jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Marcos López‐Aguilar | Marina Ramos‐Martín | Nicolás Ríos‐Lombardía | Luciana Cicco | Joaquín García‐Álvarez | Carmen Concellón | Vicente del Amo
Source: ChemCatChem (article, 2024-04-03)
Field: Chemistry — Organic Chemistry

Synergistic One‐pot Tandem Combination of Cu and Proline Catalysis: Stereodivergent Synthesis of Chiral Aldols from Primary Alcohols Abstract A new stereodivergent one‐pot tandem protocol, which granted diastereo‐ and enantioselective access to chiral aldols by starting from simple primary alcohols, is presented as a proof‐of‐concept. The synergistic combination of a chemoselective Cu(II)‐catalyzed oxidation of primary alcohols into the corresponding aldehydes (without the expected overoxidation into the corresponding carboxylic acids and using simple aerial O 2 as co‐oxidant), followed by a concomitant organocatalyzed enantioselective aldol coupling promoted by the system ( S )‐proline/HTBD‐BF 4 [TBD=1,5,7‐triazabicyclo[4.4.0]dec‐5‐ene], was achieved after fine‐tuning and compatibilizing the conditions required for the successful performance of both catalytic systems. Here, we demonstrated that selection and pairing of both catalysts needs to be extremely judicious to avoid orthogonality, kinetic, concentration or reciprocal poisoning issues. Refinement of the overall tandem protocol allowed us to design a synergistic and stereodivergent protocol which affords comparable or even better diastereoselective results than the organocatalytic system by itself. Finally, the following key factors (from a sustainable point of view) should be highlighted: i ) no external VOC solvents are needed during our one‐pot tandem synthetic protocol (by working under neat conditions); and ii ) isolation/purification of any intermediate is not required, thus reducing the chemical waste and energy/time costs, simplifying the practical aspects of our synthetic methodology. Tandem ; Enantioselective synthesis ; Chemistry ; Aldol reaction ; Combinatorial chemistry ; Catalysis ; Organocatalysis ; Primary (astronomy) ; Cascade reaction ; Organic chemistry ; Materials science Oxidative Organic Chemistry Reactions ; Asymmetric Synthesis and Catalysis ; Catalytic C–H Functionalization Methods
Authors: Pham Van Duong | Le Anh Thi | Le Duc Toan | Do Hoang Tung | Duong Hoang Hieu | Trung Le Canh | Nguyen Trong Tuyen | Minh Hoa Nguyễn
Source: Journal of Electronic Materials (article, 2024-10-24)
Field: Materials Science — Materials Chemistry

Thickness and Temperature-Dependent Traits of CdSe/CdSeS Heterostructure Nanocrystals Heterojunction ; Solid-state physics ; Nanocrystal ; Materials science ; Optoelectronics ; Nanotechnology ; Condensed matter physics ; Physics Quantum Dots Synthesis And Properties ; Chalcogenide Semiconductor Thin Films ; Advanced Semiconductor Detectors and Materials
Authors: Andrea Montero-Oleas | María Luz Martínez Ricci | Guillermo P. Ortiz | Philippe Trens | Yoann Roupioz | Stéphanie Kodjikian | M. Claudia Marchi | Xavier Cattoën | Sara A. Bilmes
Source: ChemRxiv (preprint, 2024-10-15)
Field: Materials Science — Electronic, Optical and Magnetic Materials

One-Pot Synthesis of Core-Shell Au@mSiO2 Nanoparticles for Photothermal Applications Gold-mesoporous silica (Au@mSiO2) core-shell nanoparticles (NPs) hold great promise for application in nanomedicine, as they enable the photostimulated release of guest molecules located within their pores. In this study, prioritizing the achievement of atom economy, we used a one-pot synthesis protocol, to produce core-shell Au@mSiO2 NPs from a properly defined precursor state. Upon sodium hydroxide addition, the formation of gold NPs occurs quickly, followed by the formation of a silica shell, eliminating the need to isolate the gold cores. We conducted a comprehensive mechanistic analysis that elucidates the relative kinetics of gold and silica formation, identifying key factors for fine-tuning NPs within the size range of 50 to 100 nm, ideal for biological applications. The photothermal properties of such Au@mSiO2 were characterized and modelled. Under the experimental conditions typically used for cargo release experiments, the model predicts a temperature increase for a single particle of less than 10^(-4) °C, demonstrating that the release is due to the collective heating of the medium by a myriad of NPs rather than by the temperature elevation of individual NPs under irradiation. Overall, the studies developed here will enable more effective design and preparation of Au@mSiO₂ particles, optimizing them for a broad range of photothermal applications. Photothermal therapy ; Nanotechnology ; Nanoparticle ; Colloidal gold ; Mesoporous silica ; Materials science ; Nanomedicine ; Photothermal effect ; Particle (ecology) ; Mesoporous material ; Hydroxide ; Chemical engineering ; Chemistry ; Catalysis ; Organic chemistry Gold and Silver Nanoparticles Synthesis and Applications ; Catalytic Processes in Materials Science ; Advanced Nanomaterials in Catalysis
Authors: Ya Chen | Y.H. Liu | Gaomou Xu | Tao Wang
Source: ChemRxiv (preprint, 2024-05-15)
Field: Materials Science — Materials Chemistry

