jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Peng Hu | Jialang Hu | Hao Liu | Hao Wang | Jie Zhou | Rajamani Krishna | Hongbing Ji
Source: ACS Central Science (article, 2022-07-22)
Field: Chemistry — Inorganic Chemistry

Quasi-Orthogonal Configuration of Propylene within a Scalable Metal–Organic Framework Enables Its Purification from Quinary Propane Dehydrogenation Byproducts Propylene production via nonoxidative propane dehydrogenation (PDH) holds great promise in meeting growing global demand for propylene. Effective adsorptive purification of a low concentration of propylene from quinary PDH byproducts comprising methane (CH<sub>4</sub>), ethylene (C<sub>2</sub>H<sub>4</sub>), ethane (C<sub>2</sub>H<sub>6</sub>), propylene (C<sub>3</sub>H<sub>6</sub>), and propane (C<sub>3</sub>H<sub>8</sub>) has been an unsolved academic bottleneck. Herein, we now report an ultramicroporous zinc metal-organic framework (Zn-MOF, termed as <b>1</b>) underlying a rigid one-dimensional channel, enabling trace C<sub>3</sub>H<sub>6</sub> capture and effective separation from quinary PDH byproducts. Adsorption isotherms of <b>1</b> suggest a record-high C<sub>3</sub>H<sub>6</sub> uptake of 34.0/92.4 cm<sup>3</sup> cm<sup>-3</sup> (0.01/0.1 bar) at 298 K. In situ spectroscopies, crystallographic experiments, and modeling have jointly elucidated that the outstanding propylene uptakes at lower pressure are dominated by multiple binding interactions and swift diffusion behavior, yielding quasi-orthogonal configuration of propylene in adaptive channels. Breakthrough tests demonstrate that 30.8 L of propylene with a serviceable purity of 95.0-99.4% can be accomplished from equimolar C<sub>3</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>8</sub> mixtures for 1 kg of activated <b>1</b>. Such an excellent property is also validated by the breakthrough tests of quinary mixtures containing CH<sub>4</sub>/C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>8</sub> (3/5/6/42/44, v/v/v/v/v). Particularly, structurally stable <b>1</b> can be easily synthesized on the kilogram scale using cheap materials (only $167 for per kilogram of <b>1</b>), which is important in industrial applications. Quinary ; Dehydrogenation ; Propane ; Scalability ; Process engineering ; Chemistry ; Chemical engineering ; Computer science ; Organic chemistry ; Materials science ; Combinatorial chemistry ; Database ; Engineering ; Catalysis Metal-Organic Frameworks: Synthesis and Applications ; Polyoxometalates: Synthesis and Applications ; Zeolite Catalysis and Synthesis
Authors: Yongsheng Wang | Xuejie Zhang | Ya‐Qi Ba | Tianyi Li | Guang‐Ping Hao | An‐Hui Lu
Source: Research (review, 2022-01-01)
Field: Chemistry — Inorganic Chemistry

Recent Advances in Carbon-Based Adsorbents for Adsorptive Separation of Light Hydrocarbons Light hydrocarbons (LHs) separation is an important process in petrochemical industry. The current separation technology predominantly relies on cryogenic distillation, which results in considerable energy consumption. Adsorptive separation using porous solids has received widespread attention due to its lower energy footprint and higher efficiency. Thus, tremendous efforts have been devoted to the design and synthesis of high-performance porous solids. Among them, porous carbons display exceptional stability, tunable pore structure, and surface chemistry and thus represent a class of novel adsorbents upon achieving the matched pore structures for LHs separations. In this review, the modulation strategies toward advanced carbon-based adsorbents for LHs separation are firstly reviewed. Then, the relationships between separation performances and key structural parameters of carbon adsorbents are discussed by exemplifying specific separation cases. The research findings on the control of the pore structures as well as the quantification of the adsorption sites are highlighted. Finally, the challenges of carbonaceous adsorbents facing for LHs separation are given, which would motivate us to rationally design more efficient absorbents and separation processes in future. Adsorption ; Petrochemical ; Porosity ; Distillation ; Carbon fibers ; Chemical engineering ; Separation process ; Separation (statistics) ; Materials science ; Process engineering ; Porous medium ; Carbon footprint ; Nanotechnology ; Chemistry ; Organic chemistry ; Computer science ; Composite number ; Engineering ; Greenhouse gas ; Composite material Metal-Organic Frameworks: Synthesis and Applications ; Membrane Separation and Gas Transport ; Covalent Organic Framework Applications
Authors: Xiaojuan Zhang | Rongfei Yu | Dandan Wang | Weihua Li | Yutao Zhang
Source: Frontiers in Chemistry (article, 2022-05-11)
Field: Chemistry — Inorganic Chemistry

