jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Risheng Bai | Guangyuan He | Junyan Li | Lin Li | Tianjun Zhang | Xingxing Wang | Wei Zhang | Yongcun Zou | Jichao Zhang | Donghai Mei | Avelino Corma | Jihong Yu
Source: Angewandte Chemie (article, 2024-07-29)
Field: Chemistry — Inorganic Chemistry

Heteroatoms‐Stabilized Single Palladium Atoms on Amorphous Zeolites: Breaking the Tradeoff between Catalytic Activity and Selectivity for Alkyne Semihydrogenation Abstract As a fundamental industrial catalytic process, the semihydrogenation of alkynes presents a challenge in striking a balance between activity and selectivity due to the issue of over‐hydrogenation. Herein, we develop an efficient catalytic system based on single‐atom Pd catalysts supported on boron‐containing amorphous zeolites (Pd/AZ−B), achieving the tradeoff breaking between the activity and selectivity for the selective hydrogenation of alkynes. Advanced characterizations and theoretical density functional theory calculations confirm that the incorporated B atoms in the Pd/AZ−B can not only alter the geometric and electronic properties of Pd atoms by controlling the electron migration from Pd but also mitigate the interaction between alkene and the catalyst supports. This boosts the exceptional catalytic efficacy in the semihydrogenation of phenylacetylene to styrene under mild conditions (298 K, 2 bar H 2 ), achieving a recorded turnover frequency (TOF) value of 24198 h −1 and demonstrating 95 % selectivity to styrene at full conversion of phenylacetylene. By comparison, the heteroatom‐free amorphous zeolite‐anchored Pd nanoparticles and the commercial Lindlar catalyst have styrene selectivities of 73 % and 15 %, respectively, under identical reaction conditions. This work establishes a solid foundation for developing highly active and selective hydrogenation catalysts by controllably optimizing their electronic and steric properties. Phenylacetylene ; Catalysis ; Heteroatom ; Selectivity ; Chemistry ; Styrene ; Alkyne ; Alkene ; Photochemistry ; Steric effects ; Palladium ; Combinatorial chemistry ; Materials science ; Organic chemistry ; Alkyl Metal-Organic Frameworks: Synthesis and Applications ; Advanced Photocatalysis Techniques ; Nanomaterials for catalytic reactions
Authors: Jiahuan Tong | Takumi Miyakage | Takashi Toyao | Ken‐ichi Shimizu
Source: Catalysis Science & Technology (article, 2024-01-01)
Field: Chemistry — Inorganic Chemistry

Influence of temperatures and loadings on olefin diffusion in MFI-type zeolites in one- to three-dimensions A detailed understanding of the molecular diffusion in zeolite frameworks is crucial for analysing the factors controlling their catalytic performance in alkenes. Zeolite ; Olefin fiber ; Diffusion ; Catalysis ; Chemical engineering ; Materials science ; Chemical physics ; Chemistry ; Organic chemistry ; Thermodynamics ; Engineering ; Physics Zeolite Catalysis and Synthesis ; Metal-Organic Frameworks: Synthesis and Applications ; Mesoporous Materials and Catalysis
Authors: James Nicolas Pagaduan | Nicholas Hight‐Huf | Le Zhou | Nicholas Dix | Uvinduni I. Premadasa | Benjamin Doughty | Thomas P. Russell | Ashwin Ramasubramaniam | Michael D. Barnes | Reika Katsumata | Todd Emrick
Source: ACS Central Science (article, 2024-08-06)
Field: Materials Science — Materials Chemistry

