibria. Furthermore, ion mobility separation can target individual isomers, such as ligands bound at specific sites. As a proof of concept, we investigate the solution equilibria of labile pyridine ligands coordinated in the cavity of macrocyclic porphyrin cage complexes bearing diamagnetic or paramagnetic metal centres. The effects of solvent, porphyrin coordination sphere, transition metal, and counterion on ligand dissociation are discussed. Rate constants and activation parameters for ligand dissociation in the solution can be derived from our ESI-MS approach, thereby providing mechanistic insights that are not easily obtained from traditional solution-phase techniques. Kinetics ; Mass spectrometry ; Chemistry ; Ligand (biochemistry) ; Analytical Chemistry (journal) ; Chromatography ; Physics ; Biochemistry ; Receptor Molecular Sensors and Ion Detection ; Mass Spectrometry Techniques and Applications ; Radioactive element chemistry and processing
Authors: Kan Hatakeyama‐Sato | Yasuei Uchima | Takahiro Kashikawa | Kôichi Kimura | Kenichi Oyaizu
Source: RSC Advances (article, 2023-01-01)
Field: Materials Science — Materials Chemistry

Extracting higher-conductivity designs for solid polymer electrolytes by quantum-inspired annealing Data-driven optimal structure exploration has become a hot topic in materials for energy-related devices. However, this method is still challenging due to the insufficient prediction accuracy of material properties and large exploration space for candidate structures. We propose a data trend analysis system for materials using quantum-inspired annealing. Structure-property relationships are learned by a hybrid decision tree and quadratic regression algorithm. Then, ideal solutions to maximize the property are explored by a Fujitsu Digital Annealer, which is unique hardware that can quickly extract promising solutions from the ample search space. The system's validity is investigated with an experimental study examining solid polymer electrolytes as potential components for solid-state lithium-ion batteries. A new trithiocarbonate polymer electrolyte offers a conductivity of 10<sup>-6</sup> S cm<sup>-1</sup> at room temperature, even though it is in a glassy state. Molecular design through data science will enable accelerated exploration of functional materials for energy-related devices. Conductivity ; Annealing (glass) ; Electrolyte ; Polymer electrolytes ; Polymer ; Quantum annealing ; Quantum ; Chemical engineering ; Materials science ; Nanotechnology ; Chemistry ; Ionic conductivity ; Physics ; Physical chemistry ; Composite material ; Quantum computer ; Quantum mechanics ; Electrode ; Engineering Machine Learning in Materials Science ; Fuel Cells and Related Materials ; Advanced Memory and Neural Computing
Authors: Ashkan Basande | Hadi Beitollahi
Source: Journal of Electrochemical Science and Engineering (article, 2023-10-25)
Field: Chemistry — Electrochemistry

Electrocatalytic response of nitrogen-doped hollow carbon spheres modified glassy carbon electrode for sulphite detection in water In this work, the glassy carbon electrode (GCE) surface was modified with nitrogen-doped hollow carbon spheres (N-HCSs) to achieve a new electrochemical sulphite sensor (N-HCSs/GCE) in water samples. The N-HCSs were explored for electrocatalytic behavior through voltammetric approaches using a routine three-electrode system. The findings revealed an admirable efficiency for modified electrodes towards sulphite oxidation, highlighting the effectiveness of our as-produced sulphite sensor. The differential pulse voltammetry was utilized under obtained optimal circumstances to study the as-developed sensor, the results of which underlined linear electrochemical current in relation to sulphite concentration, with dynamic range as wide as 1.0-100.0 μM and limit of detection as narrow as 0.35 μM. Moreover, N-HCSs/GCE had commendable practical applicability for sensing sulphite present in real specimens with voltammetric techniques. Differential pulse voltammetry ; Electrode ; Detection limit ; Electrochemistry ; Carbon fibers ; Materials science ; Voltammetry ; Electrochemical gas sensor ; Linear range ; Inorganic chemistry ; Cyclic voltammetry ; Analytical Chemistry (journal) ; Chemistry ; Chromatography ; Composite material Electrochemical Analysis and Applications ; Electrochemical sensors and biosensors ; Sulfur Compounds in Biology
Authors: Neza Rahayu Palapa | Alfan Wijaya
Source: Indonesian Journal of Material Research (article, 2023-11-29)
Field: Materials Science — Materials Chemistry

