jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Biju Basumatary | Hidetoshi Tsuruda | Dariusz W. Szczepanik | Jiyeon Lee | Jaehyeok Ryu | Shigeki Mori | Kyo Yamagata | Takayuki Tanaka | Atsuya Muranaka | Masanobu Uchiyama | Jiwon Kim | Masatoshi Ishida | Hiroyuki Furuta
Source: Angewandte Chemie (article, 2024-04-02)
Field: Materials Science — Materials Chemistry

Metalla‐Carbaporphyrinoids Consisting of an Acyclic N‐Confused Tetrapyrrole Analogue Served as Stable Near‐Infrared‐II Dyes Abstract We present herein the synthesis of novel pseudo ‐metalla‐carbaporphyrinoid species ( 1M : M=Pd and Pt) achieved through the inner coordination of palladium(II) and platinum(II) with an acyclic N‐confused tetrapyrrin analogue. Despite their tetrapyrrole frameworks being small, akin to well‐known porphyrins, these species exhibit an unusually narrow HOMO–LUMO gap, resulting in an unprecedentedly low‐energy absorption in the second near‐infrared (NIR‐II) region. Density functional theory (DFT) calculations revealed unique d π ‐p π ‐conjugated electronic structures involving the metal d π ‐ligand p π hybridized molecular orbitals of 1M . Magnetic circular dichroism (MCD) spectroscopy confirmed distinct electronic structures. Remarkably, the complexes feature an open‐metal coordination site in the peripheral NN dipyrrin site, forming hetero‐metal complexes ( 1Pd‐BF 2 and 1Pt‐BF 2 ) through boron difluoride complexation. The resulting hetero metalla‐carbaporphyrinoid species displayed further redshifted NIR‐II absorption, highly efficient photothermal conversion efficiencies ( η ; 62–65 %), and exceptional photostability. Despite the challenges associated with the theoretical and experimental assessment of d π ‐p π ‐conjugated metalla‐aromaticity in relatively larger (more than 18π electrons) polycyclic ring systems, these organometallic planar tetrapyrrole systems could serve as potential molecular platforms for aromaticity‐relevant NIR‐II dyes. Tetrapyrrole ; Chemistry ; Aromaticity ; Conjugated system ; HOMO/LUMO ; Photochemistry ; Density functional theory ; Ligand (biochemistry) ; Palladium ; Phosphole ; Helicene ; Ruthenium ; Crystallography ; Stereochemistry ; Molecule ; Computational chemistry ; Organic chemistry ; Polymer Porphyrin and Phthalocyanine Chemistry ; Nanoplatforms for cancer theranostics ; Luminescence and Fluorescent Materials
Authors: Tahereh Jasemizad | Jenny Malmström | Lokesh P. Padhye
Source: Environmental Science Water Research & Technology (article, 2024-01-01)
Field: Chemistry — Electrochemistry

Mechanistic investigation of the photocatalytic activity of PEDOT for aqueous contaminant removal: the role of iron and hydroxyl radicals Conducting polymers can be used as photocatalysts for aqueous contaminant remediation; however, if prepared using an iron source as an oxidant and/or dopant, they may suffer from leaching of iron during photocatalysis and misinterpretation of the results. Photocatalysis ; Aqueous solution ; Environmental remediation ; Radical ; Leaching (pedology) ; Dopant ; Zerovalent iron ; Chemistry ; Environmental chemistry ; Contamination ; Inorganic chemistry ; Materials science ; Catalysis ; Doping ; Environmental science ; Organic chemistry ; Adsorption Electrochemical Analysis and Applications ; Analytical Chemistry and Sensors ; Conducting polymers and applications
Authors: Bárbara Maria Teixeira Costa Peluzo | Renaldo T. Moura | Elfi Kraka
Source: Research Square (preprint, 2024-03-19)
Field: Chemistry — Inorganic Chemistry

