jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Ai‐Xin Zhu | Qing‐Yuan Yang | Soumya Mukherjee | Amrit Kumar | Chenghua Deng | Andrey A. Bezrukov | Mohana Shivanna | Michael J. Zaworotko
Source: Angewandte Chemie International Edition (article, 2019-10-07)
Field: Chemistry — Inorganic Chemistry

Tuning the Gate‐Opening Pressure in a Switching pcu Coordination Network, X‐pcu‐5‐Zn, by Pillar‐Ligand Substitution Coordination networks that reversibly switch between closed and open phases are of topical interest since their stepped isotherms can offer higher working capacities for gas-storage applications than the related rigid porous coordination networks. To be of practical utility, the pressures at which switching occurs, the gate-opening and gate-closing pressures, must lie between the storage and delivery pressures. Here we study the effect of linker substitution to fine-tune gate-opening and gate-closing pressure. Specifically, three variants of a previously reported pcu-topology MOF, X-pcu-5-Zn, have been prepared: X-pcu-6-Zn, 6=1,2-bis(4-pyridyl)ethane (bpe), X-pcu-7-Zn, 7=1,2-bis(4-pyridyl)acetylene (bpa), and X-pcu-8-Zn, 8=4,4'-azopyridine (apy). Each exhibited switching isotherms but at different gate-opening pressures. The N<sub>2</sub> , CO<sub>2</sub> , C<sub>2</sub> H<sub>2</sub> , and C<sub>2</sub> H<sub>4</sub> adsorption isotherms consistently indicated that the most flexible dipyridyl organic linker, 6, afforded lower gate-opening and gate-closing pressures. This simple design principle enables a rational control of the switching behavior in adsorbent materials. Linker ; Acetylene ; Substitution (logic) ; Topology (electrical circuits) ; Pillar ; Materials science ; Closing (real estate) ; Adsorption ; Chemistry ; Nanotechnology ; Computer science ; Electrical engineering ; Organic chemistry ; Mechanical engineering ; Engineering Metal-Organic Frameworks: Synthesis and Applications ; Crystallography and molecular interactions ; Supramolecular Chemistry and Complexes
Authors: Ιoannis Choinopoulos
Source: Polymers (review, 2019-02-11)
Field: Chemistry — Organic Chemistry

Grubbs’ and Schrock’s Catalysts, Ring Opening Metathesis Polymerization and Molecular Brushes—Synthesis, Characterization, Properties and Applications In this review, molecular brushes and other macromolecular architectures bearing a bottlebrush segment where the main chain is synthesized by ring opening metathesis polymerization (ROMP) mediated by Mo or Ru metal complexes are considered. A brief review of metathesis and ROMP is presented in order to understand the problems and the solutions provided through the years. The synthetic strategies towards bottlebrush copolymers are demonstrated and each one discussed separately. The initiators/catalysts for the synthesis of the backbone with ROMP are discussed. Syntheses of molecular brushes are presented. The most interesting properties of the bottlebrushes are detailed. Finally, the applications studied by different groups are presented. ROMP ; Metathesis ; Polymerization ; Ring-opening metathesis polymerisation ; Copolymer ; Ring-opening polymerization ; Materials science ; Polymer chemistry ; Catalysis ; Macromolecule ; Polymer science ; Chemistry ; Organic chemistry ; Polymer ; Composite material Synthetic Organic Chemistry Methods ; Advanced Polymer Synthesis and Characterization ; Polymer Surface Interaction Studies
Authors: Igor V. Alabugin | Edgar González-Rodríguez | Rahul Kisan Kawade | А. А. Степанов | Sergei F. Vasilevsky
Source: Molecules (review, 2019-03-15)
Field: Chemistry — Organic Chemistry

Alkynes as Synthetic Equivalents of Ketones and Aldehydes: A Hidden Entry into Carbonyl Chemistry The high energy packed in alkyne functional group makes alkyne reactions highly thermodynamically favorable and generally irreversible. Furthermore, the presence of two orthogonal π-bonds that can be manipulated separately enables flexible synthetic cascades stemming from alkynes. Behind these "obvious" traits, there are other more subtle, often concealed aspects of this functional group's appeal. This review is focused on yet another interesting but underappreciated alkyne feature: the fact that the CC alkyne unit has the same oxidation state as the -CH2C(O)- unit of a typical carbonyl compound. Thus, "classic carbonyl chemistry" can be accessed through alkynes, and new transformations can be engineered by unmasking the hidden carbonyl nature of alkynes. The goal of this review is to illustrate the advantages of using alkynes as an entry point to carbonyl reactions while highlighting reports from the literature where, sometimes without full appreciation, the concept of using alkynes as a hidden entry into carbonyl chemistry has been applied. Chemistry ; Equivalent ; Aldehyde ; Ketone ; Organic chemistry ; Combinatorial chemistry ; Biochemistry ; Catalysis Catalytic Alkyne Reactions ; Catalytic C–H Functionalization Methods ; Cyclopropane Reaction Mechanisms
Authors: Maximilian Bremerich | Christian Conrads | Tim Langletz | Carsten Bolm
Source: Angewandte Chemie International Edition (article, 2019-10-14)
Field: Chemistry — Organic Chemistry

