jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Bastian Achenbach | Lena‐Marie Liedtke | Christian Näther | Erik Svensson Grape | A. Ken Inge | Norbert Stock
Source: Chemistry - A European Journal (article, 2024-10-11)
Field: Materials Science — Materials Chemistry

Unlocking the Chemical and Structural Complexity of Aluminum Hydroxy Acetates: from Commodity Chemicals to Porous Materials Aluminum acetates have been in use for more than a century, but despite their widespread commercial applications, essential scientific knowledge of their synthesis-structure-property relationships is lacking. High-throughput screening, followed by fine tuning and extensive optimization of reaction conditions using Al<sup>3+</sup>, OH<sup>-</sup> and CH<sub>3</sub>COO<sup>-</sup> ions, has unraveled their complex synthetic chemistry, yielding for the first time the four phase pure products Al(OH)(O<sub>2</sub>CCH<sub>3</sub>)<sub>2</sub> ⋅ x H<sub>2</sub>O (x=0, 2) (1A and CAU-65, 1B), Al<sub>3</sub>O(HO<sub>2</sub>CCH<sub>3</sub>)(O<sub>2</sub>CCH<sub>3</sub>)<sub>7</sub> (2), and the porous aluminum salt [Al<sub>24</sub>(OH)<sub>56</sub>(CH<sub>3</sub>COO)<sub>12</sub>](OH)<sub>4</sub> (CAU-55-OH, 3). Structure determination by electron and X-ray diffraction was carried out and the data suggested porosity for 1B and 3, which was confirmed by physisorption experiments. Even the scale-up to the 10 L scale was accomplished for 1A, 1B and 3 with yields of up to 1.1 kg (99 %). This study of a seemingly simple chemical system provides important information on both fundamental inorganic chemistry and porous materials. Physisorption ; Porosity ; Aluminium ; Chemistry ; Porous medium ; Chemical engineering ; Nanotechnology ; Materials science ; Inorganic chemistry ; Organic chemistry ; Catalysis ; Engineering Mesoporous Materials and Catalysis ; Layered Double Hydroxides Synthesis and Applications ; Chemical Synthesis and Characterization
Authors: Ji Ma | Xinliang Feng
Source: Chem (article, 2024-01-24)
Field: Materials Science — Materials Chemistry

Chain-growth polymerization enables the controlled synthesis of graphene nanoribbons Graphene nanoribbons ; Polymerization ; Nanotechnology ; Materials science ; Graphene ; Polymer ; Composite material Graphene research and applications ; Molecular Junctions and Nanostructures ; Conducting polymers and applications
Authors: Gang Hu | Qinqin Wang | Mingyuan Zhu | Lihua Kang
Source: Chinese Journal of Chemical Engineering (article, 2024-12-26)
Field: Materials Science — Materials Chemistry

Heteropolyacid hosted to nano-silica catalyst for the oxidation of methacrolein Methacrolein ; Catalysis ; Nano- ; Chemical engineering ; Materials science ; Nanotechnology ; Chemistry ; Organic chemistry ; Engineering ; Copolymer ; Methacrylic acid Polyoxometalates: Synthesis and Applications ; Mesoporous Materials and Catalysis ; Oxidative Organic Chemistry Reactions
Authors: Razan E. Daoud | Anna Orlando | Alberto Rampino | Matteo Tretti | Massimo Desando | Daniele Padula | Thorsten Hansen | Luca De Vico
Source: The Journal of Physical Chemistry B (article, 2024-12-25)
Field: Chemistry — Spectroscopy

Computational Design of (B)Chl Models: Structural and Chemical Modifications toward Enriched Properties The functional units of natural photosynthetic systems control the process of converting sunlight into chemical energy. In this article, we explore a series of chemically and structurally modified bacteriochlorophyll and chlorophyll pigments through computational chemistry to evaluate their electronic spectroscopy properties. More specifically, we use multiconfigurational and time-dependent density functional theory methods, along with molecular dynamics simulations, to compute the models' energetics both in an implicit and explicit solvent environment. Structural modifications aimed at reducing the planarity of the macrocycle through alkyl-bridge anchoring reveal the significant role of the curvature in fine-tuning spectral properties, which mimics protein scaffold effects on naturally occurring pigments. Furthermore, chemical substitutions with a carbonyl group show potential for expanding absorption spectra toward the blue region, while incorporating an additional double bond decreases absorption efficiency. These insights lay the groundwork to design novel synthetic pigments, with potential applications in artificial light-harvesting systems and more efficient photovoltaic devices. Chemistry ; Computer science Molecular spectroscopy and chirality ; Advanced NMR Techniques and Applications ; Advanced Chemical Physics Studies
Authors: Givi Kalandia | Cuilian Liu | David E. Salazar Marcano | Mhamad Aly Moussawi | Sem Bleus | Bart Van Meerbeek | Wim Dehaen | Tatjana N. Parac‐Vogt
Source: Angewandte Chemie (article, 2024-11-13)
Field: Materials Science — Materials Chemistry

