jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: María Pilar de Lara‐Castells
Source: Small Structures (article, 2024-06-30)
Field: Materials Science — Materials Chemistry

An Ab Initio Journey toward the Molecular‐Level Understanding and Predictability of Subnanometric Metal Clusters Current advances in synthesizing and characterizing atomically precise monodisperse metal clusters (AMCs) at the subnanometer scale have opened up new possibilities in quantum materials research. Their quantizied “molecule‐like” electronic structure showcases unique stability, and physical and chemical properties differentiate them from larger nanoparticles. When integrated into inorganic materials that interact with the environment and sunlight, AMCs serve to enhance their (photo)catalytic activity and optoelectronic properties. Their tiny size makes AMCs isolated in the gas phase amenable to atom‐scale modeling using either density functional theory (DFT) or methods at a high level of ab initio theory, even addressing nonadiabatic (e.g., Jahn–Teller) effects. Surface‐supported AMCs can be routinely modeled using DFT, enabling long real‐time molecular dynamics simulations. Their optical properties can also be addressed using time‐dependent DFT or reduced density matrix (RDM) theory. These theoretical–computational efforts aim to achieve predictability and molecular‐level understanding of the stability and properties of AMCs as function of their composition, size, and structural fluxionality in different thermodynamical conditions (temperature and pressure). In this perspective, the potential of ab initio and DFT‐based modeling is illustrated through recent studies of unsupported and surface‐supported AMCs. Future directions of research are also discussed, including applications and methodological enhancements beyond the state‐of‐the‐art. Predictability ; Ab initio ; Metal ; Chemistry ; Chemical physics ; Computational chemistry ; Materials science ; Physics ; Organic chemistry ; Quantum mechanics Nanocluster Synthesis and Applications ; Machine Learning in Materials Science ; Molecular Junctions and Nanostructures
Authors: Zhen Li | Ana Arauzo | Claudio Roscini | José Giner Planas | Elena Bartolomé
Source: Journal of Materials Chemistry A (article, 2024-01-01)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Multifunctional self-refrigerated multivariate {GdLn} (Ln = Dy, Tb, Tb/Eu) metal–organic frameworks "Self-refrigerated" multifunctional MOFs combine Gd for optimal magnetocalorics with other lanthanides (Dy, Tb, Eu) as single-molecule magnets and/or luminescent units, offering exciting possibilities for information storage and processing. Lanthanide ; Metal-organic framework ; Luminescence ; Materials science ; Magnet ; Nanotechnology ; Chemistry ; Physical chemistry ; Optoelectronics ; Mechanical engineering ; Organic chemistry ; Engineering ; Adsorption Magnetism in coordination complexes ; Metal-Organic Frameworks: Synthesis and Applications ; Lanthanide and Transition Metal Complexes
Authors: Yaned Milena Correa-Navarro | Juan David Rivera | Julio Andrés Cardona-Castaño
Source: ACS Omega (article, 2024-07-04)
Field: Materials Science — Biomaterials

Modified Cellulose for Adsorption of Methylparaben and Butylparaben from an Aqueous Solution Emerging contaminants are chemical products that are found in low concentrations, are not regulated by environmental norms, and cause health effects. Among this group of contaminants are parabens, a family of <i>p</i>-hydroxybenzoic acid esters used as preservatives in cosmetics, pharmaceuticals, and food products. Recent research describes parabens as endocrine disruptors that can cause health alterations. Some of the best alternatives for pollutant removal include the adsorption process, which can use materials that are inexpensive, abundant, and susceptible to modifications. In this sense, cellulose can be an option for obtaining materials that can be used in the removal of contaminants. This research investigates the synthesis of benzoic cellulose (MCB) and magnetic cellulose (MCM) as well as its use as an adsorbent for the removal of methylparaben (MP) and butylparaben (BP) from water. Likewise, physicochemical characterization, including Fourier transform infrared (FTIR), scanning electronic microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray diffraction (XRD), and thermogravimetric analysis (TGA), for both cellulose materials was carried out. Moreover, pseudo-first-order, pseudo-second-order, Elovich, Weber, Morris, and Boyd models were used to investigate the adsorption kinetics. As a result, the pseudo-second-order model was favorable for both modified cellulose and the two parabens assayed. Finally, Freundlich, Langmuir, and Sips adsorption isotherm models were investigated; the Langmuir model was the best for the adsorption isotherm data. The adsorption of methylparaben and butylparaben was in the following order: MCM > MCB. The maximum adsorption capacity of MP and BP for MCM was 9.58 and 12.03 mg g<sup>-1</sup>, respectively. For instance, the results showed that the modified cellulose adsorbed the parabens physically, which could involve electrostatic attraction, hydrogen bonding, π-π bonding, and hydrophobic interactions. Methylparaben ; Freundlich equation ; Adsorption ; Chemistry ; Cellulose ; Thermogravimetric analysis ; Langmuir ; Aqueous solution ; Nuclear chemistry ; Fourier transform infrared spectroscopy ; Organic chemistry ; Chemical engineering ; Chromatography ; Preservative Advanced Cellulose Research Studies ; Electrospun Nanofibers in Biomedical Applications ; Adsorption and biosorption for pollutant removal
Authors: Wonyeong Jung | Dohyung Kim | Seung Hwan Ko
Source: International Journal of Precision Engineering and Manufacturing-Green Technology (article, 2024-04-20)
Field: Chemistry — Spectroscopy

