jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Niranjan Sitapure | Robert W. Epps | Milad Abolhasani | Joseph Sang‐Il Kwon
Source: Industrial & Engineering Chemistry Research (article, 2021-03-26)
Field: Materials Science — Materials Chemistry

CFD-Based Computational Studies of Quantum Dot Size Control in Slug Flow Crystallizers: Handling Slug-to-Slug Variation Recently, slug-flow crystallizers (SFCs) have been proposed for continuous manufacturing of colloidal quantum dots (QDs). Despite the intriguing advantages of SFCs for controlled manufacturing of QDs, it has been difficult to account for the wide crystal size distribution (CSD) caused by slug-to-slug (S2S) variation, and the absence of a modeling and control framework made it challenging to fine-tune the QD size distribution. In response, we developed a computational fluid dynamics (CFD) model to simulate the S2S variation in SFCs. The results from the CFD model were integrated with a slug crystallizer model, which can describe the effect of S2S heterogeneity on crystallization of QDs in SFCs. Specifically, the slug crystallizer model was constructed by combining a continuum model with a kinetic Monte Carlo model. Based on the proposed CFD-based multiscale model, an optimal operation problem was formulated to ensure a good set-point (QD size) tracking performance and a narrow CSD. Computational fluid dynamics ; Slug ; Slug flow ; Monte Carlo method ; Flow (mathematics) ; Computer science ; Materials science ; Simulation ; Mechanics ; Physics ; Two-phase flow ; Mathematics ; Geology Quantum Dots Synthesis And Properties ; Perovskite Materials and Applications ; Machine Learning and ELM
Authors: Adam J. Dannenhoffer | Hiroaki Sai | Boris Harutyunyan | Ashwin Narayanan | Natalia E. Powers‐Riggs | Alexandra N. Edelbrock | James Passarelli | Steven J. Weigand | Michael R. Wasielewski | Michael J. Bedzyk | Liam C. Palmer | Samuel I. Stupp
Source: Nano Letters (article, 2021-04-20)
Field: Materials Science — Biomaterials

Growth of Extra-Large Chromophore Supramolecular Polymers for Enhanced Hydrogen Production The control of morphology in bioinspired chromophore assemblies is key to the rational design of functional materials for light harvesting. We investigate here morphological changes in perylene monoimide chromophore assemblies during thermal annealing in aqueous environments of high ionic strength to screen electrostatic repulsion. We found that annealing under these conditions leads to the growth of extra-large ribbon-shaped crystalline supramolecular polymers of widths from about 100 nm to several micrometers and lengths from 1 to 10 μm while still maintaining a unimolecular thickness. This growth process was monitored by variable-temperature absorbance spectroscopy, synchrotron X-ray scattering, and confocal microscopy. The extra-large single-crystal-like supramolecular polymers are highly porogenic, thus creating loosely packed hydrogel scaffolds that showed greatly enhanced photocatalytic hydrogen production with turnover numbers as high as 13 500 over ∼110 h compared to 7500 when smaller polymers are used. Our results indicate great functional opportunities in thermally and pathway-controlled supramolecular polymerization. Supramolecular chemistry ; Chromophore ; Supramolecular polymers ; Polymer ; Materials science ; Supramolecular assembly ; Chemical engineering ; Perylene ; Annealing (glass) ; Polymerization ; Nanotechnology ; Crystallography ; Photochemistry ; Chemistry ; Crystal structure ; Organic chemistry ; Molecule ; Composite material Supramolecular Self-Assembly in Materials ; Polydiacetylene-based materials and applications ; Porphyrin and Phthalocyanine Chemistry
Authors: J. Narciso | Enrique V. Ramos–Fernández | José J. Delgado‐Marín | Christopher W. Affolter | Unni Olsbye | E. Redekop
Source: Microporous and Mesoporous Materials (article, 2021-07-20)
Field: Chemistry — Inorganic Chemistry

