jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Ekaterina B. Zhulina | Oleg V. Borisov
Source: Soft Matter (article, 2022-01-01)
Field: Chemistry — Organic Chemistry

Bottlebrush polymer gels: architectural control over swelling and osmotic bulk modulus Swelling behaviour and bulk moduli of polymer gels comprising of crosslinked bottlebrush subchains enable fine tuning by varying polymerization degrees of the main and side chains of the bottlebrush strands as well as their grafting densities. By using scaling approach we predict power law dependences of structural and elastic properties of swollen bottlebrush gels on the set of relevant architectural parameters and construct phase diagrams consisting of regions corresponding to different power law asymptotics for these dependences. In particular, our theory predict that bulk elastic modulus of the gel exhibits non-monotonous dependence on the degree of polymerization of side chains of the bottlebrush strands. Swelling ; Materials science ; Polymer ; Polymerization ; Phase (matter) ; Elastic modulus ; Scaling ; Power law ; Monomer ; Side chain ; Modulus ; Scaling law ; Composite material ; Polymer chemistry ; Chemistry ; Mathematics ; Geometry Advanced Polymer Synthesis and Characterization ; Polymer Surface Interaction Studies ; Hydrogels: synthesis, properties, applications
Authors: Juan M. Marmolejo‐Tejada | Martín A. Mosquera
Source: Chemical Communications (article, 2022-01-01)
Field: Materials Science — Materials Chemistry

Thermal properties of single-layer MoS<sub>2</sub>–WS<sub>2</sub> alloys enabled by machine-learned interatomic potentials Two-dimensional (2D) quantum materials are poised to transform conventional electronics for a wide spectrum of applications that will encompass chemical sciences. For the study of thermal transport in single-layer (1L) or multi-layer transition metal dichalcogenides (TMDs), this work explores the combination of density functional theory (DFT) and algorithmic training for the generation of a moment tensor potential (MTP) that models 1L-MoS<sub>2</sub>, 1L-WS<sub>2</sub> and their alloys, and demonstrates a synergy of theoretical techniques that is anticipated to play an important role in the field. From a high-performance computing perspective, these yield very convenient inter-atomic (or inter-molecular in other contexts) potentials that are useful to predict the response of quantum materials to thermal perturbations, or other driving forces. We show that our trained MTP functions successfully describe vibrational properties of the systems, and their thermal conductivities. The trained potential displays consistent agreement with DFT calculations, as well as the Stillinger-Weber (SW) potential. We also find that the thermal conductivity of the 2D alloys is little affected by sulfur vacancies. This is a behavior that may aid the fine-tuning of material's thermal properties for heat management and energy storage and conversion applications. Thermal conductivity ; Density functional theory ; Thermal ; Interatomic potential ; Materials science ; Work (physics) ; Field (mathematics) ; Thermal conduction ; Layer (electronics) ; Quantum ; Molecular dynamics ; Nanotechnology ; Computational chemistry ; Chemistry ; Thermodynamics ; Physics ; Quantum mechanics Thermal properties of materials ; Machine Learning in Materials Science ; 2D Materials and Applications
Authors: Ina Erceg | Jasminka Kontrec | Vida Strasser | Atiđa Selmani | Darija Domazet Jurašin | Marija Ćurlin | Branka Njegić Džakula | Nives Matijaković Mlinarić | Suzana Šegota | Daniel Mark Lyons | Damir Kralj | Maja Dutour Sikirić
Source: Minerals (article, 2022-02-06)
Field: Materials Science — Biomaterials