Spatial and Bidirectional Work Function Modulation of Monolayer Graphene with Patterned Polymer “Fluorozwitterists” Understanding the electronic properties resulting from soft-hard material interfacial contact has elevated the utility of functional polymers in advanced materials and nanoscale structures, such as in work function engineering of two-dimensional (2D) materials to produce new types of high-performance devices. In this paper, we describe the electronic impact of functional polymers, containing both zwitterionic and fluorocarbon components in their side chains, on the work function of monolayer graphene through the preparation of negative-tone photoresists, which we term "fluorozwitterists." The zwitterionic and fluorinated groups each represent dipole-containing moieties capable of producing distinct surface energies as thin films. Kelvin probe force microscopy revealed these polymers to have a <i>p</i>-doping effect on graphene, which contrasts the work function decrease typically associated with polymer-to-graphene contact. Copolymerization of fluorinated zwitterionic monomers with methyl methacrylate and a benzophenone-substituted methacrylate produced copolymers that were amenable to photolithographic fabrication of fluorozwitterist structures. Consequently, spatial alteration of zwitterion coverage across graphene yielded stripes that resemble a lateral <i>p</i>-<i>i</i>-<i>n</i> diode configuration, with local increase or decrease of work function. Overall, this polymeric fluorozwitterist design is suitable for enabling simple, solution-based surface patterning and is anticipated to be useful for spatial work function modulation of 2D materials integrated into electronic devices. Monolayer ; Kelvin probe force microscope ; Work function ; Graphene ; Polymer ; Materials science ; Nanoscopic scale ; Nanotechnology ; Work (physics) ; Dipole ; Soft materials ; Thin film ; Chemical physics ; Atomic force microscopy ; Chemistry ; Composite material ; Organic chemistry ; Physics ; Layer (electronics) Graphene research and applications ; Molecular Junctions and Nanostructures ; Thermal properties of materials
Authors: Jiayuan Cai | Yong Tian | Xiufang Wang
Source: Advanced Functional Materials (article, 2024-08-02)
Field: Materials Science — Materials Chemistry

Engineering of Asymmetric Hollow Carbon Nanoparticles with Tunable Architecture via Flowable Colloidal Polymer‐Emulsion Assembly Strategy Abstract Asymmetric hollow carbon (AHC) nanoparticles, celebrated for their distinctive external morphology, intricate internal topology, and exceptional carbon performance, are capturing significant attention. Nevertheless, exploring a universal emulsion assembling system to endow them with customizable architectures remains a formidable yet pending challenge. Interestingly, inspired by “plasticization”, a flowable colloidal polymer‐emulsion assembly strategy is first reported. It makes a striking debut of “dynamically growing‐like” AHC architectures, encompassing double‐headed mushroom, pleurotus eryngii, oyster mushroom, mushroom envelope, mushroom cap, and truffle‐shaped. This breakthrough creates an unprecedented “complete coverage” emulsion assembly mode, which surpasses the constraints of conventional “incomplete coverage” mode and infuses fresh vitality into the thriving nanoparticle‐library. More excitingly, it just is a brand‐new mechanism – the synergistic effect of plasticizing and swelling that flexibly manipulates the assembly between size‐variable emulsion droplet templates and flowable colloidal polymer, thereby successfully propelling the reversible architectural evolution. Remarkably, by skillfully integrating double‐headed mushroom‐shaped AHC nanoparticles with PEG and polyurethane sponge to engineer a composite adsorbent with reliable thermophysical property, it can offer a promising avenue for environmental governance. Generally, these cutting‐edge findings not only enrich the theory of emulsion assembly but also spark fresh inspiration for a vast spectrum of potential applications. Materials science ; Emulsion ; Nanotechnology ; Nanoparticle ; Polymer ; Chemical engineering ; Composite material Pickering emulsions and particle stabilization ; Advanced Materials and Mechanics ; Polymer composites and self-healing
Authors: Claudio Tosto | Lorena Saitta | Alberta Latteri | Gianluca Cicala
Source: Polymers (article, 2024-01-29)
Field: Chemistry — Organic Chemistry