Layered Double Hydroxide Coated by Carbon-Based Material for Environmental Dye Pollutant We conducted this research to modify NiAl layered double hydroxide with several carbon-based materials, including cellulose, biochar and graphite. This material was successfully prepared by coprecipitation methods and was proven by XRD, SEM and FTIR characterization. Furthermore, we conducted the adsorption process and reusability to investigate their ability as water treatments. The dose effect on M.G. removal was investigated by the highest M.G. removal capacity using the CBC-NiAl LDHs composite, which was 100 mg. M.G. removal capacity was increased with an increase in contact time, and the saturation point was reached after 60 min for CC-NiAl and CGF-NiAl LDHs, which CBC-NiAl LDH increased and saturated after 100 min with high adsorption capacity. CC-NiAl, CBC-NiAl and CGF-NiAl LDHs composite have proved efficient, sustainable materials that maintain adsorption capability in each reusable cycle. Nial ; Coprecipitation ; Adsorption ; Materials science ; Layered double hydroxides ; Hydroxide ; Composite number ; Chemical engineering ; Nuclear chemistry ; Metallurgy ; Composite material ; Chemistry ; Organic chemistry ; Intermetallic Layered Double Hydroxides Synthesis and Applications
Authors: João Victor da Silva Guerra | Luiz F. G. Alves | Didier Bourissou | Paulo Sérgio Lopes de Oliveira | György Szalóki
Source: Journal of Chemical Information and Modeling (article, 2023-05-02)
Field: Chemistry — Organic Chemistry

Cavity Characterization in Supramolecular Cages Confining molecular guests within artificial hosts has provided a major driving force in the rational design of supramolecular cages with tailored properties. Over the last 30 years, a set of design strategies have been developed that enabled the controlled synthesis of a myriad of cages. Recently, there has been a growing interest in involving in silico methods in this toolbox. Cavity shape and size are important parameters that can be easily accessed by inexpensive geometric algorithms. Although these algorithms are well developed for the detection of nonartificial cavities (e.g., enzymes), they are not routinely used for the rational design of supramolecular cages. In order to test the capabilities of this tool, we have evaluated the performance and characteristics of seven different cavity characterization software in the context of 22 analogues of well-known supramolecular cages. Among the tested software, KVFinder project and Fpocket proved to be the most software to characterize supramolecular cavities. With the results of this work, we aim to popularize this underused technique within the supramolecular community. Supramolecular chemistry ; Toolbox ; Context (archaeology) ; Characterization (materials science) ; Software ; Computer science ; Rational design ; In silico ; Nanotechnology ; Materials science ; Chemistry ; Crystallography ; Biology Supramolecular Chemistry and Complexes ; Supramolecular Self-Assembly in Materials ; Molecular Sensors and Ion Detection
Authors: Guoshuai Liu | Kang Shi | Hui Sun | Biao Yang | Yunxuan Weng
Source: Polymers (article, 2023-06-25)
Field: Materials Science — Biomaterials