Recent Progress in High-Efficiency Transparent Vacuum Insulation Technologies for Carbon Neutrality Abstract Enhancing energy efficiency in buildings is a pivotal strategy for reducing energy consumption and mitigating greenhouse gas emissions. As part of global efforts to achieve carbon neutrality by 2050, there is a heightened focus on improving window insulation because windows are a significant source of thermal loss, representing nearly 40% of a building's heat dissipation. This study explores the development and application of vacuum insulation glazing (VIG), a cutting-edge insulation technology, to substantially reduce heat transfer through windows, thereby contributing to building energy savings. With its superior insulation performance, achieving thermal transmittance levels around 0.5W/m 2 ·K, VIG technology presents a promising advancement over traditional double-glazed or gas-filled insulating glass units (IGUs). However, the adoption of VIG is challenged by economic factors, with costs significantly higher than standard IGUs and triple-glazed windows meeting passive house standards. The production of VIG, characterized by lengthy evacuation times and high processing temperatures, contributes to its elevated price. This research identifies the potential for cost reduction through optimizing manufacturing processes, including using low-melting-point solders for hermetic sealing and localized heating techniques to shorten production times. Despite the high initial cost, the potential for integrating VIG with other smart technologies suggests a promising future for achieving carbon neutrality in buildings. The study calls for further research and standardization in VIG production to overcome current technical and economic barriers, paving the way for its wider adoption and realizing next-generation energy-efficient building materials. Carbon neutrality ; Neutrality ; Engineering physics ; Materials science ; Carbon fibers ; Nanotechnology ; Optoelectronics ; Electrical engineering ; Engineering ; Composite material ; Political science ; Renewable energy Aerogels and thermal insulation ; High voltage insulation and dielectric phenomena ; Surface Modification and Superhydrophobicity
Authors: Javier Emilio Alfonso Ramos | Rebecca M. Neeser | Thijs Stuyver
Source: Digital Discovery (article, 2024-01-01)
Field: Materials Science — Materials Chemistry

Repurposing quantum chemical descriptor datasets for on-the-fly generation of informative reaction representations: application to hydrogen atom transfer reactions In this work, we explore how existing datasets of quantum chemical properties can be repurposed to build data-efficient downstream ML models, with a particular focus on predicting the activation energy of hydrogen atom transfer reactions. Hydrogen atom ; Quantum chemical ; Repurposing ; Computer science ; Focus (optics) ; Atom (system on chip) ; Quantum ; On the fly ; Work (physics) ; Transfer (computing) ; Hydrogen ; Chemical reaction ; Chemistry ; Biological system ; Molecule ; Physics ; Thermodynamics ; Quantum mechanics ; Engineering ; Organic chemistry ; Biology Machine Learning in Materials Science ; Computational Drug Discovery Methods ; Metabolomics and Mass Spectrometry Studies
Authors: Yandong Sun | Yupeng Ma | Jinyu Zhang | Tian‐Ran Wei | Xun Shi | David Rodney | Ben Xu
Source: Science Advances (article, 2024-10-18)
Field: Materials Science — Materials Chemistry