Additions to <i>N</i>‐Sulfinylamines as an Approach for the Metal‐free Synthesis of Sulfonimidamides: <i>O</i>‐Benzotriazolyl Sulfonimidates as Activated Intermediates Sulfonimidamides are obtained in moderate to very good yields from the key intermediates O-benzotriazolyl sulfonimidates, which are formed by reacting aryldiazonium tetrafluoroborates, N-tritylsulfinylamine, and N-hydroxybenzotriazole hydrate in a process mediated by a tertiary amine. The formation of the sulfonimidate proceeds in inexpensive and environmentally benign dimethyl carbonate as the solvent, it does not require anhydrous conditions, and the product yields generally exceed 70 %. The substrate scope is broad, and a wide range of sensitive organic functionalities is well tolerated. The reactions probably proceed via aryl radicals formed from diazonium cations with assistance from both the tertiary amine and the sulfinylamine. Anhydrous ; Chemistry ; Amine gas treating ; Radical ; Solvent ; Metal ; Carbonate ; Substrate (aquarium) ; Aryl ; Hydrate ; Tertiary amine ; Combinatorial chemistry ; Polymer chemistry ; Medicinal chemistry ; Organic chemistry Synthesis and Catalytic Reactions ; Sulfur-Based Synthesis Techniques ; Catalytic C–H Functionalization Methods
Authors: Abel M. Maharramov | Ulviyya Hasanova | I. A. Suleymanova | G. E. Osmanova | Nazile Hajiyeva
Source: SN Applied Sciences (article, 2019-10-10)
Field: Materials Science — Materials Chemistry

The engineered nanoparticles in food chain: potential toxicity and effects Food chain ; Organism ; Nanotechnology ; Biochemical engineering ; Nanoparticle ; Risk analysis (engineering) ; Computer science ; Business ; Materials science ; Ecology ; Engineering ; Biology Nanoparticles: synthesis and applications ; Microplastics and Plastic Pollution ; Graphene and Nanomaterials Applications
Authors: Nick Gerrits | Kh. Shakouri | Jörg Behler | Geert–Jan Kroes
Source: The Journal of Physical Chemistry Letters (article, 2019-03-28)
Field: Materials Science — Materials Chemistry

Accurate Probabilities for Highly Activated Reaction of Polyatomic Molecules on Surfaces Using a High-Dimensional Neural Network Potential: CHD<sub>3</sub> + Cu(111) An accurate description of reactive scattering of molecules on metal surfaces often requires the modeling of energy transfer between the molecule and the surface phonons. Although ab initio molecular dynamics (AIMD) can describe this energy transfer, AIMD is at present untractable for reactions with reaction probabilities smaller than 1%. Here, we show that it is possible to use a neural network potential to describe a polyatomic molecule reacting on a mobile metal surface with considerably reduced computational effort compared to AIMD. The highly activated reaction of CHD<sub>3</sub> on Cu(111) is used as a test case for this method. It is observed that the reaction probability is influenced considerably by dynamical effects such as the bobsled effect and surface recoil. A special dynamical effect for CHD<sub>3</sub> + Cu(111) is that a higher vibrational efficacy is obtained for two quanta in the CH stretch mode than for a single quantum. Polyatomic ion ; Molecule ; Potential energy surface ; Ab initio ; Quantum ; Chemical physics ; Scattering ; Reaction dynamics ; Artificial neural network ; Phonon ; Energy transfer ; Chemistry ; Atomic physics ; Computational chemistry ; Materials science ; Physics ; Quantum mechanics ; Computer science ; Machine learning Machine Learning in Materials Science ; Quantum, superfluid, helium dynamics ; Advanced Chemical Physics Studies
Authors: Ya Zhuo | Shruti Hariyani | Edward Armijo | Zainab Abolade Lawson | Jakoah Brgoch
Source: ACS Applied Materials & Interfaces (article, 2019-12-20)
Field: Materials Science — Materials Chemistry