Green Photocatalysis of Organic Pollutants by Bimetallic Zn-Zr Metal-Organic Framework Catalyst A series of bimetallic Zn-Zr metal-organic frameworks (Zn-Zr MOFs) with different Zn:Zr molar ratios has been synthesized <i>via</i> a green hydrothermal method. The structures and morphologies of these photocatalysts have been characterized and analyzed by FTIR, XRD, SEM, and nitrogen adsorption-desorption. The prepared Zn-Zr MOFs had large specific surface areas and pore volumes, favoring the adsorption of pollutant molecules, which in turn led to an improved photocatalytic effect. The photocatalytic activities of the Zn-Zr MOFs under visible light irradiation have been studied towards rhodamine B (RhB) as a target pollutant. The extent of degradation of RhB in a 40 mg/L aqueous solution reached 97.4%. The optimal photocatalyst could also degrade other dyes, suggesting a certain degree of universality. Photocatalysis ; Bimetallic strip ; Rhodamine B ; Catalysis ; Adsorption ; Aqueous solution ; Materials science ; Hydrothermal circulation ; Zirconium ; Inorganic chemistry ; Metal-organic framework ; Metal ; Pollutant ; Polyoxometalate ; Chemical engineering ; Nuclear chemistry ; Chemistry ; Photochemistry ; Organic chemistry ; Metallurgy Metal-Organic Frameworks: Synthesis and Applications ; Advanced Photocatalysis Techniques ; Advanced Nanomaterials in Catalysis
Authors: Jean Coudane | Benjamin Nottelet | Julia Mouton | Xavier Garric | Hélène Van Den Berghe
Source: Molecules (review, 2022-10-28)
Field: Materials Science — Biomaterials

Poly(ε-caprolactone)-Based Graft Copolymers: Synthesis Methods and Applications in the Biomedical Field: A Review Synthetic biopolymers are attractive alternatives to biobased polymers, especially because they rarely induce an immune response in a living organism. Poly ε-caprolactone (PCL) is a well-known synthetic aliphatic polyester universally used for many applications, including biomedical and environmental ones. Unlike poly lactic acid (PLA), PCL has no chiral atoms, and it is impossible to play with the stereochemistry to modify its properties. To expand the range of applications for PCL, researchers have investigated the possibility of grafting polymer chains onto the PCL backbone. As the PCL backbone is not functionalized, it must be first functionalized in order to be able to graft reactive groups onto the PCL chain. These reactive groups will then allow the grafting of new reagents and especially new polymer chains. Grafting of polymer chains is mainly carried out by "grafting from" or "grafting onto" methods. In this review we describe the main structures of the graft copolymers produced, their different synthesis methods, and their main characteristics and applications, mainly in the biomedical field. Caprolactone ; Copolymer ; Materials science ; Field (mathematics) ; Polymer ; Composite material ; Mathematics Electrospun Nanofibers in Biomedical Applications ; biodegradable polymer synthesis and properties ; Graphene and Nanomaterials Applications
Authors: Debashis Mondal | Manzoor Ahmad | Bijoy Dey | Abhishek Mondal | Pinaki Talukdar
Source: Nature Communications (article, 2022-10-31)
Field: Chemistry — Spectroscopy

Formation of supramolecular channels by reversible unwinding-rewinding of bis(indole) double helix via ion coordination Stimulus-responsive reversible transformation between two structural conformers is an essential process in many biological systems. An example of such a process is the conversion of amyloid-β peptide into β-sheet-rich oligomers, which leads to the accumulation of insoluble amyloid in the brain, in Alzheimer's disease. To reverse this unique structural shift and prevent amyloid accumulation, β-sheet breakers are used. Herein, we report a series of bis(indole)-based biofunctional molecules, which form a stable double helix structure in the solid and solution state. In presence of chloride anion, the double helical structure unwinds to form an anion-coordinated supramolecular polymeric channel, which in turn rewinds upon the addition of Ag<sup>+</sup> salts. Moreover, the formation of the anion-induced supramolecular ion channel results in efficient ion transport across lipid bilayer membranes with excellent chloride selectivity. This work demonstrates anion-cation-assisted stimulus-responsive unwinding and rewinding of artificial double-helix systems, paving way for smart materials with better biomedical applications. Supramolecular chemistry ; Helix (gastropod) ; Indole test ; Ion ; Chemistry ; Coordination complex ; Ion channel ; Crystallography ; Materials science ; Stereochemistry ; Biochemistry ; Crystal structure ; Metal ; Biology ; Organic chemistry Molecular Sensors and Ion Detection ; Supramolecular Chemistry and Complexes ; Mass Spectrometry Techniques and Applications
Authors: Chanjong Yu | Young Jae Kim | Jong‐Bum Kim | Kiwon Eum
Source: Nanomaterials (article, 2022-11-27)
Field: Chemistry — Inorganic Chemistry