Van der Waals semiconductor InSe plastifies by martensitic transformation Inorganic semiconductor materials are crucial for modern technologies, but their brittleness and limited processability hinder the development of flexible, wearable, and miniaturized electronics. The recent discovery of room-temperature plasticity in some inorganic semiconductors offers a promising solution, but the deformation mechanisms remain controversial. Here, we investigate the deformation of indium selenide, a two-dimensional van der Waals semiconductor with substantial plasticity. By developing a machine-learned deep potential, we perform atomistic simulations that capture the deformation features of hexagonal indium selenide upon out-of-plane compression. Unexpectedly, we find that indium selenide plastifies through a martensitic transformation; that is, the layered hexagonal structure is converted to a tetragonal lattice with specific orientation relationship. This observation is corroborated by high-resolution experimental observations and theory. It suggests a change of paradigm, where the design of new plastically deformable inorganic semiconductors can focus on compositions and structures that facilitate phase transformations, going beyond the conventional dislocation slip. Semiconductor ; Indium ; Materials science ; Selenide ; Tetragonal crystal system ; van der Waals force ; Nanotechnology ; Engineering physics ; Condensed matter physics ; Optoelectronics ; Crystallography ; Crystal structure ; Chemistry ; Metallurgy ; Physics 2D Materials and Applications ; MXene and MAX Phase Materials ; Machine Learning in Materials Science
Authors: Ditte Røjkjær Rasmussen | Nina Lock | Jonathan Quinson
Source: ChemSusChem (article, 2024-09-30)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Lights on the Synthesis of Surfactant‐Free Colloidal Gold Nanoparticles in Alkaline Mixtures of Alcohols and Water Surfactant-free colloidal syntheses in aqueous media are attractive to develop nanomaterials relevant for various applications, e. g. catalysis or medicine. However, controlled green syntheses without surfactants of metal nanoparticles in aqueous media remain scarce. Here, room temperature syntheses of gold (Au) nanoparticles (NPs) that require only HAuCl<sub>4</sub>, alkaline water and an alcohol, i. e. relatively benign chemicals and mild reaction conditions, are developed. The findings of a comprehensive multi-parameters screening performed in small volumes (<3 mL) over 1000+ experiments pave the way to greener high throughput screenings of large parametric spaces and lead to scalable (100 mL) synthetic strategies. A rational selection of the alcohol is proposed. The influence of lights with defined wavelengths (222-690 nm) is investigated. It is found that lights with lower wavelengths favor the formation of smaller 5 nm NPs. Different kinetics and formation pathways are observed for different alcohols and for lights with different wavelengths. The sensitivity to various experimental parameters increases with the alcohol used in the order glycerol<ethylene glycol<ethanol<methanol. New strategies for a rational fine size control, and to some extend shape control, are identified. The results lead to more sustainable and reproducible surfactant-free colloidal syntheses of NPs. Pulmonary surfactant ; Colloid ; Colloidal gold ; Nanoparticle ; Chemistry ; Chemical engineering ; Gold Colloid ; Colloidal particle ; Nanotechnology ; Organic chemistry ; Materials science Gold and Silver Nanoparticles Synthesis and Applications ; Nanoparticles: synthesis and applications ; Nanomaterials for catalytic reactions
Authors: David Naranjo | Sofia Paulo‐Mirasol | Sonia Lanzalaco | Haoyuan Quan | Elaine Armelín | José García‐Torres | Juan Torras
Source: Chemistry of Materials (article, 2024-04-17)
Field: Materials Science — Polymers and Plastics

Exploring the Effects and Interactions of Conducting Polymers in the Volume Phase Transition of Thermosensitive Conducting Hydrogels Conducting polymers (CPs) play a vital role in imparting electrochemical and photothermal properties to thermosensitive conducting hydrogels (TCH). The application of TCH is expanding not only for biomedical applications but also to address water scarcity. While the volume phase transition (VPT) phenomenon in thermosensitive polymers has been extensively studied, the contribution of CPs to this process and the underlying chemical interactions remain unclear and low explored. In this study, we present a novel conducting polymer hydrogel (CPH) utilizing the thermosensitive polymer poly-(<i>N</i>-isopropylacrylamide) (PNIPAAm) enriched with poly-(3,4-ethylenedioxythiophene) (PEDOT) nanoparticles as a model system. This serves as a platform for both experimental and theoretical investigations into the influence of CPs on VPT. Through a comprehensive examination of hydrogel responses to temperature employing Raman spectroscopy, atomistic simulations using advanced hybrid methodologies, and artificial intelligence, we unveil a shielding effect of CP. This effect arises from robust chemical interactions with NIPAAm, inducing a selective dehydration of the hydrogel microenvironment. Remarkably, this mirrors the phenomenon observed during VPT triggered by an increase in the hydrogel temperature. Understanding the intricate interactions between conducting and thermosensitive polymers is imperative for the systematic development and fine-tuning of the performance of future CPHs. This knowledge ensures a more precise adaptation of these materials to their intended end applications. Self-healing hydrogels ; Materials science ; Polymer ; PEDOT:PSS ; Nanotechnology ; Conductive polymer ; Phase transition ; Poly(N-isopropylacrylamide) ; Chemical engineering ; Polymer chemistry ; Thermodynamics ; Composite material ; Physics Conducting polymers and applications ; Advanced Sensor and Energy Harvesting Materials ; Hydrogels: synthesis, properties, applications
Authors: A.J. Cornet | A.M. Homborg | Prasaanth Ravi Anusuyadevi | L. 't Hoen-Velterop | J.M.C. Mol
Source: Engineering Failure Analysis (article, 2024-02-07)
Field: Materials Science — Materials Chemistry