Diverse Effects of Ferromagnetic-Paramagnetic Phase Transition on the Activity and Selectivity of Ferromagnetic Catalysts Tuning the catalyst's activity and selectivity is usually achieved by modifying the electronic structure through strategies such as alloying, doping, strain, and ligand modification, but inevitably accompanied by geometric structure changes of catalysts. It is challenging to modify a catalyst's electronic structure without changing its geometric structure. Recent studies found that the second-order ferromagnetic to paramagnetic (FM-PM) phase transition could promote catalytic performance without altering the geometric structures of active sites, which was also known as the magneto-catalytic effect (MCE). However, the understanding of the MCE is still incomplete. Herein, we conducted systematic density functional theory (DFT) calculations to clarify the complex reaction mechanisms for conversions of nitrogen-containing small molecules on both FM and PM Ni (111) surfaces. Our microkinetic modeling (MKM) results demonstrate that FM-PM phase transition promotes the N2O decomposition activity of FM Ni catalyst but decreases its activity for NO decomposition while showing a negligible influence on the activity of ammonia decomposition. These results indicate the promotion, inhibition, and disappearance mechanisms of MCE on the catalytic activity, which further changes the selectivity of different products. We anticipate the MCE will work as an effective strategy for fine-tuning the activity and selectivity of ferromagnetic catalysts in heterogeneous catalysis, providing an extra basis for rational catalyst design. Ferromagnetism ; Paramagnetism ; Selectivity ; Catalysis ; Condensed matter physics ; Phase transition ; Phase (matter) ; Materials science ; Transition metal ; Chemistry ; Physics ; Organic chemistry Catalytic Processes in Materials Science ; Catalysis and Hydrodesulfurization Studies ; Catalysis and Oxidation Reactions
Authors: S. C. Rakesh Roshan | N. Yedukondalu | R. Rakesh Kumar | Haw-Tyng Huang | Lars Ehm | John B. Parise
Source: Inorganic Chemistry (article, 2024-02-12)
Field: Materials Science — Materials Chemistry

Highly Anisotropic to Isotropic Nature and Ultralow Out-of-Plane Lattice Thermal Conductivity of Layered PbClF-Type Materials Materials with an extreme lattice thermal conductivity (κ<sub>l</sub>) are indispensable for thermal energy management applications. Layered materials provide an avenue for designing such functional materials due to their intrinsic bonding heterogeneity. Therefore, a microscopic understanding of the crystal structure, bonding, anharmonic lattice dynamics, and phonon transport properties is critically important for layered materials. Alkaline-earth halofluorides exhibit anisotropy from their layered crystal structure, which is strongly determined by axial bond(s), and it is attributed to the large axial ratio (<i>c</i>/<i>a</i> > 2) for CaBrF, CaIF, and SrIF, in which Br/I acts as a rattler, as evidenced from potential energy curves and phonon density of states. The low axial (<i>c</i>/<i>a</i>) ratio leads to relatively isotropic κ<sub>l</sub> values in the BaXF (X = Cl, Br, I) series. MXF (M = Ca, Sr, Ba) compounds exhibit highly anisotropic (a large phonon transport anisotropy ratio of 10.95 for CaIF) to isotropic (a small phonon transport anisotropy ratio of 1.49 for BaBrF) κ<sub>l</sub> values despite their iso-structure. Moreover, ultralow κ<sub>l</sub> (<1 W/m K) values have been predicted for CaBrF, CaIF, and SrIF in the out-of-plane direction due to weak van der Waals (vdWs) bonding. Overall, this comprehensive study on MXF compounds provides insights into designing low κ<sub>l</sub> layered materials with a large axial ratio by fine-tuning out-of-plane bonding from ionic to vdWs bonding. Anisotropy ; Chemistry ; Isotropy ; van der Waals force ; Phonon ; Condensed matter physics ; Thermal conductivity ; Crystal structure ; Anharmonicity ; Lattice energy ; Lattice (music) ; Crystallography ; Materials science ; Molecule ; Physics ; Optics ; Composite material Thermal properties of materials ; MXene and MAX Phase Materials ; Thermal Expansion and Ionic Conductivity
Authors: Tingting Yang | Zheng Zhang | Fei Tan | Huayu Liu | Xingyu Li | Hongqi Wang | Qing Yang
Source: Catalysts (article, 2024-12-24)
Field: Materials Science — Materials Chemistry