ZIF-L to ZIF-8 Transformation: Morphology and Structure Controls The control of the structure, shape, and components of metal-organic frameworks, in which metal ions and organic ligands coordinate to form crystalline nanopore structures, plays an important role in the use of many electrochemical applications, such as energy storage, high-performance photovoltaic devices, and supercapacitors. In this study, systematic controls of synthesis variables were performed to control the morphology of ZIF-8 during the ZIF-L-to-ZIF-8 transformation of ZIF-L, which has the same building block as ZIF-8 but forms a two-dimensional structure. Furthermore, additional precursors or surfactants (Zn<sup>2+</sup>, 2mIm, and CTAB) were introduced during the transition to determine whether the alteration could be regulated. Lastly, the partial substitution insertion of a new organic precursor, 2abIm, during the ZIF-L-to-ZIF-8 transformation of ZIF-L was achieved, and modulation of the adsorption and pore characteristics (suppression of gate-opening properties of ZIF-8) has been confirmed. Nanopore ; Materials science ; Supercapacitor ; Metal-organic framework ; Electrochemistry ; Chemical engineering ; Transformation (genetics) ; Adsorption ; Morphology (biology) ; Block (permutation group theory) ; Nanotechnology ; Chemistry ; Electrode ; Organic chemistry ; Physical chemistry Metal-Organic Frameworks: Synthesis and Applications ; MXene and MAX Phase Materials ; Boron and Carbon Nanomaterials Research
Authors: Bingbing Sun | Kun Liu | Quan Gao | Fang Wei | Lu Shuang | Chunru Wang | Chuan‐Zhi Yao | Haiqun Cao | Jie Yu
Source: Nature Communications (article, 2022-11-18)
Field: Chemistry — Organic Chemistry

Enantioselective Ugi and Ugi-azide reactions catalyzed by anionic stereogenic-at-cobalt(III) complexes Ugi reactions and related variations are proven to be atom and step-economic strategies for construction of highly valuable peptide-like skeletons and nitrogenous heterocycles. The development of structurally diverse range of novel catalytic systems and the discovery of new approaches to accommodate a broader scope of terminating reagents for asymmetric Ugi four-component reaction is still in high demand. Here, we report a strategy that enables enantioselective Ugi four-component and Ugi-azide reactions employing anionic stereogenic-at-cobalt(III) complexes as catalysts. The key nitrilium intermediates, generated through the nucleophilic addition of isocyanides to the chiral ion-pair which consists of stereogenic-at-cobalt(III) complexes counteranion and a protonated iminium, are trapped by either carboxylic acids or in situ-generated hydrazoic acid, delivering α-acylamino amides and α-aminotetrazoles in good to excellent enantioselectivities (up to 99:1 e.r.). Stereocenter ; Enantioselective synthesis ; Ugi reaction ; Combinatorial chemistry ; Chemistry ; Iminium ; Azide ; Catalysis ; Protonation ; Nucleophile ; Stereochemistry ; Organic chemistry ; Isocyanide ; Ion Click Chemistry and Applications ; Computational Drug Discovery Methods ; Chemical Synthesis and Analysis
Authors: Yifan Sun | Felipe Polo‐Garzon | Zhenghong Bao | Jisue Moon | Zhennan Huang | Hao Chen | Zitao Chen | Zhenzhen Yang | Miaofang Chi | Zili Wu | Jue Liu | Sheng Dai
Source: Advanced Science (article, 2022-01-20)
Field: Materials Science — Materials Chemistry