Host‐Guest Assemblies of Polyoxovanadate Clusters as Supramolecular Catalysts Abstract Supramolecular functional materials can be used to overcome some of the most challenging tasks in materials science, where the dynamic nature of supramolecular interactions can be leveraged to fine‐tune the properties of the material for a given task. The Lindqvist hexavanadate family of polyoxometalates (POMs) have emerged as particularly interesting candidates to be used in supramolecular materials due to their redox and Lewis acid properties that enable their application in the fields of energy conversion/storage or catalysis. Despite their promising potential, hexavanadate clusters are underrepresented in the field of supramolecular materials, mainly due to the synthetic challenges related to their inherent reactivity. In this work, pillar[5]arene was successfully grafted onto a Lindqvist hexavanadate and the resulting structure was confirmed by single crystal X‐ray diffraction (SC‐XRD), presenting the first example of a crystal structure of a POMcovalently functionalized with a pillar[5]arene. By introducing a ditopic guest molecule that could interlink pillar[5]arene moieties, host–guest interactions were leveraged as the driving force for the formation of supramolecular assemblies incorporating hexavanadate clusters in a controlled manner. The enhanced catalytic performance of the resulting aggregates confirmed their potential application as functional catalytic materials. This novel approach for developing hexavanadate‐based catalysts reported here showcases the potential of using host–guest interactions as a means to introduce catalytically active metal‐oxo clusters into supramolecular frameworks. Supramolecular chemistry ; Catalysis ; Chemistry ; Host–guest chemistry ; Nanotechnology ; Host (biology) ; Supramolecular catalysis ; Materials science ; Molecule ; Organic chemistry Polyoxometalates: Synthesis and Applications ; Metal-Organic Frameworks: Synthesis and Applications ; Vanadium and Halogenation Chemistry
Authors: Raj Laxmi | Biplab Kumar Kuila | Neelam Gupta | Anamika Anamika | Anand Maurya | Ravi Prakash Behere | Rahul Sharma | Biswajit Maiti
Source: ACS Applied Polymer Materials (article, 2024-12-11)
Field: Materials Science — Materials Chemistry

Fluorene and Triazine-Based Conjugated Polymer Networks with Tuned Frontier Orbital Energy Levels for Improving Organic Photocatalysis Here, we describe a method for fine-tuning the frontier orbital energy levels or redox potential of a conjugated polymer network (CPN) consisting of triazine and fluorene by systematically introducing electron-withdrawing groups at the fluorene moiety through simple structural modification. The band gap of CPN decreases with an increase in the strength of the electron-withdrawing group, and the relative position of the frontier orbital energy becomes more favorable for reactions like photocatalytic aerobic oxidation, which has been further confirmed by theoretical and experimental studies. The CPN with a CN group at the 9 position of fluorene (CPN3) shows the maximum photocatalytic activity (32% higher) compared to CPN1 (hydrogen at the 9 position) in white light. The best-performing catalyst CPN3 was further employed for photocatalytic reactions under white light, like the oxidation of alcohols to carbonyl and boronic acid to the corresponding alcohol, which show noteworthy characteristics like low catalyst loading, high yield, and selectivity with broad substrate scope (aliphatic, aromatic, biphenyl, and heterocyclic). CPN3 exhibited turnover frequencies of 13.33 and 10.9 mmol g–1 h–1 in 3 W blue and white LED lights, respectively, which are much higher than those of state-of-art photocatalysts. The recyclability of the catalyst was tested for up to 5 cycles without much change in the catalytic activity. The practical usefulness of the suggested method was further demonstrated by the CPN3-photocatalyzed gram-scale synthesis of high-value chemicals such as acetophenone from 1-phenylethanol and phenol from phenylboronic acid. Fluorene ; Conjugated system ; Triazine ; Frontier ; Photocatalysis ; Materials science ; Polymer ; Photochemistry ; Chemistry ; Polymer chemistry ; Organic chemistry ; Composite material ; Geography ; Catalysis Covalent Organic Framework Applications ; Metal-Organic Frameworks: Synthesis and Applications ; Advanced Photocatalysis Techniques
Authors: Nirob K. Saha | William S. Salvia | Dominik Konkolewicz | C. Scott Hartley
Source: Angewandte Chemie (article, 2024-05-21)
Field: Chemistry — Organic Chemistry

