jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Dipankar Ghosh | Sophie Coulter | Garry Laverty | Chris Holland | James Doutch | Massimo Vassalli | Dave J. Adams
Source: Biomacromolecules (article, 2024-04-29)
Field: Materials Science — Biomaterials

Metal Cross-Linked Supramolecular Gel Noodles: Structural Insights and Antibacterial Assessment Achieving precise control over gelator alignment and morphology is crucial for crafting tailored materials and supramolecular structures with distinct properties. We successfully aligned the self-assembled micelles formed by a functionalized dipeptide 2NapFF into long 1-D "gel noodles" by cross-linking with divalent metal chlorides. We identify the most effective cross-linker for alignment, enhancing mechanical stability, and imparting functional properties. Our study shows that Group 2 metal ions are particularly suited for creating mechanically robust yet flexible gel noodles because of their ionic and nondirectional bonding with carboxylate groups. In contrast, the covalent nature and high directional bonds of <i>d</i>-block metal ions with carboxylates tend to disrupt the self-assembly of 2NapFF. Furthermore, the 2NapFF-Cu noodles demonstrated selective antibacterial activity, indicating that the potent antibacterial property of the copper(II) ion is preserved within the cross-linked system. By merging insights into molecular alignment, gel extrusion processing, and integrating specific functionalities, we illustrate how the versatility of dipeptide-based gels can be utilized in creating next-generation soft materials. Supramolecular chemistry ; Dipeptide ; Chemistry ; Metal ions in aqueous solution ; Carboxylate ; Covalent bond ; Ionic bonding ; Metal ; Self-assembly ; Combinatorial chemistry ; Linker ; Micelle ; Antibacterial activity ; Nanotechnology ; Polymer chemistry ; Ion ; Molecule ; Materials science ; Organic chemistry ; Peptide Supramolecular Self-Assembly in Materials ; Metal-Organic Frameworks: Synthesis and Applications ; Nanoplatforms for cancer theranostics
Authors: Jesús Antonio Cruz-Navarro | Fabiola Hernández-García | Arturo Sánchez‐Mora | María Esther Moreno-Narváez | Viviana Reyes‐Márquez | Raúl Colorado‐Peralta | David Morales‐Morales
Source: Methane (review, 2024-08-27)
Field: Chemistry — Inorganic Chemistry

Copper-Based Metal–Organic Frameworks Applied as Electrocatalysts for the Electroreduction of Carbon Dioxide (CO2ER) to Methane: A Review The electrochemical reduction of carbon dioxide (CO2) to methane (CH4) holds tremendous potential in mitigating greenhouse gas emissions and producing renewable fuels. Thus, this review provides a comprehensive overview of the utilization of copper-based metal–organic frameworks (Cu-MOFs) as catalysts for this transformative process. Diverse key aspects of Cu-MOFs that make them ideal candidates for CO2 reduction are discussed, including their high surface areas, tunable pore sizes, and customizable active sites. Furthermore, recent advances in the design and synthesis of Cu-MOFs tailored specifically for enhanced catalytic activity and selectivity towards CH4 production are highlighted. Additionally, mechanistic insights into the CO2 reduction process on Cu-MOF catalysts are examined. Moreover, the recent application of diverse Cu-MOFs and derived materials in electrochemical reduction systems is discussed, and future research directions and potential applications of Cu-MOFs in sustainable energy conversion technologies are outlined. Thus, this review provides valuable insights into the current state of the art and the prospects for utilizing Cu-MOFs as efficient catalysts for the electrochemical conversion of CO2 to CH4, offering a pathway towards a greener and more sustainable energy future. Methane ; Metal-organic framework ; Catalysis ; Renewable energy ; Nanotechnology ; Electrochemical reduction of carbon dioxide ; Materials science ; Electrochemistry ; Greenhouse gas ; Environmental science ; Chemistry ; Carbon monoxide ; Electrode ; Engineering ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; CO2 Reduction Techniques and Catalysts ; Covalent Organic Framework Applications
Authors: Barbara Vörös-Horváth | Ala’ Salem | Barna Kovács | Aleksandar Széchenyi | Szilárd Pál
Source: Nanomaterials (article, 2024-09-27)
Field: Materials Science — Materials Chemistry