Manipulating Copper Dispersion on Ceria for Enhanced Catalysis: A Nanocrystal‐Based Atom‐Trapping Strategy Due to tunable redox properties and cost-effectiveness, copper-ceria (Cu-CeO<sub>2</sub> ) materials have been investigated for a wide scope of catalytic reactions. However, accurately identifying and rationally tuning the local structures in Cu-CeO<sub>2</sub> have remained challenging, especially for nanomaterials with inherent structural complexities involving surfaces, interfaces, and defects. Here, a nanocrystal-based atom-trapping strategy to access atomically precise Cu-CeO<sub>2</sub> nanostructures for enhanced catalysis is reported. Driven by the interfacial interactions between the presynthesized Cu and CeO<sub>2</sub> nanocrystals, Cu atoms migrate and redisperse onto the CeO<sub>2</sub> surface via a solid-solid route. This interfacial restructuring behavior facilitates tuning of the copper dispersion and the associated creation of surface oxygen defects on CeO<sub>2</sub> , which gives rise to enhanced activities and stabilities catalyzing water-gas shift reaction. Combining soft and solid-state chemistry of colloidal nanocrystals provide a well-defined platform to understand, elucidate, and harness metal-support interactions. The dynamic behavior of the supported metal species can be further exploited to realize exquisite control and rational design of multicomponent nanocatalysts. Nanocrystal ; Nanomaterial-based catalyst ; Copper ; Catalysis ; Materials science ; Nanotechnology ; Nanomaterials ; Dispersion (optics) ; Nanoparticle ; Nanostructure ; Rational design ; Chemical engineering ; Chemistry ; Metallurgy Catalytic Processes in Materials Science ; Nanomaterials for catalytic reactions ; Copper-based nanomaterials and applications
Authors: E.M. Huber
Source: ChemBioChem (review, 2022-08-23)
Field: Chemistry — Organic Chemistry

Epipolythiodioxopiperazine‐Based Natural Products: Building Blocks, Biosynthesis and Biological Activities Epipolythiodioxopiperazines (ETPs) are fungal secondary metabolites that share a 2,5-diketopiperazine scaffold built from two amino acids and bridged by a sulfide moiety. Modifications of the core and the amino acid side chains, for example by methylations, acetylations, hydroxylations, prenylations, halogenations, cyclizations, and truncations create the structural diversity of ETPs and contribute to their biological activity. However, the key feature responsible for the bioactivities of ETPs is their sulfide moiety. Over the last years, combinations of genome mining, reverse genetics, metabolomics, biochemistry, and structural biology deciphered principles of ETP production. Sulfurization via glutathione and uncovering of the thiols followed by either oxidation or methylation crystallized as fundamental steps that impact expression of the biosynthesis cluster, toxicity and secretion of the metabolite as well as self-tolerance of the producer. This article showcases structure and activity of prototype ETPs such as gliotoxin and discusses the current knowledge on the biosynthesis routes of these exceptional natural products. Biosynthesis ; Natural (archaeology) ; Synthetic biology ; Chemistry ; Computational biology ; Biochemical engineering ; Combinatorial chemistry ; Biochemistry ; Biology ; Engineering ; Gene Synthesis of heterocyclic compounds ; Chemical Synthesis and Reactions ; Synthesis and Reactivity of Sulfur-Containing Compounds
Authors: Franck Bertorelle | K. David Wegner | Martina Perić Bakulić | Hussein Fakhouri | Clothilde Comby‐Zerbino | Amin Sagar | Pau Bernadó | Ute Resch‐Genger | Vlasta Bonačić‐Koutecký | Xavier Le Guével | Rodolphe Antoine
Source: Chemistry - A European Journal (article, 2022-06-15)
Field: Materials Science — Materials Chemistry

Tailoring the NIR‐II Photoluminescence of Single Thiolated Au<sub>25</sub> Nanoclusters by Selective Binding to Proteins** Atomically precise gold nanoclusters are a fascinating class of nanomaterials that exhibit molecule-like properties and have outstanding photoluminescence (PL). Their ultrasmall size, molecular chemistry, and biocompatibility make them extremely appealing for selective biomolecule labeling in investigations of biological mechanisms at the cellular and anatomical levels. In this work, we report a simple route to incorporate a preformed Au<sub>25</sub> nanocluster into a model bovine serum albumin (BSA) protein. A new approach combining small-angle X-ray scattering and molecular modeling provides a clear localization of a single Au<sub>25</sub> within the protein to a cysteine residue on the gold nanocluster surface. Attaching Au<sub>25</sub> to BSA strikingly modifies the PL properties with enhancement and a redshift in the second near-infrared (NIR-II) window. This study paves the way to conrol the design of selective sensitive probes in biomolecules through a ligand-based strategy to enable the optical detection of biomolecules in a cellular environment by live imaging. Nanoclusters ; Biomolecule ; Photoluminescence ; Nanotechnology ; Bovine serum albumin ; Nanomaterials ; Biocompatibility ; Materials science ; Ligand (biochemistry) ; Nanoparticle ; Chemistry ; Optoelectronics ; Biochemistry Nanocluster Synthesis and Applications ; Advanced Nanomaterials in Catalysis ; Carbon and Quantum Dots Applications
Authors: Simone M. Gillbard | Hon Wai Lam
Source: Chemistry - A European Journal (review, 2022-01-05)
Field: Chemistry — Organic Chemistry