New route for the synthesis of Co-MOF from metal substrates Metal ; Metal-organic framework ; Deprotonation ; Cobalt ; Chemistry ; Redox ; Inorganic chemistry ; Ligand (biochemistry) ; Etching (microfabrication) ; Alloy ; Chemical engineering ; Materials science ; Organic chemistry ; Adsorption Metal-Organic Frameworks: Synthesis and Applications
Authors: Tommaso Fantoni | Alessandra Tolomelli | Walter Cabri
Source: Catalysis Today (article, 2021-09-17)
Field: Chemistry — Organic Chemistry

A translation of the twelve principles of green chemistry to guide the development of cross-coupling reactions Chemistry ; Green chemistry ; Translation (biology) ; Organometallic chemistry ; Coupling reaction ; Combinatorial chemistry ; Biochemical engineering ; Nanotechnology ; Catalysis ; Aniline ; Organic chemistry ; Reaction mechanism ; Engineering ; Biochemistry ; Materials science Nanomaterials for catalytic reactions ; Chemistry and Chemical Engineering ; Innovative Microfluidic and Catalytic Techniques Innovation
Authors: Salvio Suárez–García | Tullio Esposito | Jenna Neufeld-Peters | Marta Bergamo | Hua Yang | Katayoun Saatchi | Paul Schaffer | Urs O. Häfeli | Daniel Ruiz‐Molina | Cristina Rodríguez‐Rodríguez | Fernando Novio
Source: ACS Applied Materials & Interfaces (article, 2021-02-26)
Field: Materials Science — Surfaces, Coatings and Films

Hybrid Metal–Phenol Nanoparticles with Polydopamine-like Coating for PET/SPECT/CT Imaging The validation of metal-phenolic nanoparticles (MPNs) in preclinical imaging studies represents a growing field of interest due to their versatility in forming predesigned structures with unique properties. Before MPNs can be used in medicine, their pharmacokinetics must be optimized so that accumulation in nontargeted organs is prevented and toxicity is minimized. Here, we report the fabrication of MPNs made of a coordination polymer core that combines In(III), Cu(II), and a mixture of the imidazole 1,4-bis(imidazole-1-ylmethyl)-benzene and the catechol 3,4-dihydroxycinnamic acid ligands. Furthermore, a phenolic-based coating was used as an anchoring platform to attach poly(ethylene glycol) (PEG). The resulting MPNs, with effective hydrodynamic diameters of around 120 nm, could be further derivatized with surface-embedded molecules, such as folic acid, to facilitate <i>in vivo</i> targeting and multifunctionality. The prepared MPNs were evaluated for <i>in vitro</i> plasma stability, cytotoxicity, and cell internalization and found to be biocompatible under physiological conditions. First, biomedical evaluations were then performed by intrinsically incorporating trace amounts of the radioactive metals <sup>111</sup>In or <sup>64</sup>Cu during the MPN synthesis directly into their polymeric matrix. The resulting particles, which had identical physicochemical properties to their nonradioactive counterparts, were used to perform <i>in vivo</i> single-photon emission computed tomography (SPECT) and positron emission tomography (PET) in tumor-bearing mice. The ability to incorporate multiple metals and radiometals into MPNs illustrates the diverse range of functional nanoparticles that can be prepared with this approach and broadens the scope of these nanoconstructs as multimodal preclinical imaging agents. Materials science ; Nanoparticle ; Coating ; Metal ; Phenol ; Nanotechnology ; Nuclear chemistry ; Metallurgy ; Organic chemistry Polymer Surface Interaction Studies ; Dendrimers and Hyperbranched Polymers ; Nanoparticle-Based Drug Delivery
Authors: Damian Jędrzejowski | Marzena Pander | Wojciech Nitek | Wojciech Bury | Dariusz Matoga
Source: Chemistry of Materials (article, 2021-09-07)
Field: Chemistry — Inorganic Chemistry