Modulation of the Coordination Environment of Graphene-Loaded NiFe-LDH and PbO2 Catalysts by Plasma for Oxygen Evolution Reaction The generation of hydrogen through water electrolysis represents a significant advancement in the transition towards low-carbon energy systems. Graphene-supported catalysts have demonstrated significant potential in improving the oxygen evolution reaction (OER) among several electrocatalysts utilised for this process. Nonetheless, attaining exact control over the morphology and electrical configuration of these catalysts continues to pose a considerable difficulty. This study presents the development of a highly effective electrocatalyst composed of graphene-supported NiFe LDH and PbO2, incorporating sulphur anions into the structure by a plasma jet treatment method. By optimising the ratio of sulphur anions, we were able to fine-tune the local coordination environment, which effectively adjusted the properties of the OH and OOH intermediates, thereby improving the OER catalytic performance. The plasma treatment introduced vacancy defects into the catalyst, further regulating its surface morphology and electronic structure. After sulphur anion optimisation, the graphene-supported catalyst exhibited excellent electrocatalytic performance in alkaline environments, achieving an OER overpotential of 228 mV at 100 mA·cm−2. This performance, along with exceptional stability, exceeds the majority of previously documented catalysts. The results underscore the promise of sulphur anion optimisation and plasma treatment in improving OER performance, providing significant insights for the advancement of highly effective water-splitting catalysts. Graphene ; Modulation (music) ; Catalysis ; Oxygen evolution ; Oxygen ; Materials science ; Chemistry ; Chemical engineering ; Nanotechnology ; Electrode ; Physics ; Electrochemistry ; Physical chemistry ; Biochemistry ; Engineering ; Organic chemistry ; Acoustics Catalytic Processes in Materials Science ; Electrocatalysts for Energy Conversion ; Supercapacitor Materials and Fabrication
Authors: V. Rajendran | K. R. Justin Thomas
Source: Synthetic Metals (article, 2024-11-27)
Field: Materials Science — Materials Chemistry

Recent advances and importance of triphenyl acrylonitrile system as an aggregation-induced emitter Acrylonitrile ; Common emitter ; Aggregation-induced emission ; Materials science ; Polymer chemistry ; Chemistry ; Polymer science ; Chemical engineering ; Nanotechnology ; Organic chemistry ; Polymer ; Optoelectronics ; Physics ; Engineering ; Optics ; Fluorescence Luminescence and Fluorescent Materials ; Molecular Sensors and Ion Detection ; Organic Light-Emitting Diodes Research
Authors: Song Xie | Yang Zhou | Hao Zhu | Xinyi Xu | Han Zhang | Cai Yuan | Mingdong Huang | Peng Xu | Jinyu Li | Yichang Liu
Source: Research Square (preprint, 2024-04-24)
Field: Chemistry — Organic Chemistry