Systematic Study of Reaction Conditions for Size-Controlled Synthesis of Silica Nanoparticles This study presents a reproducible and scalable method for synthesizing silica nanoparticles (SNPs) with controlled sizes below 200 nm, achieved by systematically varying three key reaction parameters: ammonium hydroxide concentration, water concentration, and temperature. SNPs with high monodispersity and controlled dimensions were produced by optimizing these factors. The results indicated a direct correlation between ammonium hydroxide concentration and particle size, while higher temperatures resulted in smaller particles with increased polydispersity. Water concentration also influenced particle size, with a quadratic relationship observed. This method provides a robust approach for tailoring SNP sizes, with significant implications for biomedical applications, particularly in drug delivery and diagnostics. Using eco-friendly solvents such as ethanol further enhances the sustainability and cost-effectiveness of the process. Dispersity ; Ammonium hydroxide ; Particle size ; Materials science ; Nanoparticle ; Chemical engineering ; Nanotechnology ; Polymer chemistry Mesoporous Materials and Catalysis ; Catalytic Processes in Materials Science ; Iron oxide chemistry and applications
Authors: Ziad Alsudairy | Allea Campbell | Qi Zheng | Chelsea Harrod | Normanda Brown | Allison Saintlima | Raghu V. Maligal‐Ganesh | Conrad W. Ingram | Xinle Li
Source: Chemistry - A European Journal (article, 2024-09-30)
Field: Materials Science — Materials Chemistry

Microwave‐Assisted One‐Step Synthesis of Palladium‐Encapsulated Covalent Organic Frameworks for Heterogeneous Catalysis Metal-encapsulated covalent organic frameworks (metal/COFs) represent an emerging paradigm in heterogeneous catalysis. However, the time-intensive (usually 4 or more days) and tedious multi-step synthesis of metal/COFs remains a significant stumbling block for their broad application. To address this challenge, we introduce a facile microwave-assisted in situ metal encapsulation strategy to cooperatively combine COF formation and in situ palladium(II) encapsulation in one step. With this unprecedented approach, we synthesize a diverse range of palladium(II)-encapsulated COFs (termed Mw-Pd/COF) in the air within just an hour. Notably, this strategy is scalable for large-scale production (~0.5 g). Leveraging the high crystallinity, porosity, and structural stability, one representative Mw-Pd/COF exhibits remarkable activity, functional group tolerance, and recyclability for the Suzuki-Miyaura coupling reaction at room temperature, surpassing most previously reported Pd(II)/COF catalysts with respect to catalytic performance, preparation time, and synthetic ease. This microwave-assisted in situ metal encapsulation strategy opens a facile and rapid avenue to construct metal/COF hybrids, which hold enormous potential in a multitude of applications including heterogeneous catalysis, sensing, and energy storage. Palladium ; Catalysis ; Covalent organic framework ; Materials science ; Nanotechnology ; Heterogeneous catalysis ; Covalent bond ; Metal-organic framework ; Metal ; Porosity ; Chemistry ; Organic chemistry Covalent Organic Framework Applications ; Metal-Organic Frameworks: Synthesis and Applications ; Catalytic Cross-Coupling Reactions
Authors: Hao Gu | Takuro Yokoya | Liqun Kang | Sushila Marlow | Xinlian Su | Manxi Gong | Jay Hon Cheung Yan | Yifei Ren | Zhipeng Wang | Xuze Guan | Longxiang Liu | Zhangyi Yao | Luke L. Keenan | Hiroyuki Asakura | Feng Ryan Wang
Source: ChemRxiv (preprint, 2024-04-22)
Field: Chemistry — Physical and Theoretical Chemistry