Extraction of uranyl from spent nuclear fuel wastewater via complexation - a local vibrational mode study <title>Abstract</title> The efficient extraction of uranyl from spent nuclear fuel wastewater for subsequent reprocessing and reuse in the nuclear cycle is an essential effort towards minimization of long-lived radioactive waste. N-substituted amides and Schiff base ligands are propitious candidates, where extraction occurs via complexation with the uranyl moiety. In this study, we utilized the local vibra- tional modes theory, paired with QTAIM and NBO analyses, to explore chemical bonding in uranyl nitrate, two uranyl picolinamide, one uranyl Schiff base, and three uranyl diamide complexes. The major focus was on (i) the assessment of the equatorial uranyl-ligand O-U and N-U bonding, includ- ing the question of chelation, and (ii) how the strength of the axial uranium oxygen U=O bonds of the uranyl moiety change upon complexation. Our results reveal that the strength of the equatorial uranium-ligand interactions correlates with their covalent character and with charge donation from the O and N lone pairs into the vacant uranium orbitals. We also found an inverse relationship between the covalent character of the equatorial ligand bonds and the strength of the axial uranium-oxygen bond. In summary, our study provides valuable data for a strategic modulation of N-substituted amide and Schiff base ligands towards maximization of uranyl extraction. <bold>Methods</bold>: Quantum chemistry calculations were performed with the PBE0 level of theory, where relativistic effects were accounted for via the NESCau Hamiltonian, implemented in Cologne2020, interfaced with Gaussian16. We use a cc-pwCVTZ-X2C basis set for uranium and Dunning’s cc-pVTZ for the remaining atoms. Uranium-ligand bonding was analyzed with LModeA (local vibrational mode analysis), AIMALL (QTAIM analysis), and NBO 7.0 f(NBO analysis. Uranyl ; Wastewater ; Extraction (chemistry) ; Actinide ; Spent nuclear fuel ; Mode (computer interface) ; Chemistry ; Nuclear chemistry ; Waste management ; Environmental science ; Uranium ; Materials science ; Computer science ; Engineering ; Metallurgy ; Chromatography Radioactive element chemistry and processing
Authors: Emanuele Pompei | Ylea Vlamidis | Letizia Ferbel | Valentina Zannier | S. Rubini | Daniel Arenas Esteban | Sara Bals | C. Marinelli | Georg Pfusterschmied | Markus Leitgeb | U. Schmid | Stefan Heun | Stefano Veronesi
Source: Nanoscale (article, 2024-01-01)
Field: Materials Science — Materials Chemistry

Functionalization of three-dimensional epitaxial graphene with metal nanoparticles We demonstrate the first successful functionalization of epitaxial three-dimensional graphene with metal nanoparticles. The functionalization is obtained by immersing three-dimensional graphene in a nanoparticle colloidal solution. This method is versatile and demonstrated here for gold and palladium, but can be extended to other types of nanoparticles. We have measured the nanoparticle density on the top surface and in the porous layer volume by scanning electron microscopy and scanning transmission electron microscopy. The samples exhibit a wide coverage of nanoparticles with minimal clustering. We demonstrate that high-quality graphene promotes the functionalization, leading to higher nanoparticle density both on the surface and in the pores. X-ray photoelectron spectroscopy shows the absence of contamination after the functionalization process. Moreover, it confirms the thermal stability of the Au- and Pd-functionalized three-dimensional graphene up to 530 °C. Our approach opens new avenues for utilizing three-dimensional graphene as a versatile platform for catalytic applications, sensors, and energy storage and conversion. Materials science ; Graphene ; Surface modification ; Nanotechnology ; Epitaxy ; Metal ; Thermal stability ; Nanoparticle ; Porosity ; Chemical engineering ; Composite material ; Metallurgy Graphene research and applications ; Supercapacitor Materials and Fabrication ; Graphene and Nanomaterials Applications
Authors: Lewis E. MacKenzie | Kirton, Peter
Source: arXiv (Cornell University) (preprint, 2024-12-17)
Field: Materials Science — Materials Chemistry

Superfluorescent upconversion nanoparticles as an emerging second generation quantum technology material Superfluorescence (SF) in lanthanide doped upconversion nanoparticles (UCNPs) is a room-temperature quantum phenomenon, first discovered in 2022. In a SF process, the many emissive lanthanide ions within a single UCNP are coherently coupled by an ultra-short (ns or fs) high-power excitation laser pulse. This leads to a superposition of excited emissive states which decrease the emissive lifetime of the UCNP by a factor proportional to the square of the number of lanthanide ions which are coherently coupled. This results in a dramatic decrease in UCNP emission lifetime from the microsecond regime to the nanosecond regime. Thus SF offers a tantalizing prospect to achieving superior upconversion photon flux in upconversion materials, with potential applications such as imaging and sensing. This perspective article contextualizes how SF-UCNPs can be regarded as a second generation quantum technology, and notes several challenges, opportunities, and open questions for the development of SF-UCNPs. Photon upconversion ; Nanoparticle ; Nanotechnology ; Quantum dot ; Optoelectronics ; Quantum ; Materials science ; Computer science ; Physics ; Doping ; Quantum mechanics Luminescence Properties of Advanced Materials ; Radiation Detection and Scintillator Technologies ; Photorefractive and Nonlinear Optics
Authors: Linh Wei Tran | Romain Berraud‐Pache | Maguy Jaber
Source: ChemRxiv (preprint, 2024-02-21)
Field: Chemistry — Analytical Chemistry