Transient Covalent Polymers through Carbodiimide‐Driven Assembly Abstract Biochemical systems make use of out‐of‐equilibrium polymers generated under kinetic control. Inspired by these systems, many abiotic supramolecular polymers driven by chemical fuel reactions have been reported. Conversely, polymers based on transient covalent bonds have received little attention, even though they have the potential to complement supramolecular systems by generating transient structures based on stronger bonds and by offering a straightforward tuning of reaction kinetics. In this study, we show that simple aqueous dicarboxylic acids give poly(anhydrides) when treated with the carbodiimide EDC. Transient covalent polymers with molecular weights exceeding 15,000 are generated which then decompose over the course of hours to weeks. Disassembly kinetics can be controlled using simple substituent effects in the monomer design. The impact of solvent polarity, carbodiimide concentration, temperature, pyridine concentration, and monomer concentration on polymer properties and lifetimes has been investigated. The results reveal substantial control over polymer assembly and disassembly kinetics, highlighting the potential for fine‐tuned kinetic control in nonequilibrium polymerization systems. Carbodiimide ; Covalent bond ; Polymer ; Transient (computer programming) ; Chemistry ; Polymer chemistry ; Materials science ; Organic chemistry ; Computer science Advanced Polymer Synthesis and Characterization ; Synthetic Organic Chemistry Methods ; Catalytic Cross-Coupling Reactions
Authors: Agnideep Das | Oscar Charpentier | Cheriehan Hessin | Jules Schleinitz | David Pianca | Nolwenn Le Breton | Sylvie Choua | Laurence Grimaud | Christophe Gourlaouen | Marine Desage‐El Murr
Source: Angewandte Chemie (article, 2024-04-17)
Field: Chemistry — Organic Chemistry

Site‐Selective Radical Aromatic C−H Functionalization of Alloxazine and Flavin through Ground‐State Single Electron Transfer Abstract Flavins and their alloxazine isomers are key chemical scaffolds for bioinspired electron transfer strategies. Their properties can be fine‐tuned by functional groups, which must be introduced at an early stage of the synthesis as their aromatic ring is inert towards post‐functionalization. We show that the introduction of a remote metal‐binding redox site on alloxazine and flavin activates their aromatic ring towards direct C−H functionalization. Mechanistic studies are consistent with a synthetic sequence involving ground‐state single electron transfer (SET) with an electrophilic source followed by radical‐radical coupling. This unprecedented reactivity opens new opportunities in molecular editing of flavins by direct aromatic post‐functionalization and the utility of the method is demonstrated with the site‐selective C6 functionalization of alloxazine and flavin with a CF 3 group, Br or Cl, that can be further elaborated into OH and aryl for chemical diversification. Surface modification ; Flavin group ; Electron transfer ; Chemistry ; Ground state ; Photochemistry ; Organic chemistry ; Atomic physics ; Physics ; Physical chemistry Radical Photochemical Reactions ; Fluorine in Organic Chemistry ; Catalytic C–H Functionalization Methods
Authors: Kiara L. Lacy | Sujeung Lim | Emil Lundqvist | Yuyao Kuang | Harrison C. Jeong | Tayloria N. G. Adams | Herdeline Ann M. Ardoña
Source: ChemSystemsChem (article, 2024-10-10)
Field: Chemistry — Organic Chemistry

Non‐Uniform Electric Field Manipulation of Chromogenic Peptide Amphiphile Assemblies This work investigates the influence of dielectrophoretic forces on the structural features and the resulting aggregates of a chromogenic model system, peptide-diacetylene (D<sub>3</sub>GV-DA) amphiphiles. Here, we systematically investigate how non-uniform electric fields impact the (i) peptide-directed supramolecular assembly stage and (ii) topochemical photopolymerization stage of polydiacetylenes (PDAs) in a quadrupole-based dielectrophoresis (DEP) device, as well as the (iii) manipulation of D<sub>3</sub>GV-DA aggregates in a light-induced DEP (LiDEP) platform. The conformation-dependent chromatic phases of peptide-PDAs are utilized to probe the chain-level effect of DEP exposure after the supramolecular assembly or after the topochemical photopolymerization stage. Steady-state spectroscopic and microscopy analyses show that structural features such as the chirality and morphologies of peptidic 1-D nanostructures are mostly conserved upon DEP exposure, but applying mild, non-uniform fields at the self-assembly stage is sufficient for fine-tuning the chromatic phase ratio in peptide-PDAs and manipulating their aggregates via LiDEP. Overall, this work provides insights into how non-uniform electric fields offer a controllable approach to fine-tune or preserve the molecularly preset assembly order of DEP-responsive supramolecular or biopolymeric assemblies, as well as manipulate their aggregates using light projections, which have future implications for the precision fabrication of macromolecular systems with hierarchical structure-dependent function. Diacetylene ; Supramolecular chemistry ; Photopolymer ; Electric field ; Dielectrophoresis ; Nanotechnology ; Peptide ; Materials science ; Amphiphile ; Polydiacetylenes ; Self-assembly ; Chromatic aberration ; Chromatic scale ; Chemistry ; Crystallography ; Optics ; Polymerization ; Physics Polydiacetylene-based materials and applications ; Supramolecular Self-Assembly in Materials ; Antimicrobial Peptides and Activities
Authors: Nicolas Deroose | Laurens Parmentier | Bart Devreese | Peter Dubruel
Source: Biomacromolecules (article, 2024-12-02)
Field: Materials Science — Biomaterials