Turning Flexibility into Rigidity: Stepwise Locking of Interpenetrating Networks in a MOF Crystal through Click Reaction Post-synthetic modifications of metal-organic frameworks (MOFs) enable synthesis of materials with enhanced performance characteristics or those inaccessible by direct synthetic routes.In this work, for the first time, we utilize inverse-electron demand Diels-Alder (iEDDA) modification to control the structural flexibility and porosity of an open framework material.We selected a series of dienophiles with increasing bulkiness including ethyl vinyl ether (eve), cyclohexene (chx), norbornene (nor), and 5norbornene-2-methanol (noh) to modify a tetrazine-based linker (3,6-dipyridyl-1,2,4,5tetrazine, dpt) incorporated in a unique doubly interpenetrated 3D hybrid MOF-HOF porous material (HOF, hydrogen-bonded organic framework), {[Cd 2 (coh) 2 (dpt) 2 ] guests} n (JUK-20).Each subnetwork in JUK-20 is built of 2D coordination layers stacked by strong complementary CO H-N hydrogen bonds between carbohydrazide dibenzoate linkers (coh).By using the [4 + 2] click reactions of JUK-20, which proceed in a prominent single-crystal-to-single-crystal manner, we obtained a series of JUK-20-dienophile MOFs.The modifications lead to a stepwise decrease in structural flexibility of the JUK-20 platform until the highest rigidity and stability is reached for JUK-20-noh.Consequently, the adsorption capacity in the JUK-20-dienophile series increases, as revealed collectively by single-crystal X-ray diffraction, physisorption isotherms (N 2 , CO 2 , and MeOH), and grand canonical Monte Carlo simulations.Our work demonstrates that post-synthetic iEDDA modification is a versatile and efficient tool for systematic functionalization of open framework materials under mild conditions. Norbornene ; Tetrazine ; Materials science ; Crystal engineering ; Single crystal ; Crystallography ; Crystal structure ; Chemistry ; Polymer chemistry ; Supramolecular chemistry ; Organic chemistry ; Composite material ; Polymer ; Polymerization Metal-Organic Frameworks: Synthesis and Applications ; Covalent Organic Framework Applications ; Nanoplatforms for cancer theranostics
Authors: Pol Sallés | Iván Caño | Roger Guzmán | Camilla Dore | Agustín Mihi | Wu Zhou | Mariona Coll
Source: Advanced Materials Interfaces (article, 2021-01-14)
Field: Materials Science — Materials Chemistry

Facile Chemical Route to Prepare Water Soluble Epitaxial Sr<sub>3</sub>Al<sub>2</sub>O<sub>6</sub> Sacrificial Layers for Free‐Standing Oxides Abstract The growth of epitaxial complex oxides has been essentially limited to specific substrates that can induce epitaxial growth and stand high temperature thermal treatments. These restrictions hinder the opportunity to manipulate and integrate such materials into new artificial heterostructures including the use of polymeric and silicon substrates and study emergent phenomena for novel applications. To tackle this bottleneck, herein, a facile chemical route to prepare water‐soluble epitaxial Sr 3 Al 2 O 6 thin films to be used as sacrificial layer for future free‐standing epitaxial complex oxide manipulation is described. Two solution processes are put forward based on metal nitrate and metalorganic precursors to prepare dense, homogeneous and epitaxial Sr 3 Al 2 O 6 thin films that can be easily etched by milli‐Q water. Moreover, as a proof of concept, a basic heterostructure consisting of Al 2 O 3 /Sr 3 Al 2 O 6 on SrTiO 3 is fabricated to subsequently exfoliate the Al 2 O 3 thin film and transfer it to a polymer substrate. This is a robust chemical and low‐cost methodology that could be adopted to prepare a wide variety of thin films to fabricate artificial heterostructures to go beyond the traditional electronic, spintronic, and energy storage and conversion devices. Materials science ; Epitaxy ; Heterojunction ; Thin film ; Substrate (aquarium) ; Nanotechnology ; Oxide ; Chemical engineering ; Layer (electronics) ; Optoelectronics ; Metallurgy Ferroelectric and Piezoelectric Materials ; Electronic and Structural Properties of Oxides ; Microwave Dielectric Ceramics Synthesis
Authors: Anna Fortunato | Miriam Mba
Source: Gels (article, 2021-07-07)
Field: Materials Science — Biomaterials