Rapid and complete prediction of Madder natural dyes’ color and properties through computational method Experimental chemists traditionally hold experimentation in high regard, but computational chemistry has the potential to revolutionize this perspective. Our work exemplifies this shift, employing computational methods such as Density Functional Theory (DFT), Time-Dependent Density Functional Theory (TD-DFT), and Quantum Mechanic/Molecular Mechanic (QM/MM) to delve into the realm of photodegradation of color. Focused on Madder dye, a natural and historical pigment renowned for its diverse color properties, we tackle challenges that traditional experimentation struggled to address. The historical difficulty in deciphering the spectroscopic properties of Madder's colorants due to extraction challenges, impurities, and high costs is overcome through computational spectroscopy techniques. By marrying computational insights with experimental data, we predict UV-Vis, color, and NMR spectra, considering factors like pH, solvent effects, and conformers. The study underscores the impact of solute-solvent interactions on reproducing experimental measurements, laying the foundation for a comprehensive database to understand color properties in cultural heritage. These initial findings pave the way for future exploration of complex systems like Madder lake. This transformative shift empowers researchers and scientists to conquer crucial challenges in comprehending the properties of ancient colors for cultural heritage preservation, advancing the development of durable bio-sourced colors, and discovering new color applications. Cultural heritage ; Density functional theory ; Computer science ; Chemistry ; Realm ; Computational chemistry ; Biochemical engineering ; Artificial intelligence ; Archaeology ; Engineering ; Geography Dye analysis and toxicity ; Cultural Heritage Materials Analysis ; Pigment Synthesis and Properties
Authors: Hassan A. Hassan | Kar Tim Chan | Nurisya Mohd Shah | Norhazilan Md Noor | C. H. Raymond Ooi
Source: Modelling and Simulation in Materials Science and Engineering (article, 2024-11-26)
Field: Materials Science — Materials Chemistry

Strain effect on structural, electronic and optical properties of Gra/MoS<sub>2</sub> heterobilayer Abstract Heterobilayers formed by stacking graphene and MoS 2 monolayers have been successfully synthesized in the laboratory, presenting a highly promising material with versatile applications due to its flexibility and enhanced optical properties. In this study, we employ density functional theory to investigate the impact of biaxial and uniaxial strain on the structural, electronic and optical properties of Graphene/MoS 2 (Gra/MoS 2 ) heterobilayer. The unstrained Gra/MoS 2 is shown to be a thermodynamically stable structure with binding energy <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" overflow="scroll"> <mml:mrow> <mml:mo>−</mml:mo> <mml:mn>0.736</mml:mn> </mml:mrow> </mml:math> eV and a band gap of 1.899 meV, which opens at the Dirac point of graphene. Gra/MoS 2 is also shown to have a better refractive index and absorption coefficient when compared to MoS 2 monolayer in the visible region. Under biaxial strain, heterobilayer became unstable as the structure of both monolayers changed. The variation of biaxial strain from −4% to 4% enables tuning of the band gap within a range of 1.07–6.623 meV. The Fermi level shifted towards the conduction band under compressive strain and towards the valence band under expansive strain. Manipulation of biaxial strain also facilitates tunability in energy peaks for optical properties such as the real and imaginary parts of the dielectric function, refractive index and absorption coefficient in the visible spectrum. In contrast, uniaxial strain induces minimal changes in the overall structure and stability of the heterobilayer, resulting in a limited band gap range of 1.118–2.4 meV. Furthermore, uniaxial strain fails to introduce significant tunability in the optical properties of the heterobilayer. Materials science ; Strain (injury) ; Composite material 2D Materials and Applications ; Chalcogenide Semiconductor Thin Films ; Heusler alloys: electronic and magnetic properties
Authors: Ghazal Borhan | Mehdi Sahihi
Source: Journal of Molecular Graphics and Modelling (article, 2024-10-11)
Field: Materials Science — Materials Chemistry