Interface-driven structural evolution on diltiazem as novel uPAR inhibitors: From in silico design to in vitro evaluation <title>Abstract</title> The urokinase-type plasminogen activator receptor (uPAR) emerges as a key target for anti-metastasis owing to its pivotal role in facilitating the invasive and migratory processes of cancer cells. Recently, we identified the uPAR-targeting anti-metastatic ability of diltiazem (<bold>22</bold>), a commonly used antihypertensive agent. Fine-tuning the chemical structures of known hits represents a vital branch of drug development. To develop novel anti-metastatic drugs, we performed an interface-driven structural evolution strategy on <bold>22</bold>. The uPAR-targeting and anti-cancer abilities of this antiphypertenisve drug was identified by us recently. Based on <italic>in-silico</italic> strategy, including extensive molecular dynamics (MD) simulations, hierarchical binding free energy predictions, and ADMET profilings, we designed, sythesized and identified three new diltiazem derivatives (<bold>221-8</bold>, <bold>221-57</bold>, and <bold>221-68</bold>) as uPAR inhibitors. Indeed, all of these three derivatives exhibited uPAR-depending inhibitory activity against PC-3 cell line invasion at micromolar level. Particularly, derivatives <bold>221-68</bold> and <bold>221-8</bold> showed enhanced uPAR-dependent inhibitory activity against the tumor cell invasion compared to the original compound. Microsecond timesclae MD simulations demonstrated the optimized moiety of <bold>221-68</bold> and <bold>221-8</bold> forming more comprehensive interactions with the uPAR, highlighting the reasonbility of our stragy. This work introduces three novel uPAR inhibitors, which not only paves the way for the development of effective anti-metastatic therapeutics, but also emphasizes the efficacy and robustness of an <italic>in silico</italic>-based lead compound optimization strategy in drug design. Urokinase receptor ; In silico ; Chemistry ; Diltiazem ; Cancer research ; In vitro ; Biophysics ; Computational biology ; Cell ; Biology ; Biochemistry ; Gene Click Chemistry and Applications ; Enzyme function and inhibition ; Protease and Inhibitor Mechanisms
Authors: Alexandru‐Constantin Stoica | Madalin Damoc | Adrian Bele | Ioan‐Andrei Dascălu | Ana‐Maria Macsim | Sergiu Shova | Mihaela Dascălu | Maria Cazacu
Source: Reactive and Functional Polymers (article, 2024-03-02)
Field: Chemistry — Inorganic Chemistry

A 3D coordination polymer of Cd(II) with conformationally flexible mixed ligands as an active filler for silicone elastomers Crystallography ; Intermolecular force ; Coordination complex ; Chemistry ; Siloxane ; Polymer ; Materials science ; Ligand (biochemistry) ; Metal ; Molecule ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; Silicone and Siloxane Chemistry ; Polyoxometalates: Synthesis and Applications
Authors: Pyung Soo Lee | Elsa Tsegay Tikue | Su Kyung Kang | Hee Ju Ko | Se Wan Kim | Abduljelil Worku Sabir
Source: SSRN Electronic Journal (preprint, 2024-01-01)
Field: Chemistry — Inorganic Chemistry

Fabrication of Lta Zeolite Core and Uio-66 Shell Structures Via Surface Zeta Potential Modulation and Sequential Seeded Growth for Zeolite/Polymer Composite Membranes Zeolite ; Zeta potential ; Materials science ; Membrane ; Fabrication ; Composite number ; Chemical engineering ; Polymer ; Shell (structure) ; Core (optical fiber) ; Seeding ; Composite material ; Nanotechnology ; Chemistry ; Nanoparticle ; Catalysis ; Organic chemistry Zeolite Catalysis and Synthesis ; Chemical Synthesis and Characterization ; Muon and positron interactions and applications
Authors: Yiying Yang | Xiaotai Wang | Dongju Zhang
Source: SSRN Electronic Journal (preprint, 2024-01-01)
Field: Materials Science — Materials Chemistry

Illuminating Tandem Reactions Characterized by Temporal Separation of Catalytic Activities Via Dft Calculations: A Case Study of Ni-Catalyzed Alkyne Semi-Hydrogenation Alkyne ; Catalysis ; Tandem ; Combinatorial chemistry ; Chemistry ; Organic chemistry ; Materials science Machine Learning in Materials Science
Authors: Joanatan M. Bautista-Renedo | Joel Ireta
Source: Physical Chemistry Chemical Physics (article, 2024-01-01)
Field: Chemistry — Physical and Theoretical Chemistry