Precipitation of Calcium Phosphates and Calcium Carbonates in the Presence of Differently Charged Liposomes Liposomes (lipid vesicles) are often considered to be a versatile tool for the synthesis of advanced materials, as they allow various control mechanisms to tune the materials’ properties. Among diverse materials, the synthesis of calcium phosphates (CaPs) and calcium carbonates (CaCO3) using liposomes has attracted particular attention in the development of novel (bio)materials and biomineralization research. However, the preparation of materials using liposomes has not yet been fully exploited. Most of the liposomes used have been anionic and/or zwitterionic, while data on the influence of cationic liposomes are limited. Therefore, the aim of this study was to investigate and compare the influence of differently charged liposomes on CaPs and CaCO3 formation. Zwitterionic 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC), negatively charged 1,2-dimyristoyl-sn-glycero-3-phospho-L-serine (DMPS), and positively charged 1,2-dioleoyl-sn-glycero-3-ethylphosphocholine (EPC) lipids were used to prepare the respective liposomes. The presence of liposomes during the spontaneous precipitation of CaPs and CaCO3 affected both the precipitation and transformation kinetics, as well as the morphology of the precipitates formed. The most prominent effect was noted for both materials in the presence of DMPS liposomes, as (nano) shell structures were formed in both cases. The obtained results indicate possible strategies to fine-tune the precipitation process of CaPs and CaCO3, which may be of interest for the production of novel materials. Liposome ; Biomineralization ; Precipitation ; Vesicle ; Calcium ; Chemistry ; Cationic liposome ; Chemical engineering ; Calcium carbonate ; Materials science ; Biophysics ; Membrane ; Organic chemistry ; Biochemistry Calcium Carbonate Crystallization and Inhibition ; Bone Tissue Engineering Materials ; Polymer Surface Interaction Studies
Authors: Bong‐Rim Shin | In Cheol Yu | Uroš Puc | Won Tae Kim | Woojin Yoon | Chaeyoon Kim | Hoseop Yun | Dongwook Kim | Mojca Jazbinšek | Fabıan Rotermund | O‐Pil Kwon
Source: Advanced Optical Materials (article, 2022-10-26)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Design and Validation of Isomorphic Crystal Library for Nonlinear Optics and THz Wave Generation Abstract Development of new organic crystals possessing large second‐order optical nonlinearity is very challenging because of strong tendency of centrosymmetric dipole–dipole molecular assembly in crystals. This tendency makes it difficult to develop various analogous crystals that allow fine tuning of optical and physical properties to enhance the device performance. A design approach of an isomorphic crystal library consisting of 11 highly efficient nonlinear optical salt crystals is reported. Analyzing the so‐called isomorphic tolerance space in previously reported mother crystals (PMnXQ chromophores, where PM denotes piperidin‐4‐ylmethanol electron donor, n corresponds to the substituted position of halogen (X) group on the quinolinium (Q) electron acceptor), various substituents are introduced into the PMnXQ crystals at different positions, considering their space‐filling characteristics and interionic interaction ability. All 11 PMnXQ crystals exhibit an isomorphic (or pseudo‐isomorphic) crystal structure, in which the cationic chromophores form a perfectly parallel assembly for maximizing the second‐order nonlinear optical susceptibility. The optical, physical, and crystal characteristics of newly designed, synthesized, and grown isomorphic PMnXQ crystals show both similarities and differences. Excellent THz wave‐generation performance is demonstrated in both kHz‐ and MHz‐repetition optical pump systems with new PMnXQ crystals. Therefore, the design approach using isomorphic tolerance space is very attractive for developing diverse isomorphic analogous organic crystals. Chromophore ; Materials science ; Crystal (programming language) ; Dipole ; Nonlinear optics ; Space group ; Second-harmonic generation ; Nonlinear optical ; Crystallography ; Acceptor ; Diffraction ; Nonlinear system ; Optoelectronics ; Optics ; Condensed matter physics ; X-ray crystallography ; Laser ; Physics ; Chemistry ; Photochemistry ; Computer science ; Quantum mechanics Nonlinear Optical Materials Research ; Solid-state spectroscopy and crystallography ; Crystallography and molecular interactions
Authors: Manuela Stefanelli | Gabriele Magna | Corrado Di Natale | Roberto Paolesse | Donato Monti
Source: International Journal of Molecular Sciences (review, 2022-12-09)
Field: Materials Science — Materials Chemistry

Stereospecific Self-Assembly Processes of Porphyrin-Proline Conjugates: From the Effect of Structural Features and Bulk Solvent Properties to the Application in Stereoselective Sensor Systems Conjugating the porphyrin ring with an amino acid via amide linkage represents a straightforward way for conferring both amphiphilicity and chirality to the macrocycle. Proline residue is a good choice in this context since its conformational rigidity allows for porphyrin assembling where molecular chirality is efficiently transferred and amplified using properly honed aqueous environments. Herein, we describe the evolution of the studies carried out by our group to achieve chiral systems from some porphyrin-proline derivatives, both in solution and in the solid state. The discussion focuses on some fundamental aspects reflecting on the final molecular architectures obtained, which are related to the nature of the appended group (stereochemistry and charge), the presence of a metal ion coordinated to the porphyrin core and the bulk solvent properties. Indeed, fine-tuning the mentioned parameters enables the achievement of stereospecific structures with distinctive chiroptical and morphological features. Solid films based on these chiral systems were also obtained and their recognition abilities in gaseous and liquid phase are here described. Porphyrin ; Chirality (physics) ; Chemistry ; Stereospecificity ; Self-assembly ; Solvent ; Proline ; Amide ; Combinatorial chemistry ; Amino acid ; Stereochemistry ; Organic chemistry ; Catalysis Porphyrin and Phthalocyanine Chemistry ; Molecular Sensors and Ion Detection ; Supramolecular Chemistry and Complexes
Authors: Balaji Gowrivel Vijayakumar | Deepthi Ramesh | Manikandan Krishnan | Mary Theresa | Aiswarya Sethumadhavan | V. Brindha Priyadarisini | E. K. Radhakrishnan | Maheswaran Mani | Tharanikkarasu Kannan
Source: Journal of Materials Chemistry B (article, 2022-01-01)
Field: Materials Science — Biomaterials