Oxygen vacancy formation as the rate-determining step in the Mars-van Krevelen mechanism The Mars-van Krevelen mechanism (MvK) is a widely recognized model for describing the role of lattice oxygen in catalysis. Following the MvK mechanism, the formation and conversion of surface oxygen vacancy (VO) are considered as the key steps. CeO2-ZrO2 (CZ) mixed oxides are the typical catalyst support in MvK mechanism. They have the unique property of hosting remarkable amount of VO without significant change in lattice structure, offering O storage and release capability that maintains the required concentration of active O on the catalytic surface. In this regard, the rate of VO formation and conversion directly affect their catalytic performance. In this work, we obtained the VO formation and conversion kinetics by measuring the rate of the Ce4+ reduction and oxidation via operando energy dispersive Extended X-ray Absorption Fine Structure (EDE). The main conclusions are: 1) VO formation is 10 times faster than VO conversion; 2) VO formation rates are comparable with the CO oxidation rates, thereby serving as the rate-determining step in CO oxidation; 3) Pd and Cu serve as catalysts for VO formation by significantly improving its rate by 50 times at 250 C by weakening the metal-O bonding strength, whereas the activation energy have been reduced to 58.4 kJ/mol and 36.5 kJ/mol, respectively. Our method in measuring and analysing partial reaction rates within a turnover is therefore important for all chemical reactions. Mars Exploration Program ; Mechanism (biology) ; Oxygen ; Astrobiology ; Chemistry ; Physics ; Philosophy ; Epistemology ; Organic chemistry thermodynamics and calorimetric analyses ; Chemical Thermodynamics and Molecular Structure ; Advanced Control Systems Optimization
Authors: Josephine Bicknell | Sidhaesh A. Agarwal | Kyle J. Petersen | Jesus Daniel Loya | Nicholas Lutz | Paulina M. Sittinger | Simon J. Teat | Nicholas S. Settineri | Gonzalo Campillo‐Alvarado
Source: Crystal Growth & Design (article, 2024-05-30)
Field: Chemistry — Physical and Theoretical Chemistry

Engineering Lipophilic Aggregation of Adapalene and Adamantane-Based Cocrystals via van der Waals Forces and Hydrogen Bonding Lipophilic aggregation using adamantanes is a widely exploited molecular property in medicinal and materials chemistry. Adamantanes are traditionally installed to molecular units via covalent bonds. However, the noncovalent installation of adamantanes has been relatively underexplored and presents the potential to bring properties associated with adamantanes to molecules without affecting their intrinsic properties (e.g., pharmacophores). Here, we systematically study a series of adamantanecarboxylic acids with varying substitution levels of methyl groups and their cocrystals with bipyridines. Specifically, single-crystal X-ray diffraction shows that while the directionality of single-component adamantanes is notably sensitive to changes in methyl substitution, hydrogen-bonded cocrystals with bipyridines show consistent and robust packing due to π-stacking predominance. Our observations are supported by Hirshfeld surface and energy framework analyses. The applicability of cocrystal formation of adamantanes bearing carboxylic acids was used to generate the first cocrystals of adapalene, an adamantane-bearing retinoid used for treating acne vulgaris. We envisage our study to inspire noncovalent (i.e., cocrystal) installation of adamantanes to generate lipophilic aggregation in multicomponent systems. Cocrystal ; Adamantane ; Non-covalent interactions ; Chemistry ; Hydrogen bond ; van der Waals force ; Crystal engineering ; Stacking ; Supramolecular chemistry ; Covalent bond ; Stereochemistry ; Molecule ; Crystallography ; Organic chemistry Crystallography and molecular interactions ; Chemical Thermodynamics and Molecular Structure ; Porphyrin and Phthalocyanine Chemistry
Authors: Shaowen Deng | Zhong-Yan Li | Lin Yuan | Huaqiang Zeng
Source: Molecules (article, 2024-03-01)
Field: Chemistry — Spectroscopy

An Exceptionally Active and Highly Selective Perchlorate Transporter Containing a Trimesic Amide Scaffold We report here a series of alkyl group-modified trimesic amide molecules (<b>TA</b>s) with excellent anion transport activities. Among them, <b>TA6,</b> with the highest ion transport activity and excellent selectivity, efficiently transports anions across the membrane in the order of ClO<sub>4</sub><sup>-</sup> > I<sup>-</sup> > NO<sub>3</sub><sup>-</sup> > Br<sup>-</sup> > Cl<sup>-</sup>, with an <i>EC</i><sub>50</sub> value as low as 17.6 nM (0.022 mol% relative to lipid molecules) for ClO<sub>4</sub><sup>-</sup>, which outperforms other anions by 5- to 22-folds and manifests as the best perchlorate transporter ever reported. Perchlorate ; Selectivity ; Trimesic acid ; Amide ; Alkyl ; Transporter ; Chemistry ; Molecule ; Scaffold ; Ion ; Membrane ; Divalent ; Organic chemistry ; Biochemistry ; Gene ; Medicine Molecular Sensors and Ion Detection ; Supramolecular Self-Assembly in Materials ; DNA and Nucleic Acid Chemistry
Authors: Ga-Ram Hong | Kyoung–Jin Kim | Seon-Yong Ahn | Beom‐Jun Kim | Bong–Gyeong Shin | Min-Ju Oh | Yeol–Lim Lee | Hyun‐Seog Roh
Source: Catalysts (article, 2024-01-25)
Field: Materials Science — Materials Chemistry