Epoxy-Based Blend Formulation for Dual Curing in Liquid Crystal Display 3D Printing: A Study on Thermomechanical Properties Variation for Enhanced Printability The aim of this study was to explore the thermal properties of epoxy-acrylate blends for the liquid crystal display (LCD) 3D printing technique. Starting from an epoxy-acrylate blend with a ratio of epoxy to acrylate of 50:50, the effect of adding a reactive monofunctional epoxy diluent was evaluated. The diluent was a resin composed by oxirane, mono[(C12-14 alkyl) methyl] derivatives selected for its low viscosity (i.e., 1.8 Poise) at room temperature and its reactivity. The diluent content varied from 15 to 25 wt% and, for all the formulation, double curing cycles, where thermal curing followed photocuring, were studied. The effect of different curing temperatures was also evaluated. The control of the diluent content and of the curing temperature allowed tailoring of the thermomechanical resin properties while improving the resin's processability. The glass transition ranged from 115.4 °C to 90.8 °C depending on the combination of diluent content and post-curing temperature. The resin developed displayed a faster processing time tested on a reference part with printing time of 4 h and 20 min that was much lower than the printing times (7 and 16 h) observed for the starting formulations. Diluent ; Materials science ; Curing (chemistry) ; Epoxy ; Glass transition ; Composite material ; Acrylate ; UV curing ; Thermal stability ; Thermomechanical analysis ; Polymer chemistry ; Chemical engineering ; Thermal expansion ; Polymer ; Organic chemistry ; Chemistry Photopolymerization techniques and applications ; Additive Manufacturing and 3D Printing Technologies ; Epoxy Resin Curing Processes
Authors: Su Min Lee | Hongryeol Yun | Min‐Jung Kang | Hyojin Kim | Dong Won Kang | Chang Seop Hong
Source: ChemSusChem (article, 2024-07-17)
Field: Materials Science — Materials Chemistry

Tailored Postsynthetic Nitration of a Hypercrosslinked Polymer for Single‐Step Ethylene Purification from a Ternary C<sub>2</sub> Gas Mixture Purifying C<sub>2</sub>H<sub>4</sub> from a ternary C<sub>2</sub>H<sub>2</sub>/C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub> mixture poses a substantial industrial challenge due to their close physical and chemical properties. In this study, we introduce an innovative design approach to regulate and optimize the nitration degree of a hypercrosslinked polymer to achieve targeted separation performance. We synthesized a porous organic polymer (HCP) using the solvent knitting method and carried out its postsynthetic nitration, resulting in HCP-NO<sub>2</sub>-1 and HCP-NO<sub>2</sub>-2 with different nitration degrees. Notably, the adsorption capacity shifted from C<sub>2</sub>H<sub>6</sub> > C<sub>2</sub>H<sub>4</sub> ≈ C<sub>2</sub>H<sub>2</sub> for HCP to C<sub>2</sub>H<sub>2</sub> > C<sub>2</sub>H<sub>6</sub> > C<sub>2</sub>H<sub>4</sub> for HCP-NO<sub>2</sub>-1 and to C<sub>2</sub>H<sub>2</sub> > C<sub>2</sub>H<sub>4</sub> ≈ C<sub>2</sub>H<sub>6</sub> for HCP-NO<sub>2</sub>-2, demonstrating the controllable nature of the separation process via the polar nitro group insertion. Remarkably, HCP-NO<sub>2</sub>-1 exhibited a desirable, selective separation of C<sub>2</sub>H<sub>4</sub> from the C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>2</sub> mixture thanks to an exquisite combination of the acidic proton-polar nitro group and nonpolar C-H⋅⋅⋅π interactions. Separation capability was further corroborated by computational simulations and breakthrough tests. This work marks a significant advancement as the first successful postsynthetic functionalization strategy for C<sub>2</sub>H<sub>4</sub> purification from a ternary gas mixture among porous organic polymers. Nitration ; Ternary operation ; Polymer ; Adsorption ; Chemical engineering ; Materials science ; Solvent ; Nitro ; Separation process ; Chemistry ; Organic chemistry ; Chromatography Covalent Organic Framework Applications ; Metal-Organic Frameworks: Synthesis and Applications ; Membrane Separation and Gas Transport
Authors: Federico Coppola | Raoul Carfora | Paola Cimino | Alessio Petrone | Nadia Rega
Source: Theoretical Chemistry Accounts (article, 2024-11-09)
Field: Chemistry — Spectroscopy