Metal Cation Triggered Peptide Hydrogels and Their Application in Food Freshness Monitoring and Dye Adsorption Metal-ligand interactions have emerged as an important tool to trigger and modulate self-assembly, and to tune the properties of the final supramolecular materials. Herein, we report the metal-cation induced self-assembly of a pyrene-peptide conjugate to form hydrogels. The peptide has been rationally designed to favor the formation of β-sheet 1D assemblies and metal coordination through the Glu side chains. We studied in detail the self-assembly process in the presence of H<sup>+</sup>, Li<sup>+</sup>, Na<sup>+</sup>, K<sup>+</sup>, Ca<sup>2+</sup>, Ni<sup>2+</sup>, Cu<sup>2+</sup>, Zn<sup>2+</sup>, Cd<sup>2+</sup>, Co<sup>2+</sup>, Fe<sup>3+</sup>, and Cr<sup>3+</sup> and found that the morphology and mechanical properties of the hydrogels are ion-dependent. Moreover, thanks to the presence of the metal, new applications could be explored. Cu<sup>2+</sup> metallogels could be used for amine sensing and meat freshness monitoring, while Zn<sup>2+</sup> metallogels showed good selectivity for cationic dye adsorption and separation. Self-healing hydrogels ; Adsorption ; Peptide ; Metal ; Chemical engineering ; Chemistry ; Materials science ; Nanotechnology ; Polymer chemistry ; Organic chemistry ; Biochemistry Supramolecular Self-Assembly in Materials ; Polydiacetylene-based materials and applications ; Advanced biosensing and bioanalysis techniques
Authors: Sovan Biswas | Ben F. Van Steijvoort | Marjo Waeterschoot | Narendraprasad Reddy Bheemireddy | Gwilherm Evano | Bert U. W. Maes
Source: Angewandte Chemie International Edition (article, 2021-06-18)
Field: Chemistry — Organic Chemistry

Expedient Synthesis of Bridged Bicyclic Nitrogen Scaffolds via Orthogonal Tandem Catalysis Bridged nitrogen bicyclic skeletons have been accessed via unprecedented site- and diastereoselective orthogonal tandem catalysis from readily accessible reactants in a step economic manner. Directed Pd-catalyzed γ-C(sp<sup>3</sup> )-H olefination of aminocyclohexane with gem-dibromoalkenes, followed by a consecutive intramolecular Cu-catalyzed amidation of the 1-bromo-1-alkenylated product delivers the interesting normorphan skeleton. The tandem protocol can be applied on substituted aminocyclohexanes and aminoheterocycles, easily providing access to the corresponding substituted, aza- and oxa-analogues. The Cu catalyst of the Ullmann-Goldberg reaction additionally avoids off-cycle Pd catalyst scavenging by alkenylated reaction product. The picolinamide directing group stabilizes the enamine of the 7-alkylidenenormorphan, allowing further product post functionalizations. Without Cu catalyst, regio- and diastereoselective Pd-catalyzed γ-C(sp<sup>3</sup> )-H olefination is achieved. Catalysis ; Tandem ; Chemistry ; Intramolecular force ; Bicyclic molecule ; Combinatorial chemistry ; Enamine ; Stereochemistry ; Organic chemistry ; Materials science Catalytic C–H Functionalization Methods ; Synthesis and Catalytic Reactions ; Sulfur-Based Synthesis Techniques
Authors: Aitor Bermejo‐López | Sergio Carrasco | Pedro J. Tortajada | Kenji P. M. Kopf | Amparo Sanz‐Marco | Mathias S. Hvid | Nina Lock | Belén Martı́n-Matute
Source: ACS Sustainable Chemistry & Engineering (article, 2021-10-18)
Field: Chemistry — Organic Chemistry