Evaluating Thermal Quenching Temperature in Eu<sup>3+</sup>-Substituted Oxide Phosphors via Machine Learning One of society's grand challenges is to reduce energy usage in ways that are cost-effective, sustainable, and environmentally benign. Replacing incandescent and compact fluorescent light bulbs with energy-efficient, solid-state white lighting is one of the easiest and most promising solutions. Eu<sup>3+</sup>-substituted inorganic oxide phosphors are one class of materials that can serve as the red component in these new light bulbs, allowing the creation of warm white light. Unfortunately, the emission intensity in most of these materials cannot be reliably maintained at elevated temperatures. There is therefore a need to discover entirely novel phosphor materials that are thermally robust; however, this is generally a prolonged and expensive process requiring extensive synthetic effort. In this work, we develop a machine-learning regression algorithm based on 134 experimentally measured temperature-dependent Eu<sup>3+</sup> emission data points to rapidly estimate the thermal quenching temperature (<i>T</i><sub>50</sub>), which is defined as the temperature when the emission intensity is half of the initial value. The <i>T</i><sub>50</sub> was then predicted for more than 1000 potential oxide Eu<sup>3+</sup> phosphor hosts using this model. Five compounds with predicted thermal quenching temperatures >423 K were subsequently selected and synthesized for validation of this approach. The phosphors, Sr<sub>2</sub>ScO<sub>3</sub>F, Cs<sub>2</sub>MgSi<sub>5</sub>O<sub>12</sub>, Ba<sub>2</sub>P<sub>2</sub>O<sub>7</sub>, LiBaB<sub>9</sub>O<sub>15</sub>, and Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub>, all exhibit good thermal stability when substituted with Eu<sup>3+</sup>, suggesting the success of our methodology. Phosphor ; Materials science ; Quenching (fluorescence) ; Oxide ; Emission intensity ; Incandescent light bulb ; Thermal ; Intensity (physics) ; Thermal stability ; Fluorescence ; Chemical engineering ; Analytical Chemistry (journal) ; Nuclear engineering ; Optoelectronics ; Luminescence ; Thermodynamics ; Optics ; Metallurgy ; Chemistry ; Organic chemistry ; Physics Luminescence Properties of Advanced Materials ; Perovskite Materials and Applications ; Advanced Photocatalysis Techniques
Authors: David Dubbeldam | Krista S. Walton | Thijs J. H. Vlugt | Sofı́a Calero
Source: Advanced Theory and Simulations (article, 2019-09-23)
Field: Chemistry — Inorganic Chemistry

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials Abstract Molecular simulations are an excellent tool to study adsorption and diffusion in nanoporous materials. Examples of nanoporous materials are zeolites, carbon nanotubes, clays, metal‐organic frameworks (MOFs), covalent organic frameworks (COFs) and zeolitic imidazolate frameworks (ZIFs). The molecular confinement these materials offer has been exploited in adsorption and catalysis for almost 50 years. Molecular simulations have provided understanding of the underlying shape selectivity, and adsorption and diffusion effects. Much of the reliability of the modeling predictions depends on the accuracy and transferability of the force field. However, flexibility and the chemical and structural diversity of MOFs add significant challenges for engineering force fields that are able to reproduce experimentally observed structural and dynamic properties. Recent developments in design, parameterization, and implementation of force fields for MOFs and zeolites are reviewed. Nanoporous ; Adsorption ; Zeolitic imidazolate framework ; Molecular dynamics ; Force field (fiction) ; Materials science ; Nanotechnology ; Flexibility (engineering) ; Transferability ; Diffusion ; Metal-organic framework ; Chemical physics ; Computational chemistry ; Chemistry ; Computer science ; Physical chemistry ; Thermodynamics ; Physics Metal-Organic Frameworks: Synthesis and Applications ; Machine Learning in Materials Science ; Dendrimers and Hyperbranched Polymers
Authors: Sourangsu Banerji | Berardi Sensale‐Rodriguez
Source: Scientific Reports (article, 2019-04-09)
Field: Materials Science — Electronic, Optical and Magnetic Materials