Tetracyanoethylene $$\hbox {Na}^+$$/$$\hbox {K}^+$$ radical anion coordination sites unveiled via electronic and vibrational fingerprints Abstract Tetracyanoethylene (TCNE) is a very effective electron acceptor and can form stable complexes with various chemical species and is known for its interesting electronic and optical properties. The formation of the monoanion gives TCNE unique electronic and chemical properties, making it a material of interest for several technological applications including solar cells, organic battery electrodes, sodium/potassium-ion batteries and information storage devices. The chemico-physical characterization of $$\hbox {Na}^+$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mtext>Na</mml:mtext> <mml:mo>+</mml:mo> </mml:msup> </mml:math> and $$\hbox {K}^+$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mtext>K</mml:mtext> <mml:mo>+</mml:mo> </mml:msup> </mml:math> coordination of TCNE in solution is not available so far, although it would be valuable for understanding the molecular mechanisms of charging and discharging processes in innovative battery devices. The present theoretical-computational study characterizes the vibrational and electronic properties of ion-coordinated TCNE in solution. We analyzed the ground electronic state through equilibrium structures, focusing on structural features, stability, optical properties and Raman vibrational modes. The $$\hbox {Na}^+$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mtext>Na</mml:mtext> <mml:mo>+</mml:mo> </mml:msup> </mml:math> and $$\hbox {K}^+$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mtext>K</mml:mtext> <mml:mo>+</mml:mo> </mml:msup> </mml:math> cations, coordinated at two distinct sites, significantly alter the geometry, and modulate electronic and vibrational properties. Using ab initio molecular dynamics simulations, we computed vibrational spectra, finding that TCNE complexes serve as effective probes for detecting environmental variations, with key vibrational modes on CC and CN moieties being sensitive to cation interactions. Additionally, a correlation between C=C bond distances and vibrational frequencies was observed. In conclusion, this study provides further insight into the role of TCNE in optoelectronic applications and nonaqueous battery systems. Tetracyanoethylene ; Ion ; Chemistry ; Crystallography ; Computational chemistry ; Stereochemistry ; Photochemistry ; Organic chemistry Molecular Sensors and Ion Detection ; Electrochemical Analysis and Applications ; Photochemistry and Electron Transfer Studies
Authors: Christian A. Totoiu | Alec H. Follmer | Paul H. Oyala | Ryan G. Hadt
Source: The Journal of Physical Chemistry B (article, 2024-10-11)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Probing Bioinorganic Electron Spin Decoherence Mechanisms with an Fe <sub>2</sub> S <sub>2</sub> Metalloprotein Recent efforts have sought to develop paramagnetic molecular quantum bits (qubits) as a means to store and manipulate quantum information. Emerging structure-property relationships have shed light on electron spin decoherence mechanisms. While insights within molecular quantum information science have derived from synthetic systems, biomolecular platforms would allow for the study of decoherence phenomena in more complex chemical environments and further leverage molecular biology and protein engineering approaches. Here we have employed the exchange-coupled <i>S</i><sub>T</sub> = 1/2 Fe<sub>2</sub>S<sub>2</sub> active site of putidaredoxin, an electron transfer metalloprotein, as a platform for fundamental mechanistic studies of electron spin decoherence toward spin-based biological quantum sensing. At low temperatures, decoherence rates were anisotropic, reflecting a hyperfine-dominated decoherence mechanism, standing in contrast to the anisotropy of molecular systems observed previously. This mechanism provided a pathway for probing spatial effects on decoherence, such as protein vs solvent contributions. Furthermore, we demonstrated spatial sensitivity to single point mutations via site-directed mutagenesis and temporal sensitivity for monitoring solvent isotope exchange. Thus, this study demonstrates a step toward the design and construction of biomolecular quantum sensors. Bioinorganic chemistry ; Quantum decoherence ; Metalloprotein ; Spin (aerodynamics) ; Condensed matter physics ; Electron ; Azurin ; Physics ; Materials science ; Chemistry ; Nuclear magnetic resonance ; Redox ; Inorganic chemistry ; Quantum mechanics ; Enzyme ; Stereochemistry Magnetism in coordination complexes ; Electron Spin Resonance Studies ; Porphyrin and Phthalocyanine Chemistry
Authors: Cintya Pinilla | Mario García-Zarza | Ana C. Albéniz
Source: Organic Chemistry Frontiers (article, 2024-10-31)
Field: Chemistry — Organic Chemistry