Enhanced Tunability of Photo-Cross-Linkable Silk Sericins from <i>Bombyx mori</i> Over the past decade, silk sericin has emerged as a promising material for biomedical applications, especially in tissue engineering, where fine-tuning the physicochemical properties is crucial. However, previous studies, including those on the methacrylation of sericin (yielding SS-MA), showed limited tunability. Here, we developed a photo-cross-linkable sericin-based material modified with 2-aminoethyl methacrylate (AEMA) using two synthesis routes: sequential modification of SS-MA with AEMA (SS-MA-AEMA) and an efficient one-pot synthesis (SS-AEMA). The one-pot synthesis yielded materials containing only methacrylate groups, unlike the sequential modification that yielded a combination of methacrylamides and methacrylates. Our approach resulted in superior physicochemical properties. The resulting materials, including the previously described SS-MA, exhibited a broad range of properties, such as cross-linking kinetics (0.9-64.0 s), swelling behavior (311-3775%), and mechanical properties (10-140 kPa). These properties support applications across various tissues, from dermis to fibrous tissue. The materials also demonstrated fibroblast cytocompatibility with cell viabilities exceeding 96%. Sericin ; Methacrylate ; SILK ; Bombyx mori ; Swelling ; Materials science ; Polymer chemistry ; Copolymer ; Dermis ; Tissue engineering ; Tissue transglutaminase ; Chemical engineering ; Chemistry ; Composite material ; Polymer ; Biomedical engineering ; Anatomy ; Organic chemistry ; Biochemistry ; Enzyme Silk-based biomaterials and applications ; Electrospun Nanofibers in Biomedical Applications ; Surface Modification and Superhydrophobicity
Authors: Drialys Cárdenas-Morcoso | Justine Debard | Faezeh Farzin | Nicolas D. Boscher
Source: Macromolecules (article, 2024-10-02)
Field: Materials Science — Polymers and Plastics