The Effect of Precursor Concentration on the Crystallite Size of CeO2 to Enhance the Sulfur Resistance of Pt/CeO2 for Water Gas Shift To develop customized sulfur–resistant catalysts for the water gas shift (WGS) reaction in the waste–to–hydrogen process, the effects of changing the nucleation conditions of the CeO2 support on catalytic performance were investigated. Supersaturation is a critical kinetic parameter for nuclei formation. The degree of supersaturation of the CeO2 precipitation solution was controlled by varying the cerium precursor concentration from 0.02 to 0.20 M. Next, 2 wt.% of Pt was impregnated on those various CeO2 supports by the incipient wetness impregnation method. The prepared samples were then evaluated in a WGS reaction using waste–derived synthesis gas containing 500 ppm H2S. The Pt catalyst supported by CeO2 prepared at the highest precursor concentration of 0.20 M exhibited the best sulfur resistance and catalytic activity regeneration. The sulfur tolerance of the catalyst demonstrated a close correlation with its oxygen storage capacity and easier reducibility. The formation of oxygen vacancies in CeO2 supports is promoted by the formation of small crystals due to a high degree of supersaturation. Crystallite ; Sulfur ; Chemical engineering ; Materials science ; Chemistry ; Metallurgy Catalytic Processes in Materials Science ; Catalysis and Hydrodesulfurization Studies ; Industrial Gas Emission Control
Authors: Yerbolat Magazov | Asset Aliyev | Kuanysh Moldabekov | Aliya Rakymbekova | Assel Rakymbekova | Magzhan Amze | N. Kh. Ibrayev | V. I. Kudryashov
Source: ES Energy & Environments (review, 2024-01-01)
Field: Materials Science — Materials Chemistry

Photoelectrochemical Water Splitting Using Cuprous Oxide (Cu2O)-Based Photocathode – A Review Here, we present a critical mini-review of the progression achieved and bottlenecks faced in the context of cuprous oxide (Cu2O)-based hybrid cells for photoelectrochemical water splitting, with a special focus on their integration with upconversion materials, photovoltaic systems and photoanodes for unbiased tandem devices.Cu2O photocathodes exhibit attractive properties that make them an appealing option, including a suitable bandgap, low-cost processing, and the potential for solarto-hydrogen efficiencies of up to 18% over a theoretical limit; however, their widespread application is limited by photocorrosion, low photocurrent, and poor light absorption.These systems demonstrate solutions to these challenges in solar-driven hydrogen generation, such as adding upconversion materials to increase the absorption spectrum and a tandem configuration for photovoltage and overall efficiency.It highlights the compact and modular features of this type of cell while reviewing its design principles, material strategies, performance metrics, and large-scale blending with renewable hydrogen production. Photocathode ; Water splitting ; Oxide ; Materials science ; Optoelectronics ; Photoelectrochemistry ; Photoelectrochemical cell ; Electrochemistry ; Chemistry ; Physics ; Metallurgy ; Photocatalysis ; Catalysis ; Electrode ; Physical chemistry Copper-based nanomaterials and applications ; ZnO doping and properties ; Electronic and Structural Properties of Oxides
Authors: Shunhan Jia | Xiaofu Sun | Buxing Han
Source: Chemical Communications (review, 2024-12-11)
Field: Materials Science — Materials Chemistry