Metal–ligand cooperation and synergistic palladium catalysis for the dual ligand system [2,2′-bipyridin]-6(1<i>H</i>)–one/PCy<sub>3</sub>: milder conditions for the undirected C–H arylation of arenes The mixture of Pd(OAc) 2 and two ligands segregate into distinct active species working synergistically for the C–H arylation of simple arenes. Chemistry ; Palladium ; Ligand (biochemistry) ; Dual (grammatical number) ; Catalysis ; Metal ; Dual role ; Combinatorial chemistry ; Medicinal chemistry ; Stereochemistry ; Organic chemistry ; Receptor Catalytic C–H Functionalization Methods ; Catalytic Cross-Coupling Reactions ; Asymmetric Hydrogenation and Catalysis
Authors: Belén Lobato | Samantha L. Flores‐López | Lucía dos Santos‐Gómez | Ana B. Garcı́a | A.M. Pernía | M.J. Prieto | María G. Busto | Ana Arenillas
Source: Nanomaterials (article, 2024-12-18)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Designing and Optimizing Electrode Materials for Energy Harvesting in CAPMIX Cells The growing demand for clean, decentralized energy has increased interest in blue energy, which generates power from water with different salt concentrations. Despite its potential as a renewable, low-cost energy source, optimizing electrode materials remains a challenge. This work presents a nanomaterial developed via microwave-assisted sol-gel methodology for blue energy applications, where ion diffusion and charge storage are critical. AX-7 carbon, designed for this study, features wide pores, enhancing ion diffusion. Compared to commercial NORIT carbon, AX-7 has a higher mesopore volume and external surface area, improving its overall performance. The synthesis process has been optimized and scaled up for evaluation in CAPMIX electrochemical cell stacks. Moreover, the lower series resistance (Rs) significantly boosts energy recovery, with AX-7 demonstrating superior performance. This advantage is especially evident during fresh-water cycles, where this material achieves significantly lower Rs compared to the commercial one. Materials science ; Renewable energy ; Electrode ; Energy storage ; Carbon fibers ; Specific energy ; Nanotechnology ; Electrochemistry ; Diffusion ; Nanomaterials ; Energy harvesting ; Mesoporous material ; Chemical engineering ; Process engineering ; Power (physics) ; Composite material ; Electrical engineering ; Chemistry ; Catalysis ; Composite number Supercapacitor Materials and Fabrication ; Membrane-based Ion Separation Techniques ; Advanced battery technologies research
Authors: Carolina Méndez‐Gálvez | Boris Olsthoorn | Fredrik Barnå | David Estébanez Rosich | Paul J. Gates | Lukasz T. Pilarski
Source: ChemRxiv (preprint, 2024-03-28)
Field: Chemistry — Inorganic Chemistry