Unravelling corrosion degradation of aged aircraft components protected by chromate-based coatings Despite extensive research, eliminating hexavalent chromium-based inhibitors from aerospace coatings remains challenging due to a lack of understanding of coating degradation during aircraft service. This study addresses the issue by investigating the protective mechanisms and aging processes of chromate-containing coatings on aircraft components after service for over 35 years. Four aircraft parts underwent visual inspection, disassembly, and analysis using scanning electron microscopy (SEM) and X-ray Photoelectron Spectroscopy (XPS). While most coating areas remained intact after extended use, three distinct degradation modes were identified: tip erosion, corrosion around rivets, and corrosion around fasteners at the leading edge. These findings reveal the complexity of corrosion protection, emphasizing that hexavalent chromium-containing coatings may not offer comprehensive protection at local design heterogeneities. The study also highlights the need to revisit traditional laboratory analysis protocols based on accelerated corrosion testing of oversimplified sample configurations, given the revealed end-of-service failure mechanisms. Chromate conversion coating ; Corrosion ; Hexavalent chromium ; Materials science ; Coating ; Degradation (telecommunications) ; Aerospace ; Scanning electron microscope ; Metallurgy ; Conversion coating ; Service life ; X-ray photoelectron spectroscopy ; Rivet ; Forensic engineering ; Cathodic protection ; Chromium ; Composite material ; Engineering ; Chemical engineering ; Chemistry ; Aerospace engineering Corrosion Behavior and Inhibition ; Hydrogen embrittlement and corrosion behaviors in metals ; Concrete Corrosion and Durability
Authors: Lu Chen | Xuze Guan | Xinbang Wu | Hiroyuki Asakura | David G. Hopkinson | Christopher S. Allen | June Callison | Paul J. Dyson | Feng Ryan Wang
Source: Proceedings of the National Academy of Sciences (article, 2024-07-23)
Field: Materials Science — Materials Chemistry

Thermally stable high-loading single Cu sites on ZSM-5 for selective catalytic oxidation of NH <sub>3</sub> Rigorous comparisons between single site- and nanoparticle (NP)-dispersed catalysts featuring the same composition, in terms of activity, selectivity, and reaction mechanism, are limited. This limitation is partly due to the tendency of single metal atoms to sinter into aggregated NPs at high loadings and elevated temperatures, driven by a decrease in metal surface free energy. Here, we have developed a unique two-step method for the synthesis of single Cu sites on ZSM-5 (termed Cu<sub>S</sub>/ZSM-5) with high thermal stability. The atomic-level dispersion of single Cu sites was confirmed through scanning transmission electron microscopy, X-ray absorption fine structure (XAFS), and electron paramagnetic resonance spectroscopy. The Cu<sub>S</sub>/ZSM-5 catalyst was compared to a CuO NP-based catalyst (termed Cu<sub>N</sub>/ZSM-5) in the oxidation of NH<sub>3</sub> to N<sub>2</sub>, with the former exhibiting superior activity and selectivity. Furthermore, operando XAFS and diffuse reflectance infrared Fourier transform spectroscopy studies were conducted to simultaneously assess the fate of the Cu and the surface adsorbates, providing a comprehensive understanding of the mechanism of the two catalysts. The study shows that the facile redox behavior exhibited by single Cu sites correlates with the enhanced activity observed for the Cu<sub>S</sub>/ZSM-5 catalyst. Catalysis ; Selectivity ; X-ray absorption fine structure ; ZSM-5 ; Electron paramagnetic resonance ; Dispersion (optics) ; Diffuse reflectance infrared fourier transform ; Redox ; Fourier transform infrared spectroscopy ; Scanning electron microscope ; Metal ; Thermal stability ; Chemistry ; Diffuse reflection ; Spectroscopy ; Copper ; Infrared spectroscopy ; Absorption (acoustics) ; Inorganic chemistry ; Materials science ; Chemical engineering ; Molecular sieve ; Nuclear magnetic resonance ; Photocatalysis ; Organic chemistry Catalytic Processes in Materials Science ; Advanced Photocatalysis Techniques ; Nanomaterials for catalytic reactions
Authors: Bidyut Bikash Sarma | Dominik Neukum | Dmitry E. Doronkin | Ajai Raj Lakshmi Nilayam | Lorena Baumgarten | B. Krause | Jan‐Dierk Grunwaldt
Source: Chemical Science (article, 2024-01-01)
Field: Materials Science — Materials Chemistry