Triflate Salts as Alternative Non-Chlorinated Oxidants for the Oxidative Chemical Vapor Deposition and Electronic Engineering of Conjugated Polymers Oxidative chemical vapor deposition (oCVD) stands as an attractive approach for the synthesis, engineering, and integration of conjugated polymers for advanced electronic and optoelectronic applications. In oCVD, the oxidant significantly influences the conformational and optoelectronic properties of the resulting conjugated polymer thin films. In this work, triflate salts of iron(III) and copper(II) (Fe(OTf)<sub>3</sub> and Cu(OTf)<sub>2</sub>, respectively) are investigated for the first time as suitable alternative oxidants to the widely used iron(III) chloride (FeCl<sub>3</sub>) for the oCVD of conjugated polymers. Structural and compositional characterizations of the resulting thin films evidenced the successful polymerization of cobalt(II) 5,15-diphenyl porphyrin using either Fe(OTf)<sub>3</sub> or Cu(OTf)<sub>2</sub>. Along with an intermolecular dehydrogenative C-C coupling reaction, the occurrence of side reactions, such as the inclusion of -CF<sub>3</sub> groups and demetalation and subsequent insertion of copper(II) in the porphyrin macrocycle when using Cu(OTf)<sub>2</sub>, were evidenced. Interestingly, the inclusion of -CF<sub>3</sub> groups into the polymer backbone when using triflate salts results in a deepening of the frontier energy levels, while the insertion of copper(II) contributes to a reduction in the band gap energy. This work demonstrates that the careful selection of the oxidant agent in oCVD enables fine-tuning the optoelectronic properties of conjugated polymers to suit specific application requirements. Trifluoromethanesulfonate ; Conjugated system ; Polymer ; Chemistry ; Organic chemistry ; Polymer chemistry ; Inorganic chemistry ; Catalysis Conducting polymers and applications ; Organic Electronics and Photovoltaics ; Luminescence and Fluorescent Materials
Authors: Adem Dahi | Arnaud Rogemont | Yoann Brûlé | Christophe Labbez | Rémi Chassagnon | Aurélien Coillet | Erik Dujardin | Julien Boudon | Benoît Cluzel
Source: The Journal of Physical Chemistry C (article, 2024-02-08)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Gold Nanorod Growth and Etching Activated by Femtosecond Irradiation and Surface Plasmon Resonance Metal nanoparticles (NPs) colloids provide a unique combination of optical, magnetic, electronic, and thermal properties, finding applications in various fields ranging from optoelectronics to cancer therapy. The chemical synthesis of such NPs has been refined to a high degree of control of crystallinity, shape, and size distribution. Among them, gold NPs are of particular interest because they host plasmonic resonances that enhance their interactions with light. Their size and shape impose the resonance wavelengths, which, depending on the application, must be tunable. For this, the synthesis processes are generally adapted on a case-by-case basis, preventing the development of a generic recipe that can cover a wide range of applications. We present here a different approach and propose to modify the size distribution of postsynthesis NPs by laser irradiation in the presence of a gold salt to tune their resonance wavelengths. Plasmonic resonances driven by femtosecond laser irradiation are used to tune the redox activity of AuCl4– ions in the presence of gold nanorods, which leads to a reshaping of NPs. All chemical intermediates and products are monitored by in situ UV–visible spectroscopy and ex situ electron microscopy analysis and then compared to 3D simulations in order to unveil the underlying photochemical processes. As such, these results not only pave the way for the fine-tuning of the plasmon resonance of gold colloids over a wide spectral range, which can have an impact on many application areas such as plasmonic colors, sensors, or absorbers but also feed into the very active field of plasmonic photocatalysis. Plasmon ; Nanorod ; Surface plasmon resonance ; Materials science ; Colloidal gold ; Femtosecond ; Nanotechnology ; Nanoparticle ; Resonance (particle physics) ; Isotropic etching ; Laser ; Optoelectronics ; Etching (microfabrication) ; Optics ; Layer (electronics) ; Physics Gold and Silver Nanoparticles Synthesis and Applications ; Laser-Ablation Synthesis of Nanoparticles ; Nanocluster Synthesis and Applications
Authors: Zheng Wang | Junjie Pan | Xin‐Qi Chen | Mengyang Li | Meng‐Yang Li | Shi‐Cheng Wang
Source: Chemistry - A European Journal (article, 2024-08-24)
Field: Materials Science — Materials Chemistry

Facile Synthesis of Ln‐Doped Hydrogen‐Bonded Organic Frameworks with Rare‐Earth‐Characteristic Long Persistent Luminescence Tunable luminescence-assisted information storage and encryption holds increasing significance in today's society. A promising approach to incorporating the benefits of both organic long persistent luminescent (LPL) materials and rare-earth (RE) luminescence lies in utilizing organic host materials to sensitize RE luminescence, as well as employing Förster resonance energy transfer from hydrogen-bonded organic framework (HOF) phosphorescence to RE compound luminescence. This work introduces a one-pot, in situ pyrolytic condensation method, achieved through high-temperature melting calcination, to synthesize lanthanide ion-doped HOF materials. This method circumvents the drawback of molecular triplet energy annihilation, enabling the creation of organic LPL materials with RE characteristics. The HOF material serves as the host, exhibiting blue phosphorescence and cyan LPL. By fine-tuning the doping amount, the composite material U-Tb-100 achieves green LPL with a luminescent quantum yield of 56.4 %, and an LPL duration of approximately 2-3 s, demonstrating tunable persistence. Single-crystal X-ray diffraction, spectral analysis, and theoretical calculation unveil that U-Tb-100 exhibits exceptional quantum yield and long-lived luminescence primarily due to the efficient sensitization of U monomer to RE ions and the PRET process between U and RE complexes. This ingenious strategy not only expands the repertoire of HOF materials but also facilitates the design of multifunctional LPL materials. Luminescence ; Phosphorescence ; Materials science ; Persistent luminescence ; Quantum yield ; Doping ; Photochemistry ; Optoelectronics ; Chemistry ; Optics Lanthanide and Transition Metal Complexes ; Metal-Organic Frameworks: Synthesis and Applications ; Luminescence Properties of Advanced Materials