Electrocatalytic systems for NO<sub><i>x</i></sub> upgrading Chemical manufacturing utilizing renewable resources and energy presents a promising avenue toward sustainability and carbon neutrality. Electrocatalytic upgrading of nitrogen oxides (NO<sub><i>x</i></sub>) into nitrogenous chemicals is a potential strategy for synthesizing chemicals and mitigating NO<sub><i>x</i></sub> pollution. However, this approach is currently hindered by low selectivity and efficiency, limited reaction pathways, and economic challenges, primarily due to the development of suboptimal electrocatalytic systems for NO<sub><i>x</i></sub> upgrading. In this review, we focus on electrocatalytic systems for NO<sub><i>x</i></sub> upgrading and discuss newly developed components, including catalysts, solvents, electrolysers, and upstream/downstream processes. These advancements enable recent developments in NO<sub><i>x</i></sub> upgrading reactions that yield various products, including green ammonia (NH<sub>3</sub>), dinitrogen (N<sub>2</sub>), nitrogenous chemicals beyond NH<sub>3</sub> and N<sub>2</sub> (<i>e.g.</i>, hydroxylamine and hydrazine), and organonitrogen compunds. Additionally, we provide an outlook to highlight future directions in the emerging field of novel electrocatalytic systems for NO<sub><i>x</i></sub> upgrading. NOx ; Renewable energy ; Electrocatalyst ; Carbon neutrality ; Sustainability ; Chemistry ; Carbon fibers ; Nitrogen oxides ; Environmental science ; Nanotechnology ; Waste management ; Materials science ; Electrochemistry ; Electrode ; Organic chemistry ; Engineering ; Combustion ; Composite number Catalytic Processes in Materials Science ; Catalysis and Oxidation Reactions ; Electrocatalysts for Energy Conversion
Authors: Francesco Dalena | Eddy Dib | Barbara Onida | Giorgia Ferrarelli | Marco Daturi | G. Giordano | Massimo Migliori | Svetlana Mintova
Source: Molecules (article, 2024-09-19)
Field: Chemistry — Inorganic Chemistry

Evaluation of Zeolite Composites by IR and NMR Spectroscopy In this study, we assessed the quantity, strength, and acidity of zeolite composites comprising Silicalite-1 grown on ZSM-5 crystals using a combination of infrared (IR) and solid-state nuclear magnetic resonance (NMR) spectroscopy. The composites were created through the direct growth of Silicalite-1 crystals on ZSM-5 (P_ZSM-5), either with or without the organic structure-directing agent (OSDA) introduced into the ZSM-5 channels (samples: H_ZSM-5_Sil1 and TPA_ZSM-5_Sil1). The results revealed that Silicalite-1 grew differently when the ZSM-5 core was in the H<sup>+</sup> form (empty pores) compared to when the OSDA was still present in the sample. This distinction was evident in the textural properties, with a decrease in the micropore surface area and an increase in the external surface area in the H_ZSM-5_Sil1 compared to the parent sample. The TPA_ZSM-5_Sil1 composite exhibited characteristics similar to the parent zeolite. These findings were further supported by <sup>29</sup>Si NMR, which revealed a comparable local order for the parent (P_ZSM-5) and TPA_ZSM-5_Sil1 samples, along with a broadening of the Q<sup>4</sup> peak for the H_ZSM-5_Sil1 composite. Additionally, the acid sites were preserved in the TPA_ZSM-5_Sil1 composite, while in the H<sup>+</sup>-form core, the concentration of Brønsted acid sites significantly decreased. This reduction in isolated Brønsted acid sites was further corroborated by <sup>1</sup>H NMR. Zeolite ; ZSM-5 ; Microporous material ; Chemistry ; Composite number ; Brønsted–Lowry acid–base theory ; Infrared spectroscopy ; Nuclear magnetic resonance spectroscopy ; Spectroscopy ; Solid-state nuclear magnetic resonance ; Materials science ; Composite material ; Nuclear magnetic resonance ; Catalysis ; Organic chemistry Zeolite Catalysis and Synthesis ; Advanced NMR Techniques and Applications ; Clay minerals and soil interactions
Authors: Shihao Cui | Dejian Xu | Zhiyuan Wang | Libo Wang | Yikun Zhao | Wei Deng | Qingshan Zhao | Mingbo Wu
Source: Nanomaterials (article, 2024-10-22)
Field: Chemistry — Organic Chemistry

Pd Nanoparticles Immobilized on Pyridinic N-Rich Carbon Nanosheets for Promoting Suzuki Cross-Coupling Reactions Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h<sup>-1</sup> for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h<sup>-1</sup> even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds. Nanoparticle ; Suzuki reaction ; Chemical engineering ; Coupling (piping) ; Chemistry ; Carbon fibers ; Materials science ; Nanotechnology ; Catalysis ; Organic chemistry ; Palladium ; Metallurgy ; Composite number ; Composite material ; Engineering Catalytic Cross-Coupling Reactions ; Polyoxometalates: Synthesis and Applications ; Catalytic C–H Functionalization Methods