Chitosan with pendant (<i>E</i>)-5-((4-acetylphenyl)diazenyl)-6-aminouracil groups as synergetic antimicrobial agents Conventional antimicrobial agents are losing the war against drug resistance day-by-day. Chitosan biopolymer is one of the alternative materials that lends itself well to this application by fine-tuning its bioactivity using different pendant groups. Herein, we report the synthesis of novel chitosan with pendant (<i>E</i>)-5-((4-acetylphenyl)diazenyl)-6-aminouracil (APAU) groups by forming Schiff base linkages between chitosan and the pendant groups. These chitosan biopolymers with pendant APAU groups form films superior in thermal stability compared to the neat chitosan. Interestingly, APAU alone was inactive against <i>K. pneumoniae</i>, <i>E. coli</i>, <i>S. aureus</i>, <i>T. rubrum</i> and <i>C. albicans</i>. However, novel chitosan samples were active against <i>S. aureus</i> with an MIC of 390 μg mL<sup>-1</sup>, half that of plain chitosan at 780 μg mL<sup>-1</sup>. APAU modified chitosan samples, CA80 and CA100 showed an MIC (against <i>K. pneumoniae</i> and <i>E. coli</i>) of 23.4 μg mL<sup>-1</sup>, superior to plain chitosan's MIC of 187.5 μg mL<sup>-1</sup> and is close to commercial Fluconazole's MIC of 11.7 μg mL<sup>-1</sup>. The activity of chitosan changes with APAU content and at higher concentrations shows a strong synergetic antimicrobial effect. Chitosan ; Antimicrobial ; Biopolymer ; Candida albicans ; Chemistry ; Nuclear chemistry ; Microbiology ; Organic chemistry ; Biology ; Polymer Nanocomposite Films for Food Packaging ; Antimicrobial agents and applications ; Advanced Drug Delivery Systems
Authors: Yanhui Feng | Xingjun Li | Shan Lu | Renfu Li | Zhongliang Gong | Xiaoying Shang | Yifan Pei | Wei Zheng | Datao Tu | Xueyuan Chen
Source: Nano Research (article, 2022-08-06)
Field: Chemistry — Inorganic Chemistry

Modulator-directed assembly of hybrid composites based on metal-organic frameworks and upconversion nanoparticles Hybrid composites made of metal-organic frameworks (MOFs) and lanthanide-doped upconversion nanoparticles (UCNPs) have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing, photocatalysis, anticounterfeiting and nanomedicine. However, precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth mechanisms. Herein, we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites (ZIF-8 = zeolitic imidazolate framework-8). The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission, which were verified by steady-state/transient photoluminescence (PL) spectroscopy and single-particle imaging. Ethylenediamine (EDA) was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the composites. By adjusting the concentration of EDA from 0 to 25 mmol/L, the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron (RD) to truncated rhombic dodecahedron (TRD), cube with truncated edges (CTE), cube, and finally a unique form of interpenetration twins (IT). The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy (SEM) images and the formation mechanism was thoroughly revealed. Furthermore, we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and shapes. The proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications. Materials science ; Dodecahedron ; Zeolitic imidazolate framework ; Imidazolate ; Nanoparticle ; Nanotechnology ; Metal-organic framework ; Nucleation ; Photoluminescence ; Photocatalysis ; Composite material ; Lanthanide ; Photon upconversion ; Prussian blue ; Chemical engineering ; Doping ; Optoelectronics ; Chemistry ; Crystallography ; Catalysis ; Adsorption Metal-Organic Frameworks: Synthesis and Applications ; Luminescence Properties of Advanced Materials ; Luminescence and Fluorescent Materials
Authors: M.H. Yoo | Eunji Kang | Hyunwoo Ha | Jieun Yun | Hyuk Choi | Ju Hyeok Lee | Tae Jun Kim | Ji-Ho Min | Jin-Seok Choi | Kug‐Seung Lee | Namgee Jung | Sungtak Kim | Chunjoong Kim | Young‐Sang Yu | Hyun You Kim
Source: The Journal of Physical Chemistry Letters (article, 2022-02-14)
Field: Materials Science — Materials Chemistry