Selective Synthesis of Imines by Photo-Oxidative Amine Cross-Condensation Catalyzed by PCN-222(Pd) Palladium-metalated PCN-222 enables the aerobic photo-oxidative cross-condensation of anilines with benzylic amines yielding a series of linear and cyclic imines. The reaction is very efficient under mild conditions, which allows the isolation of simple, yet elusive, intermediates such as 2-(benzylideneamino)aniline and 2-(benzylideneamino)phenols. Recyclability studies show excellent activity and selectivity after five runs. The methodology was successfully applied for the synthesis of an antitumor agent (PMX-610). Aniline ; Chemistry ; Palladium ; Amine gas treating ; Catalysis ; Selectivity ; Condensation ; Oxidative phosphorylation ; Phenols ; Combinatorial chemistry ; Condensation reaction ; Organic chemistry ; Photochemistry Catalytic C–H Functionalization Methods ; Synthesis and Biological Evaluation ; Click Chemistry and Applications
Authors: Magdalena Maciejewska | Anna Sowińska‐Baranowska
Source: Polymers (article, 2021-05-19)
Field: Materials Science — Polymers and Plastics

Influence of Fillers and Ionic Liquids on the Crosslinking and Performance of Natural Rubber Biocomposites This work concerns the effect of fillers and ionic liquids on the cure characteristics of natural rubber (NR) compounds, as well as the mechanical and thermal properties of the vulcanizates. Three types of white filler were applied, such as cellulose, nanosized silica and hydrotalcite, to modify the performance of NR composites. Additionally, ionic liquids (ILs) with bromide anion and different cations, i.e., 1-butyl-3-methylimidazolium (Bmi) and 1-butyl-3-methylpyrrolidinium (Bmpyr), were used to improve the cure characteristics of NR compounds and functional properties of the vulcanizates. The type of filler and the structure of ILs were proved to affect the rheometric properties and cure characteristics of NR compounds as well as the performance of the NR vulcanizates. Owing to the adsorption of curatives onto the surface, silica reduced the activity of the crosslinking system, prolonging the optimal vulcanization time of NR compounds and reducing the crosslinking degree of the elastomer. However, silica-filled NR exhibited the highest thermal stability. Hydrotalcite increased the crosslink density and, consequently, the mechanical properties of the vulcanizates, but deteriorated their thermal stability. ILs beneficially influenced the cure characteristics of NR compounds, as well as the crosslink density and mechanical performance of the vulcanizates, particularly those filled with silica. Cellulose did not significantly affect the vulcanization of NR compounds and crosslink density of the vulcanizates compared to the unfilled elastomer, but deteriorated their tensile strength. On the other hand, cellulose improved the thermal stability and did not considerably alter the damping properties of the vulcanizates. Vulcanization ; Materials science ; Thermal stability ; Ultimate tensile strength ; Elastomer ; Natural rubber ; Composite material ; Filler (materials) ; Hydrotalcite ; Ionic liquid ; Cellulose ; Chemical engineering ; Organic chemistry ; Chemistry Polymer Nanocomposites and Properties ; biodegradable polymer synthesis and properties ; Natural Fiber Reinforced Composites
Authors: Mikko K. Mäkelä | Evgeny Bulatov | Kiia Malinen | Juulia Talvitie | Martin Nieger | Michele Melchionna | Anna Lenarda | Tao Hu | Tom Wirtanen | Juho Helaja
Source: Advanced Synthesis & Catalysis (article, 2021-07-09)
Field: Chemistry — Organic Chemistry