Unwinding DNA strands by single-walled carbon nanotubes: Molecular docking and MD simulation approach Carbon nanotube ; Molecular dynamics ; DNA ; Docking (animal) ; Materials science ; Nanotechnology ; Chemistry ; Computational chemistry ; Biochemistry ; Medicine Carbon Nanotubes in Composites ; Advanced biosensing and bioanalysis techniques ; Nanopore and Nanochannel Transport Studies
Authors: Nwar Egbaria | Mohamed Agbaria | Veniamin A. Borin | Roy E. Hoffman | Benny Bogoslavsky | Igor Schapiro | Zackaria Nairoukh
Source: Chemistry - A European Journal (article, 2024-07-11)
Field: Materials Science — Materials Chemistry

The Conformational Behaviour of Fluorinated Tetrahydrothiopyran We present a comprehensive study on the conformational behavior of diversely substituted 4-fluorotetrahydrothiopyran derivatives. Through quantum chemical simulations including DFT as well as NBO and NPA analysis, we elucidate the pivotal role of electrostatic interactions, occasionally complemented by hyperconjugative interactions, in stabilizing axial fluorine conformers. Less polar conformers were occasionally obtained, attributed to the interplay of electrostatic and hyperconjugative interactions. Experimental validation through NMR spectroscopy aligns with the computational analysis, thus providing a coherent understanding of the structural dynamics of these compounds. Conformational isomerism ; Natural bond orbital ; Computational chemistry ; Quantum chemical ; Chemistry ; Polar ; Fluorine ; Electrostatics ; Nuclear magnetic resonance spectroscopy ; Molecular dynamics ; Chemical physics ; Molecule ; Stereochemistry ; Density functional theory ; Physics ; Physical chemistry ; Organic chemistry ; Quantum mechanics Photochromic and Fluorescence Chemistry ; Organic Chemistry Cycloaddition Reactions ; Molecular spectroscopy and chirality
Authors: Akari Sugano | Natsuki Inaba | Keitaro Matsuoka | Kazuki Sada
Source: ChemRxiv (preprint, 2024-01-30)
Field: Chemistry — Organic Chemistry

Water-Soluble Soft Nylons: Novel Class of Soft Matter Exhibiting LCST-type Thermo-Responsiveness High crystallinity and low solubility are inherent characteristics of polyamides. Research efforts have primarily focused on exploring their bulk properties as fibers, with less emphasis on their solution properties. Herein, we report on the synthesis and properties of soft and soluble N-methylated nylons as a novel class of soft polymer matter. Surprisingly, N-methylated nylons have scarcely been reported and are almost not registered with CAS SciFindern, while their unit structure is very simple. The N-methylation of nylons resulted in softness and high solubility by eliminating hydrogen bonds between polymer backbones and generating two conformers (cis and trans) of the tertiary amide group. Remarkably, some of them exhibit lower critical solution temperature (LCST)-type phase separation in water. By manipulating the carbon number within polymer backbones, we have found that the quantitative hydrophilic/hydrophobic balance for LCST is its unit formula per amide group equal to C6H11NO, which aligns with typical LCST polymers like poly(N-isopropylacrylamide) (PNIPAM). Despite the structural similarity to PNIPAM, polymer scientists have never found LCST-type behavior of N-methylated nylons during over 50 years of soft polymer matter research. The long-standing assumption that polyamides are inherently rigid and cannot exhibit softness and solubility has impeded their application to soft polymer matter. Lower critical solution temperature ; Soft matter ; Type (biology) ; Chemistry ; Materials science ; Composite material ; Polymer ; Biology ; Copolymer ; Organic chemistry ; Ecology Advanced Polymer Synthesis and Characterization ; biodegradable polymer synthesis and properties ; Hydrogels: synthesis, properties, applications
Authors: Lars‐Åke Näslund | Esko Kokkonen | Martin Magnuson
Source: arXiv (Cornell University) (preprint, 2024-04-04)
Field: Materials Science — Materials Chemistry