Interspersing CeO<sub><i>x</i></sub> Clusters to the Pt–TiO<sub>2</sub> Interfaces for Catalytic Promotion of TiO<sub>2</sub>-Supported Pt Nanoparticles We propose an interface-engineered oxide-supported Pt nanoparticle-based catalyst with improved low-temperature activity toward CO oxidation. By wet-impregnating 1 wt % Ce on TiO<sub>2</sub>, we synthesized hybrid oxide support of CeO<sub><i>x</i></sub>-TiO<sub>2</sub>, in which dense CeO<sub><i>x</i></sub> clusters formed on the surface of TiO<sub>2</sub>. Then, the Pt/CeO<sub><i>x</i></sub>-TiO<sub>2</sub> catalyst was synthesized by impregnating 2 wt % Pt on the CeO<sub><i>x</i></sub>-TiO<sub>2</sub> supporting oxide. Pt-CeO<sub><i>x</i></sub>-TiO<sub>2</sub> triphase interfaces were eventually formed upon impregnation of Pt on CeO<sub><i>x</i></sub>-TiO<sub>2</sub>. The Pt-CeO<sub><i>x</i></sub>-TiO<sub>2</sub> interfaces open up the interface-mediated Mars-van Krevelen CO oxidation pathway, thus providing additional interfacial reaction sites for CO oxidation. Consequently, the specific reaction rate of Pt/CeO<sub><i>x</i></sub>-TiO<sub>2</sub> for CO oxidation was increased by 3.2 times compared with that of Pt/TiO<sub>2</sub> at 140 °C. Our results demonstrate a widely applicable and straightforward method of catalytic activation of the interfaces between metal nanoparticles and supporting oxides, which enabled fine-tuning of the catalytic performance of oxide-supported metal nanoparticle classes of heterogeneous catalysts. Catalysis ; Materials science ; Oxide ; Nanoparticle ; Chemical engineering ; Metal ; Nanotechnology ; Chemistry ; Metallurgy ; Organic chemistry Catalytic Processes in Materials Science ; Nanomaterials for catalytic reactions ; Catalysis and Oxidation Reactions
Authors: Erika Michela Dematteis | Jussara Barale | Giovanni Capurso | Stefano Deledda | Magnus H. Sørby | Fermín Cuevas | M. Latroche | Marcello Baricco
Source: Journal of Alloys and Compounds (article, 2022-11-20)
Field: Materials Science — Materials Chemistry

In-situ neutron diffraction during reversible deuterium loading in Ti-rich and Mn-substituted Ti(Fe,Mn)0.90 alloys Neutron diffraction ; Deuterium ; Materials science ; Hydrogen storage ; Hydrogen ; Alloy ; Neutron ; Crystal structure ; Metallurgy ; Crystallography ; Chemistry ; Atomic physics ; Nuclear physics Hydrogen Storage and Materials ; Nuclear Materials and Properties ; Hybrid Renewable Energy Systems
Authors: Sergey N. Trukhan | S. S. Yakushkin | Oleg N. Martyanov
Source: The Journal of Physical Chemistry C (article, 2022-06-24)
Field: Chemistry — Analytical Chemistry

Fine-Tuning Simulation of the ESR Spectrum─Sensitive Tool to Identify the Local Environment of Asphaltenes In Situ An original method to study the local environment of vanadyl-containing components of heavy oils based on fine-tuning simulation of their electron spin resonance (ESR) spectra in situ is developed. The approach is backgrounded on precise computation of anisotropic ESR spectra of individual porphyrin complexes in specific solvents modeling a particular local environment of certain polarity using specific g and A tensor components, their dispersion, and linewidth determined by unresolved super-hyperfine interaction with the closest nitrogen. The high level of simulation accuracy allowed us to differentiate the values of the g and A tensor components related to individual vanadyl complexes in different solvents with certain polarity in reference systems and attribute the observed variation to the interaction of the vanadyl complex with surrounding molecules located in its axial direction. The method developed for the model systems is successfully applied to the real oil-based systems where different vanadyl complexes with different local environments are presented, forming the experimentally observed ESR spectrum. The Monte Carlo procedure was suggested to define the relative contribution (weight) of the individual spectra having tiny peculiarities related to vanadyl fragments in different local environments and finally mapping the g and A tensor components distribution which is characteristic for the particular oil-based sample. Extraordinary sensitivity to the localization and interaction with surrounding molecules of vanadyl-containing complexes which are present in heavy oil as a natural spin probe or can be specially introduced give us a unique opportunity to in situ study the local environment of asphaltenes and their intermolecular interactions with other oil components. Electron paramagnetic resonance ; Spectral line ; Monte Carlo method ; Intermolecular force ; Hyperfine structure ; Anisotropy ; Asphaltene ; Chemistry ; Polarity (international relations) ; In situ ; Tensor (intrinsic definition) ; Laser linewidth ; Chemical physics ; Asymmetry ; Spin (aerodynamics) ; Molecule ; Biological system ; Molecular physics ; Nuclear magnetic resonance ; Physics ; Atomic physics ; Organic chemistry ; Optics Petroleum Processing and Analysis ; Hydrocarbon exploration and reservoir analysis ; NMR spectroscopy and applications
Authors: Suchart Limkatanyu | Worathep Sae‐Long | Hamid M. Sedighi | Jaroon Rungamornrat | Piti Sukontasukkul | Woraphot Prachasaree | Thanongsak Imjai
Source: Nanomaterials (article, 2022-01-24)
Field: Materials Science — Materials Chemistry