Carbocatalytic Cascade Synthesis of Polysubstituted Quinolines from Aldehydes and 2‐Vinyl Anilines Abstract Oxidized active carbon (oAC) catalyses the formation of polysubstituted quinolines from o ‐vinyl anilines and aldehydes. The reaction proceeds in a cascade manner through condensation, electrocyclization and dehydrogenation, and gives access to a wide range of quinolines with alkyl and/or aryl substituents as demonstrated with 40 examples. The metal‐free catalytic procedure allows a heterogeneous protocol for the synthesis of various polysubstituted quinolines. The mechanistic studies imply that both the acid and quinoidic groups in oAC are integral for the catalytic manifold. magnified image Chemistry ; Dehydrogenation ; Catalysis ; Aryl ; Alkyl ; Cascade reaction ; Cascade ; Combinatorial chemistry ; Organic chemistry ; Condensation ; Brønsted–Lowry acid–base theory Catalytic C–H Functionalization Methods ; Catalytic Cross-Coupling Reactions ; Asymmetric Hydrogenation and Catalysis
Authors: Tao Zhang | Zhiyuan Liu | Yiqiang Sun | Dilong Liu | Cuncheng Li | Weiping Cai | Yue Li
Source: Chemical Science (article, 2021-01-01)
Field: Materials Science — Electronic, Optical and Magnetic Materials

A universal route with fine kinetic control to a family of penta-twinned gold nanocrystals Some of the major difficulties hindering the synthesis of different types of colloidal nanocrystals are their complex synthetic methods and the lack of a universal growth mechanism in one system. Herein, we propose a general strategy of kinetically controlled seed-mediated growth to synthesize a family of penta-twinned gold nanocrystals. Specifically, different kinds of penta-twinned nanocrystals (truncated penta-twinned decahedra, truncated bipyramids, bipyramids, truncated bipyramids with tips, star-like penta-twinned nanocrystals, decahedra with concave edges, and decahedra) with tunable sizes and high purity were readily achieved in one system solely by tailoring the deposition kinetics of adatoms on different sites of decahedral seeds. The controllable deposition kinetics can be realized by changing the ratio of reductant/gold precursors (<i>R</i>), which dictates whether horizontal or vertical features along the 5-fold axis direction of Au decahedral seeds are produced. Additionally, the selective growth of a second metal (silver) on penta-twinned gold seeds can be reached through minor modification of <i>R</i>, which opens a new avenue for mechanistic investigation by visualizing the seed localization within the final particles. The present work demonstrates a general paradigm for the kinetic growth of penta-twinned crystals and would be extended to the synthesis of other families of nanocrystals. Nanocrystal ; Materials science ; Deposition (geology) ; Nanotechnology ; Kinetics ; Kinetic energy ; Crystallography ; Metal ; Chemical physics ; Chemical engineering ; Chemistry ; Metallurgy ; Physics ; Geology Gold and Silver Nanoparticles Synthesis and Applications ; Quantum Dots Synthesis And Properties ; Nanocluster Synthesis and Applications
Authors: Norbert Koch
Source: Applied Physics Letters (article, 2021-12-27)
Field: Materials Science — Materials Chemistry

Opportunities for energy level tuning at inorganic/organic semiconductor interfaces The aim of this Perspective is to provide an overview of approaches that can be employed to tune the energy level alignment at interfaces between inorganic and organic semiconductors for use in electronic and optoelectronic devices. The approaches include tailoring intramolecular dipolar bond distribution, controlling molecular orientation at interfaces, and the insertion of a molecularly thin interlayer that abruptly shifts the electrostatic potential between the two semiconductors and, thus, affords level tuning. With these state of the art methods, the frontier energy levels at an inorganic/organic heterojunction can be varied up to ca. 3 eV, i.e., covering the energy gap of most semiconductors. By combining two or more of these approaches or by employing interfacial molecular switches, it is envisioned that unconventional and dynamically switchable interfacial energy level scenarios can be created, enabling expanded or superior device functionality. Semiconductor ; Heterojunction ; Organic semiconductor ; Materials science ; Optoelectronics ; Nanotechnology ; Dipole ; Intramolecular force ; Band gap ; Chemistry Quantum Dots Synthesis And Properties ; Molecular Junctions and Nanostructures ; Organic Electronics and Photovoltaics