Nickel‐Catalyzed Arylative Cyclizations of Alkyne‐ and Allene‐Tethered Electrophiles using Arylboron Reagents The use of arylboron reagents in metal-catalyzed domino addition-cyclization reactions is a well-established strategy for the preparation of diverse, highly functionalized carbo- and heterocyclic products. Although rhodium- and palladium-based catalysts have been commonly used for these reactions, more recent work has demonstrated nickel catalysis is also highly effective, in many cases offering unique reactivity and access to products that might otherwise not be readily available. This review gives an overview of nickel-catalyzed arylative cyclizations of alkyne- and allene-tethered electrophiles using arylboron reagents. The scope of the reactions is discussed in detail, and general mechanistic concepts underpinning the processes are described. Allene ; Alkyne ; Electrophile ; Reagent ; Catalysis ; Nickel ; Chemistry ; Combinatorial chemistry ; Organic chemistry Catalytic C–H Functionalization Methods ; Catalytic Cross-Coupling Reactions ; Catalytic Alkyne Reactions
Authors: Yves H. Kwan | Glenn Wagner | Nick Bultinck | Steven H. Simon | S. A. Parameswaran
Source: Physical Review X (article, 2022-07-29)
Field: Materials Science — Materials Chemistry

Skyrmions in Twisted Bilayer Graphene: Stability, Pairing, and Crystallization We study the excitations that emerge upon doping the translationally invariant correlated insulating states in magic-angle twisted bilayer graphene at various integer filling factors . We identify parameter regimes where these are excitations associated with skyrmion textures in the spin or pseudospin degrees of freedom, and explore both short-distance pairing effects and the formation of long-range ordered skyrmion crystals. We perform a comprehensive analysis of the pseudospin skyrmions that emerge upon doping insulators at even , delineating the regime in parameter space where these are the lowest-energy charged excitations by means of self-consistent Hartree-Fock calculations on the interacting Bistritzer-MacDonald model. We explicitly demonstrate the purely electron-mediated pairing of skyrmions, a key ingredient behind a recent proposal of skyrmion superconductivity. Building upon this, we construct hopping models to extract the effective masses of paired skyrmions, and discuss our findings and their implications for skyrmion superconductivity in relation to experiments, focusing on the dome-shaped dependence of the transition temperature on the twist angle. We also investigate the properties of spin skyrmions about the quantized anomalous Hall insulator at 3. In both cases, we demonstrate the formation of robust spin or pseudospin skyrmion crystals upon doping to a finite density away from integer filling. Skyrmion ; Pairing ; Condensed matter physics ; Physics ; Bilayer graphene ; Superconductivity ; Spin (aerodynamics) ; Quantum mechanics ; Graphene Graphene research and applications ; Quantum and electron transport phenomena ; Topological Materials and Phenomena
Authors: Andrew L. Ferguson | Keith A. Brown
Source: Annual Review of Chemical and Biomolecular Engineering (review, 2022-03-03)
Field: Materials Science — Materials Chemistry

Data-Driven Design and Autonomous Experimentation in Soft and Biological Materials Engineering This article reviews recent developments in the applications of machine learning, data-driven modeling, transfer learning, and autonomous experimentation for the discovery, design, and optimization of soft and biological materials. The design and engineering of molecules and molecular systems have long been a preoccupation of chemical and biomolecular engineers using a variety of computational and experimental techniques. Increasingly, researchers have looked to emerging and established tools in artificial intelligence and machine learning to integrate with established approaches in chemical science to realize powerful, efficient, and in some cases autonomous platforms for molecular discovery, materials engineering, and process optimization. This review summarizes the basic principles underpinning these techniques and highlights recent successful example applications in autonomous materials discovery, transfer learning, and multi-fidelity active learning. Underpinning ; Computer science ; Fidelity ; Process (computing) ; Variety (cybernetics) ; Data science ; Artificial intelligence ; Biochemical engineering ; Systems engineering ; Human–computer interaction ; Management science ; Engineering Machine Learning in Materials Science ; Computational Drug Discovery Methods ; Innovative Microfluidic and Catalytic Techniques Innovation