Enhancing Hydrophobicity and Oxygen Barrier of Xylan/PVOH Composite Film by 1,2,3,4-Butane Tetracarboxylic Acid Crosslinking Hemicellulose has potential advantages in food packaging because of its abundant reserves, degradability and regeneration. However, compared with fossil-derived plastic films, hemicellulose-based films show inferior hydrophobicity and barrier properties because of their low degree of polymerization and strong hydrophilicity. Focusing on such issues, this work covers the modification of a xylan/polyvinyl alcohol (PVOH) film using 1,2,3,4-butane tetracarboxylic acid (BTCA) as esterifying agent. The thus prepared composite film was more compact owing to the esterification reaction with xylan and PVOH forming a crosslinked network structure and reducing the distance between molecular chains. The results showed that BTCA had a positive effect on the oxygen barrier, hydrophobicity and mechanical properties of the composite film. The tensile strength of the xylan/PVOH composite film with 10% BTCA content increased from 11.19 MPa to 13.99 MPa. A 20% BTCA loading resulted in an increase in the contact angle of the composite film from 87.1° to 108.2°, and a decrease in the oxygen permeability from 2.11 to 0.43 (cm3·µm)/(m2·d·kPa), corresponding to increase in the contact angle by 24% and a decrease in oxygen permeability by 80%. The overall performance enhancement indicates the potential application of such composites as food packaging. Oxygen permeability ; Contact angle ; Composite number ; Ultimate tensile strength ; Polyvinyl alcohol ; Materials science ; Hemicellulose ; Chemical engineering ; Xylan ; Composite material ; Composite film ; Oxygen ; Polymer chemistry ; Chemistry ; Organic chemistry ; Cellulose Advanced Cellulose Research Studies ; Nanocomposite Films for Food Packaging ; biodegradable polymer synthesis and properties
Authors: Xuan Ding | Jiayi Liu | Hui Shi | Yi Zhou | Lei Zhou | Wei Ren | Penghui Shao | Liming Yang | Derun Zhao | Yun Wei | Xubiao Luo
Source: iScience (article, 2023-10-19)
Field: Chemistry — Inorganic Chemistry

Regulating steric hindrance in difunctionalized porous aromatic frameworks for the selective separation of Pb(II) Efficient and selective removal of Pb(II) from wastewater with complex matrix remains a challenging task. Porous aromatic frameworks (PAFs) with predesigned functional building blocks provide a favorable platform for the selective separation of Pb(II). Herein, the bifunctional SPAFs with the introduction of -OH and -SO<sub>3</sub>H were synthesized through rationally optimizing their steric hindrance. As a result, the SPAF-0.75 exhibits favorable adsorption capacity of Pb(II) (212.34 mg g<sup>-1</sup>), which is 22 times larger than pristine framework. Competition experiment indicates that SPAF-0.75 possess the selective removal of Pb(II) without interfering from co-existing metal ions. The removal rate of SPAF-0.75 still retain at 100% after six successive cycles. The DFT calculation illustrates that -OH and -SO<sub>3</sub>H are co-participate in the process of capturing Pb(II), revealing SPAF-0.75 preferred removal of Pb(II) owing to the lowest adsorption energy (Δ<i>E</i><sub><i>ab</i></sub> = -3.99 eV). This study extend the understanding of the structure-property relationship and facilitate new possibilities for PAFs. Steric effects ; Chemistry ; Bifunctional ; Adsorption ; Metal-organic framework ; Computational chemistry ; Stereochemistry ; Organic chemistry ; Catalysis Metal-Organic Frameworks: Synthesis and Applications ; Extraction and Separation Processes ; Gas Sensing Nanomaterials and Sensors
Authors: Hyun-Myung Woo | Xiaoning Qian | Li Lynn Tan | Shantenu Jha | Francis J. Alexander | Edward R. Dougherty | Byung-Jun Yoon
Source: Patterns (article, 2023-11-01)
Field: Materials Science — Materials Chemistry

Optimal decision-making in high-throughput virtual screening pipelines The need for efficient computational screening of molecular candidates that possess desired properties frequently arises in various scientific and engineering problems, including drug discovery and materials design. However, the enormous search space containing the candidates and the substantial computational cost of high-fidelity property prediction models make screening practically challenging. In this work, we propose a general framework for constructing and optimizing a high-throughput virtual screening (HTVS) pipeline that consists of multi-fidelity models. The central idea is to optimally allocate the computational resources to models with varying costs and accuracy to optimize the return on computational investment. Based on both simulated and real-world data, we demonstrate that the proposed optimal HTVS framework can significantly accelerate virtual screening without any degradation in terms of accuracy. Furthermore, it enables an adaptive operational strategy for HTVS, where one can trade accuracy for efficiency. Computer science ; Virtual screening ; Pipeline (software) ; Fidelity ; Throughput ; Pipeline transport ; High fidelity ; Distributed computing ; Drug discovery ; Wireless ; Engineering Machine Learning in Materials Science ; Innovative Microfluidic and Catalytic Techniques Innovation ; Computational Drug Discovery Methods