Interaction and kinetics of H2, CO2, and H2O on Ti3C2Tx MXene probed by X-ray photoelectron spectroscopy One of the most explored MXenes is Ti3C2Tx, where Tx is designated to inherently form termination species. Among many applications, Ti3C2Tx is a promising material for energy storage, energy conversion, and CO2-capturing devices. However, active sites for adsorption and surface reactions on the Ti3C2Tx-surface are still open questions to explore, which have implications for preparation methods when to obtain correct and optimized surface requirements. Here we use X-ray photoelectron spectroscopy (XPS) to study the adsorption of common gas molecules such as H2, CO2, and H2O, which all may be present in energy storage, energy converting, and CO2-capturing devices based on Ti3C2Tx. The study shows that H2O, with a strong bonding to the Ti-Ti bridge-sites, can be considered as a termination species. An O and H2O terminated Ti3C2Tx-surface restricts the CO2 adsorption to the Ti on-top sites and may reduce the ability to store positive ions, such as Li+ and Na+. On the other hand, an O and H2O terminated Ti3C2Tx-surface shows the capability to split water. The results from this study have implications for the correct selection of MXene preparations and the environment around the MXene in different implementations, such as energy storage, CO2-capturing, energy conversion, gas sensing, and catalysts. X-ray photoelectron spectroscopy ; Adsorption ; Materials science ; Spectroscopy ; X-ray spectroscopy ; Chemical engineering ; Chemistry ; Physical chemistry ; Physics ; Engineering MXene and MAX Phase Materials ; 2D Materials and Applications ; Inorganic Chemistry and Materials
Authors: Jun Qian | Liang Ma | Yida Wang
Source: Zeitschrift für Kristallographie - New Crystal Structures (article, 2024-10-28)
Field: Chemistry — Organic Chemistry

Crystal structure of (3,6-di(2-pyridyl)-4-phenylaminopyridazine-κ<sup>2</sup>N,N′)-bis(2-(p-toluene)pyridinyl-κ<sup>2</sup>C,N)-iridium(III) hexafluorophosphate –dichloromethane (1/1), C<sub>45</sub>H<sub>37</sub>Cl<sub>2</sub>F<sub>6</sub>IrN<sub>7</sub>P Abstract C 45 H 37 Cl 2 F 6 IrN 7 P, monoclinic, P 2 1 / c (no. 14), a = 23.518(5) Å, b = 11.702(2) Å, c = 15.426(3) Å, β = 101.44(3)°, V = 4161.0(15) Å 3 , Z = 4, R gt ( F ) = 0.0474, wR ref ( F 2 ) = 0.0924, T = 293 K. Iridium ; Hexafluorophosphate ; Toluene ; Dichloromethane ; Chemistry ; Crystal structure ; Medicinal chemistry ; Crystallography ; Organic chemistry ; Solvent ; Catalysis Synthesis and Reactivity of Heterocycles ; Catalytic Cross-Coupling Reactions ; Synthesis and Characterization of Heterocyclic Compounds
Authors: Chloé Puteaux | Isabelle Toubia | Lina Truong | Marie Hubert‐Roux | Laëtitia Bailly | Hassan Oulyadi | Pierre‐Yves Renard | Cyrille Sabot
Source: Angewandte Chemie International Edition (article, 2024-07-14)
Field: Chemistry — Organic Chemistry

Light‐Induced Unlocking Reactivity of Fragments for Fast Target‐Guided Synthesis of Carbonic Anhydrase Inhibitors We showcase the successful combination of photochemistry and kinetic target-guided synthesis (KTGS) for rapidly pinpointing enzyme inhibitors. KTGS is a fragment-based drug discovery (FBDD) methodology in which the biological target (BT) orchestrates the construction of its own ligand from fragments featuring complementary reactive functionalities. Notably, fragments interacting with the protein binding sites leverage their spatial proximity, facilitating a preferential reaction. Consequently, the resulting bivalent ligand exhibits heightened affinity. Within the realm of KTGS strategies, in situ click chemistry stands out as the most widely used to identify potent protein binders. This approach requires significant protein contributions, such as binding interactions and appropriate orientations of fragments, to overcome high activation barriers. This leads to prolonged incubation times and the potential for generating false negatives, thereby limiting this strategy to proteins that are stable enough in buffer. We herein unveil the possibility to integrate photochemistry into the realm of KTGS, accelerating the ligation reaction between fragments to a time scale of minutes. This approach should significantly expand the narrow reactivity window of traditional KTGS reactions, paving the way for the exploration and development of novel photo-KTGS reactions. Chemistry ; Carbonic anhydrase ; Combinatorial chemistry ; Target protein ; Ligand (biochemistry) ; Carbonic anhydrase II ; Drug discovery ; Limiting ; Enzyme ; Click chemistry ; Ligand efficiency ; Biophysics ; Computational biology ; Biochemistry ; Biology ; Receptor Click Chemistry and Applications ; Chemical Synthesis and Analysis ; Synthesis and Catalytic Reactions