Spurious proton transfer in hydrogen bonded dimers In some hydrogen bonded systems, the proton may translocate along the hydrogen bond (hb) upon geometry optimization with electronic structure methods like density functional theory (DFT). Such proton transfer (pt) events, however, may be spurious. In this work, spurious pt events are investigated in a set of hydrogen bonded dimers formed with molecules HXN, where X stands for C, Si, Ge and Sn. It is found that standard approximations to the electronic exchange and correlation (xc) functional either predict spurious pt events or too strong hbs in all the (HXN)<sub>2</sub> dimers except the (HCN)<sub>2</sub> one. The latter result is revealed by comparing DFT calculations against wave function methods. Such spurious pt events may be avoided by fine-tuning the percentage of exact exchange (ex) in hybrid xc-functionals. It is shown that the minimum amount of ex to avoid a spurious pt event ranged from 8% to 90%, depending on the system, basis set and xc-functional approximation used. However, these fine-tuned xc-functionals inadequately describe the hb in the (HXN)<sub>2</sub> dimers. Moreover, it is determined that the spurious pt event originates from a wrong description of the isolated HXN molecules by xc-functionals that do not include ex or a small amount of it. Therefore, it is argued that one can determine if a pt event is spurious by analyzing the geometry and electronic structure of the isolated molecule. Spurious relationship ; Proton ; Hydrogen ; Chemical physics ; Chemistry ; Transfer (computing) ; Materials science ; Physics ; Computer science ; Organic chemistry ; Nuclear physics Chemical Reactions and Mechanisms ; Photochemistry and Electron Transfer Studies ; Chemical Reaction Mechanisms
Authors: Maximilian Seydi Kilic | Isabel Mae Merchant | E. Elliott | Justus Pawlak | Jules Brehme | Arthur Sander | Taisei Suzuki | Takuya Shiga | Masayuki Nihei | Franz Renz
Source: European Journal of Inorganic Chemistry (article, 2024-10-30)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Modification of the Spin Transition Properties in Hetero‐Anionic Iron(II)‐Triazole Complexes Abstract The phenomenon which is called spin crossover is known to occur in some coordination compounds with an octahedral ligand field and electron configurations from 3d 4 to 3d 7 . Thereby, a reversible transition between spin states (high spin and low spin state) is possible, through several external stimuli. Iron(II) triazole complexes exhibit this phenomenon at a wide range of temperatures depending on the ligands and anions used. For this reason, they are often considered for several possible practical applications. It is also possible to combine ligands or anions to modify the transition temperature. The latter of which was rarely discussed in the past. In this study we synthesized a series of iron(II)‐4‐Aminotriazole complexes, with different ratios of chloride‐ and tetrafluoroborate‐anions, of the formula [Fe(Atrz) 3 ]Cl 2−X (BF 4 ) X . We show that the combination of these anions leads to transition temperatures between those of their corresponding pure anion complexes. We furthermore present that a simple modification of the synthesis leads to a possible easy way of fine‐tuning transitions temperatures. Chemistry ; Transition metal ; Spin crossover ; Triazole ; 1,2,4-Triazole ; Spin transition ; Polymer chemistry ; Nanotechnology ; Crystallography ; Organic chemistry ; Catalysis Magnetism in coordination complexes ; Lanthanide and Transition Metal Complexes ; Metal complexes synthesis and properties
Authors: Alison Sy-min Chang | Melanie A. Kascoutas | Quinn Valentine | Kiera How | Rachel Thomas | Amanda K. Cook
Source: ChemRxiv (preprint, 2024-05-12)
Field: Chemistry — Inorganic Chemistry

Alkene Isomerization using a Heterogeneous Nickel-Hydride Catalyst Transition metal-catalyzed alkene isomerization is an enabling technology used to install an alkene distal to its original site. Due to their well-defined structure, homogeneous catalysts can be fine-tuned to optimize reactivity, stereoselectivity, and positional selectivity, but they often suffer from instability and non-recyclability. Heterogeneous catalysts are generally highly robust but continue to lack active-site specificity and are challenging to rationally improve through structural modification. Known single-site heterogeneous catalysts for alkene isomerization utilize precious metals and bespoke, expensive, and synthetically intense supports. Additionally, they generally have mediocre reactivity, inspiring us to develop a heterogeneous catalyst with an active site made from readily available compounds made of Earth-abundant elements. Previous work demonstrated that a very active homogeneous catalyst is formed upon protonation of Ni[P(OEt)3]4 by H2SO4, generating a [Ni–H]+ active site. This catalyst is incredibly active, but also decomposes readily, which severely limits its utility. Herein we show that by using a solid acid (sulfated zirconia, SZO300), not only is this de-composition prevented, but high activity is maintained, improved selectivity is achieved, and a broader scope of functional groups is tolerated. Preliminary mechanistic experiments suggest that the catalytic reaction likely goes through an intermolecular, two-electron pathway. A detailed kinetic study comparing the state-of-the-art Ni and Pd isomerization catalysts reveals that the highest activity and selectivity is seen with the Ni/SZO300 system. The reactivity of Ni/SZO300, is not limited to alkene isomerization; it is also a competent catalyst for hydroalkenylation, hydroboration, and hydrosilylation, demonstrating the broad application of this heterogeneous catalyst. Isomerization ; Alkene ; Nickel ; Catalysis ; Hydride ; Chemistry ; Photochemistry ; Organic chemistry ; Hydrogen Asymmetric Hydrogenation and Catalysis ; Catalysis and Oxidation Reactions ; Organometallic Complex Synthesis and Catalysis