Strain-Gradient Bar-Elastic Substrate Model with Surface-Energy Effect: Virtual-Force Approach This paper presents an alternative approach to formulating a rational bar-elastic substrate model with inclusion of small-scale and surface-energy effects. The thermodynamics-based strain gradient model is utilized to account for the small-scale effect (nonlocality) of the bar-bulk material while the Gurtin-Murdoch surface theory is adopted to capture the surface-energy effect. To consider the bar-surrounding substrate interactive mechanism, the Winkler foundation model is called for. The governing differential compatibility equation as well as the consistent end-boundary compatibility conditions are revealed using the virtual force principle and form the core of the model formulation. Within the framework of the virtual force principle, the axial force field serves as the fundamental solution to the governing differential compatibility equation. The problem of a nanowire embedded in an elastic substrate medium is employed as a numerical example to show the accuracy of the proposed bar-elastic substrate model and advantage over its counterpart displacement model. The influences of material nonlocality on both global and local responses are thoroughly discussed in this example. Compatibility (geochemistry) ; Boundary value problem ; Quantum nonlocality ; Elastic energy ; Mechanics ; Elasticity (physics) ; Classical mechanics ; Materials science ; Physics ; Mathematics ; Mathematical analysis ; Thermodynamics ; Composite material Nonlocal and gradient elasticity in micro/nano structures ; Numerical methods in engineering ; Composite Structure Analysis and Optimization
Authors: Beatrice Rosetti | Erica Scarel | Laura Colomina‐Alfaro | Simone Adorinni | Giovanni Pierri | Ottavia Bellotto | Kevin Mamprin | Maurizio Polentarutti | Antonella Bandiera | Consiglia Tedesco | Silvia Marchesan
Source: Polymers (article, 2022-10-27)
Field: Materials Science — Biomaterials

Self-Assembly of Homo- and Hetero-Chiral Cyclodipeptides into Supramolecular Polymers towards Antimicrobial Gels There is an increasing interest towards the development of new antimicrobial coatings, especially in light of the emergence of antimicrobial resistance (AMR) towards common antibiotics. Cyclodipeptides (CDPs) or diketopiperazines (DKPs) are attractive candidates for their ability to self-assemble into supramolecular polymers and yield gel coatings that do not persist in the environment. In this work, we compare the antimicrobial cyclo(Leu-Phe) with its heterochiral analogs cyclo(D-Leu-L-Phe) and cyclo(L-Leu-D-Phe), as well as cyclo(L-Phe-D-Phe), for their ability to gel. The compounds were synthesized, purified by HPLC, and characterized by <sup>1</sup>H-NMR, <sup>13</sup>C-NMR, and ESI-MS. Single-crystal X-ray diffraction (XRD) revealed details of the intermolecular interactions within the supramolecular polymers. The DKPs were then tested for their cytocompatibility on fibroblast cells and for their antimicrobial activity on <i>S. aureus</i>. Overall, DKPs displayed good cytocompatibility and very mild antimicrobial activity, which requires improvement towards applications. Supramolecular chemistry ; Antimicrobial ; Polymer ; Materials science ; Combinatorial chemistry ; Carbon-13 NMR ; Chemistry ; Nanotechnology ; Stereochemistry ; Crystallography ; Organic chemistry ; Crystal structure Supramolecular Self-Assembly in Materials ; Chemical Synthesis and Analysis ; Antimicrobial Peptides and Activities