A Computational Design Framework for Efficient, Fabrication Error-Tolerant, Planar THz Diffractive Optical Elements We demonstrate ultra-thin (1.5-3λ<sub>0</sub>), fabrication-error tolerant efficient diffractive terahertz (THz) optical elements designed using a computer-aided optimization-based search algorithm. The basic operation of these components is modeled using scalar diffraction of electromagnetic waves through a pixelated multi-level 3D-printed polymer structure. Through the proposed design framework, we demonstrate the design of various ultrathin planar THz optical elements, namely (i) a high Numerical Aperture (N.A.), broadband aberration rectified spherical lens (0.1 THz-0.3 THz), (ii) a spectral splitter (0.3 THz-0.6 THz) and (iii) an on-axis broadband transmissive hologram (0.3 THz-0.5 THz). Such an all-dielectric computational design-based approach is advantageous against metallic or dielectric metasurfaces from the perspective that it incorporates all the inherent structural advantages associated with a scalar diffraction based approach, such as (i) ease of modeling, (ii) substrate-less facile manufacturing, (iii) planar geometry, (iv) high efficiency along with (v) broadband operation, (vi) area scalability and (vii) fabrication error-tolerance. With scalability and error tolerance being two major bottlenecks of previous design strategies. This work is therefore, a significant step towards the design of THz optical elements by bridging the gap between structural and computational design i.e. through a hybrid design-based approach enabling considerably less computational resources than the previous state of the art. Furthermore, the approach used herein can be expanded to a myriad of optical elements at any wavelength regime. Terahertz radiation ; Fabrication ; Computer science ; Optoelectronics ; Optics ; Planar ; Materials science ; Scalability ; Diffraction ; Broadband ; Diffraction efficiency ; Grating ; Physics Metamaterials and Metasurfaces Applications ; Terahertz technology and applications ; Microwave Engineering and Waveguides
Authors: Jianwei Su | Kailang Liu | Fakun Wang | Bao Jin | Yabin Guo | Guiheng Liu | Huiqiao Li | Tianyou Zhai
Source: Advanced Materials Interfaces (article, 2019-08-09)
Field: Materials Science — Materials Chemistry

Van der Waals 2D Transition Metal Tellurides Abstract As important members of transition metal chalcogenides (TMCs), transition metal tellurides (TMTs) have drawn much attention for their various crystal structures with various physical properties. These various structures and structural transitions between them not only are fascinating in the fundamental studies, but also provide unprecedented opportunities in novel device design and applications. In this review, the recent developments in the area of TMTs are outlined. First, the unique crystal and electronic structures of TMTs are introduced. Then the TMTs preparation strategies, including novel exfoliation technique and chemical vapor deposition (CVD), are reviewed. Moreover, the distinctive physical properties of TMTs such as phase transition, intrinsic ferromagnetism, and superconductivity are summarized. Additionally, an overview of device applications in the electronics and optoelectronics field is provided. The prospect for the research of TMTs is presented at the end. Materials science ; van der Waals force ; Transition metal ; Chemical vapor deposition ; Nanotechnology ; Physics ; Chemistry ; Quantum mechanics ; Molecule ; Organic chemistry 2D Materials and Applications ; Perovskite Materials and Applications ; Chalcogenide Semiconductor Thin Films
Authors: Alemayehu Kidanemariam | Jiwon Lee | Juhyun Park
Source: Polymers (review, 2019-12-13)
Field: Chemistry — Inorganic Chemistry

Recent Innovation of Metal-Organic Frameworks for Carbon Dioxide Photocatalytic Reduction The accumulation of carbon dioxide (CO<sub>2</sub>) pollutants in the atmosphere begets global warming, forcing us to face tangible catastrophes worldwide. Environmental affability, affordability, and efficient CO<sub>2</sub> metamorphotic capacity are critical factors for photocatalysts; metal-organic frameworks (MOFs) are one of the best candidates. MOFs, as hybrid organic ligand and inorganic nodal metal with tailorable morphological texture and adaptable electronic structure, are contemporary artificial photocatalysts. The semiconducting nature and porous topology of MOFs, respectively, assists with photogenerated multi-exciton injection and adsorption of substrate proximate to void cavities, thereby converting CO<sub>2</sub>. The vitality of the employment of MOFs in CO<sub>2</sub> photolytic reaction has emerged from the fact that they are not only an inherently eco-friendly weapon for pollutant extermination, but also a potential tool for alleviating foreseeable fuel crises. The excellent synergistic interaction between the central metal and organic linker allows decisive implementation for the design, integration, and application of the catalytic bundle. In this review, we presented recent MOF headway focusing on reports of the last three years, exhaustively categorized based on central metal-type, and novel discussion, from material preparation to photocatalytic, simulated performance recordings of respective as-synthesized materials. The selective CO<sub>2</sub> reduction capacities into syngas or formate of standalone or composite MOFs with definite photocatalytic reaction conditions was considered and compared. Metal-organic framework ; Photocatalysis ; Materials science ; Formate ; Adsorption ; Syngas ; Nanotechnology ; Catalysis ; Chemical engineering ; Chemistry ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; Advanced Photocatalysis Techniques ; Covalent Organic Framework Applications
Authors: Tao Jiang | Xi Wang | Jie Wang | Guoping Hu | Xiang Ma
Source: ACS Applied Materials & Interfaces (article, 2019-03-27)
Field: Chemistry — Organic Chemistry