Understanding the role of supported Rh atoms and clusters during hydroformylation and CO hydrogenation reactions with <i>in situ</i>/<i>operando</i> XAS and DRIFT spectroscopy Supported Rh single-atoms and clusters on CeO<sub>2</sub>, MgO, and ZrO<sub>2</sub> were investigated as catalysts for hydroformylation of ethylene to propionaldehyde and CO hydrogenation to methanol/ethanol with <i>in situ</i>/<i>operando</i> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray absorption spectroscopy (XAS). Under hydroformylation reaction conditions, <i>operando</i> spectroscopic investigations unravel the presence of both single atoms and clusters and detected at first propanal and then methanol. We find that the formation of methanol is associated with CO hydrogenation over Rh clusters which was further confirmed under CO hydrogenation conditions at elevated pressure. The activity of catalysts synthesized <i>via</i> a precipitation (PP) method over various supports towards the hydroformylation reaction follows the order: Rh/ZrO<sub>2</sub> > Rh/CeO<sub>2</sub> > Rh/MgO. Comparing Rh/CeO<sub>2</sub> catalysts synthesized <i>via</i> different methods, catalysts prepared by flame spray pyrolysis (FSP) showed catalytic activity for the hydroformylation reaction at lower temperatures (413 K), whereas catalysts prepared by wet impregnation (WI) showed the highest stability. These results not only provide fundamental insights into the atomistic level of industrially relevant reactions but also pave the way for a rational design of new catalysts in the future. Hydroformylation ; X-ray absorption spectroscopy ; In situ ; Rhodium ; Catalysis ; Spectroscopy ; Chemistry ; Absorption spectroscopy ; Photochemistry ; Organic chemistry ; Physics Catalytic Processes in Materials Science ; Catalysts for Methane Reforming ; Catalysis and Hydrodesulfurization Studies
Authors: Ankit K. Yadav | Andrzej Gładysiak | Ah‐Young Song | Lei Gan | Casey R. Simons | Nawal M. Alghoraibi | Ammar Alahmed | Mourad Younes | Jeffrey A. Reimer | Hongliang Huang | José Giner Planas | Kyriakos C. Stylianou
Source: JACS Au (article, 2024-12-03)
Field: Chemistry — Inorganic Chemistry

Sequential Pore Functionalization in MOFs for Enhanced Carbon Dioxide Capture The capture of carbon dioxide (CO<sub>2</sub>) is crucial for reducing greenhouse emissions and achieving net-zero emission goals. Metal-organic frameworks (MOFs) present a promising solution for carbon capture due to their structural adaptability, tunability, porosity, and pore modification. In this research, we explored the use of a copper (Cu(II))-based MOF called <i>m</i> <b>CBMOF-1</b>. After activation, <i>m</i> <b>CBMOF-1</b> generates one-dimensional channels with square cross sections, featuring sets of four Cu(II) open metal sites spaced by 6.042 Å, allowing strong interactions with coordinating molecules. To investigate this capability, <i>m</i> <b>CBMOF-1</b> was exposed to ammonia (NH<sub>3</sub>) gas, resulting in hysteretic NH<sub>3</sub> isotherms indicative of strong interactions between Cu(II) and NH<sub>3</sub>. At 150 mbar and 298 K, the NH<sub>3</sub>-loaded (∼1 mmol/g) material exhibited a 106% increase in CO<sub>2</sub> uptake compared to that of the pristine <i>m</i> <b>CBMOF-1</b>. Carbon-13 solid-state nuclear magnetic resonance spectra and density functional theory calculations confirmed that the sequential loading of NH<sub>3</sub> followed by CO<sub>2</sub> adsorption generated a copper-carbamic acid complex within the pores of <i>m</i> <b>CBMOF-1</b>. Our study highlights the effectiveness of sequential pore functionalization in MOFs as an attractive strategy for enhancing the interactions of MOFs with small molecules such as CO<sub>2</sub>. Surface modification ; Carbon dioxide ; Chemical engineering ; Materials science ; Nanotechnology ; Chemistry ; Organic chemistry ; Engineering Metal-Organic Frameworks: Synthesis and Applications ; Carbon Dioxide Capture Technologies ; Gas Sensing Nanomaterials and Sensors