Grind-and-Heat: Solvent-free Catalytic C–H and C–X Functionalization Without a Ball Mill This study describes an accessible approach to various solvent-free transition metal-catalyzed C–H and C–X functionalizations. Conditions from eight different Rh-, Ru-, Ir- and Pd-based mechanochemical reactions are adapted to proceed with generally high efficiency by substituting automated ball milling with pestle and mortar grinding and subsequent heating. This is a low-cost, operationally simple method that requires no specialized equipment and offers similar sustainability benefits. The reaction scope encompasses 10 heterocycle types, many pendant functional groups and is demonstrated on the late-stage modification of a variety of bioactive compounds. Grind ; Surface modification ; Ball mill ; Mill ; Catalysis ; Ball (mathematics) ; Materials science ; Chemical engineering ; Chemistry ; Metallurgy ; Mechanical engineering ; Organic chemistry ; Engineering ; Mathematics ; Grinding ; Geometry Asymmetric Hydrogenation and Catalysis ; Catalytic C–H Functionalization Methods ; Catalytic Processes in Materials Science
Authors: R. Kiran | Nimitha S. Prabhu | Vikash Mishra | M.I. Sayyed | Sudha D. Kamath
Source: Indian Journal of Physics (article, 2024-10-07)
Field: Materials Science — Materials Chemistry

Nuanced synthesis strategies and comprehensive analysis of intricate multifarious luminescent phosphor hosts Abstract This paper primarily addresses various methodologies for synthesizing novel phosphors, with our focus mainly on the mixed alkaline tungstate phosphor Ca 2 MgWO 6 . In the initial synthesis phase, we used precisely weighed CaCO 3 , MgO, and WO 3 for the synthesis. The XRD patterns indicated the presence of an impure phase, specifically CaWO 4 , in the resulting product. We adeptly tackled the formation of CaWO 4 and mitigated it by employing a multifaceted approach. These included adding an excess amount of MgO, opting for an alternative chemical route, and the incorporation of flux during synthesis. It was observed that the product obtained through the addition of flux exhibited a purity level of approximately 99.75% with a margin of error of ± 0.02%. Ultimately, we have carried out structural, morphological, optical, and thermal characterizations, along with density functional theory (DFT) simulations, to assess the fundamental parameters of the pure sample. Phosphor ; Luminescence ; Computer science ; Materials science ; Nanotechnology ; Optoelectronics Luminescence Properties of Advanced Materials ; Radiation Detection and Scintillator Technologies ; Solid-state spectroscopy and crystallography
Authors: Stefania M. Scalzullo | Garreth L. Morgans | Robin Klintworth | Charles B. de Koning | Manuel A. Fernandes | Willem A. L. van Otterlo | Joseph P. Michael
Source: European Journal of Organic Chemistry (article, 2024-01-09)
Field: Chemistry — Organic Chemistry

Chromenone‐Fused Pyrrolizines and Pyrrolizine Analogues of Lamellarins: Expanding the Lamellarin Family Abstract Several N ‐ethoxycarbonylmethyl enaminones, prepared by Eschenmoser sulfide contraction between N ‐(ethoxycarbonylmethyl)pyrrolidine‐2‐thione and various ortho ‐oxygenated phenacyl halides, underwent cyclisation to give ethyl 6‐aryl‐2,3‐dihydro‐1 H ‐pyrrolizine‐5‐carboxylates upon microwave heating with silica gel in xylene. With enaminones made from ortho ‐hydroxyphenacyl halides, not only did dihydropyrrolizine formation take place, but spontaneous lactonisation also occurred to give 9,10‐dihydrochromeno[4,3‐ b ]pyrrolizin‐6(8 H )‐ones. Bromination and Suzuki‐Miyaura arylation of these chromenopyrrolizines at the free C−H site on the pyrrole ring afforded four analogues of the lamellarin alkaloids in which a pyrrolidine ring replaces the isoquinoline system in the fused polycyclic core. The product 11‐(3,4‐dimethoxyphenyl)‐2,3‐dimethoxy‐9,10‐dihydrochromeno[4,3‐ b ]pyrrolizin‐6(8 H )‐one, in particular, is a congener of the well‐known lamellarin G trimethyl ether. Preliminary results pertaining to an extension to chromenone‐fused indolizines are also reported. Chemistry ; Pyrrolidine ; Stereochemistry ; Pyrrole ; Isoquinoline ; Medicinal chemistry ; Halide ; Ring (chemistry) ; Ether ; Organic chemistry Synthesis and Characterization of Pyrroles ; Synthesis and Reactions of Organic Compounds ; Porphyrin and Phthalocyanine Chemistry