Humidity- and Temperature-Tunable Multicolor Luminescence of Cucurbit[8]uril-Based Supramolecular Assembly Fabrication of tunable luminescent materials by a single luminophore is a challenge owning to the limit of emissive properties of monofluorophores. Herein, a type of temperature and humidity dual-responsive luminescent material based on host-guest supramolecular self-assembly was developed. Included into the cavity of cucurbit[8]uril (CB[8]) to form a 1:2 host-guest binding motif, the highly blue-emissive thiazolothiazole methyl-viologen (TMV) molecules were promoted to stack closely with a sharp luminescence decrease at 460 nm and rise of the dimer emission at 535 nm, especially at high concentrations in aqueous solution, which was demonstrated by fluorescence spectra, UV-vis absorbance spectra, NMR, and ITC data. Accordingly, when printed on paper, the 1/2 CB[8]/TMV complex presented a reversibly humidity-dependent emissive behavior with luminescent color changing from greenish-yellow in wet to blue upon evaporation. Besides, the sensitivity of the host-guest interaction endowed the CB[8]/TMV complexes with temperature-tunable emission which showed a considerably enhanced blue luminescence at higher temperature. Subsequently, a ratiometric temperature-responsive emitter which luminesced reversibly from pink to white and then to blue light at temperature ranging from 0 to 70 °C was fabricated by mixing the CB[8]/TMV complex with thermal-sensitized emitting GSH-Au nanoclusters. These fine-tuning abilities make the CB[8]/TMV supramolecular complex applicable in visual luminescent devices such as anti-counterfeiting labels and fluorescent thermometers. Materials science ; Luminescence ; Humidity ; Supramolecular chemistry ; Nanotechnology ; Supramolecular assembly ; Optoelectronics ; Crystallography ; Thermodynamics ; Crystal structure Supramolecular Chemistry and Complexes ; Luminescence and Fluorescent Materials ; Molecular Sensors and Ion Detection
Authors: Christian Schneider | David Bodesheim | Michael G. Ehrenreich | Valentina Crocellà | J. Mink | Roland A. Fischer | Keith T. Butler | Gregor Kieslich
Source: Journal of the American Chemical Society (article, 2019-06-11)
Field: Materials Science — Materials Chemistry

Tuning the Negative Thermal Expansion Behavior of the Metal–Organic Framework Cu<sub>3</sub>BTC<sub>2</sub> by Retrofitting The modular building principle of metal-organic frameworks (MOFs) presents an excellent platform to explore and establish structure-property relations that tie microscopic to macroscopic properties. Negative thermal expansion (NTE) is a common phenomenon in MOFs and is often ascribed to collective motions that can move through the structure at sufficiently low energies. Here, we show that the introduction of additional linkages in a parent framework, retrofitting, is an effective approach to access lattice dynamics experimentally, in turn providing researchers with a tool to alter the NTE behavior in MOFs. By introducing TCNQ (7,7,8,8-tetracyanoquinodimethane) into the prototypical MOF Cu<sub>3</sub>BTC<sub>2</sub> (BTC = 1,3,5-benzenetricarboxylate; HKUST-1), NTE can be tuned between α<sub>V</sub> = -15.3 × 10<sup>-6</sup> K<sup>-1</sup> (Cu<sub>3</sub>BTC<sub>2</sub>) and α<sub>V</sub> = -8.4 × 10<sup>-6</sup> K<sup>-1</sup> (1.0TCNQ@Cu<sub>3</sub>BTC<sub>2</sub>). We ascribe this phenomenon to a general stiffening of the framework as a function of TCNQ loading due to additional network connectivity, which is confirmed by computational modeling and far-infrared spectroscopy. Our findings imply that retrofitting is generally applicable to MOFs with open metal sites, opening yet another way to fine-tune properties in this versatile class of materials. Chemistry ; Retrofitting ; Metal-organic framework ; Thermal ; Thermal expansion ; Chemical engineering ; Inorganic chemistry ; Physical chemistry ; Thermodynamics ; Structural engineering Thermal Expansion and Ionic Conductivity ; Advanced Battery Materials and Technologies ; Magnetic and transport properties of perovskites and related materials