jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Roman Guntermann | David Helminger | Laura Frey | Peter M. Zehetmaier | Christian Wangnick | Apeksha Singh | Tianhao Xue | Dana D. Medina | Thomas Bein
Source: Angewandte Chemie International Edition (article, 2024-08-14)
Field: Materials Science — Materials Chemistry

Tunable Isometric Donor‐Acceptor Wurster‐Type Covalent Organic Framework Photocathodes Covalent organic frameworks (COFs) offer remarkable versatility, combining ordered structures, high porosity, and tailorable functionalities in nanoscale reaction spaces. Herein, we report the synthesis of a series of isostructural, photoactive Wurster-type COFs achieved by manipulating the chemical and electronic nature of the Wurster aromatic amine building blocks. A series of donor-acceptor-donor (D-A-D) Wurster building block molecules was synthesized by incorporating heteroaromatic acceptors with varying strengths between triphenylamine donor groups. These tailored building blocks were integrated into a 2D COF scaffold, resulting in highly crystalline structures and similar morphologies across all COFs. Remarkably, this structural uniformity was also achieved in the synthesis of homogeneous and oriented thin films. Steady-state photoluminescence revealed a tunable red-shift in film emission exceeding 100 nm, demonstrating effective manipulation of their optical properties. Furthermore, photoelectrochemical (PEC) water splitting studies exhibited a doubled current density (8.1 μA cm<sup>-2</sup> at 0.2 V<sub>RHE</sub>) for the COF with the strongest acceptor unit. These findings highlight the potential of Wurster D-A-D COFs in photoelectrochemical water splitting devices and pave the way for further exploration of chemical functionality-reactivity-property relationships in this promising class of photoactive materials. Triphenylamine ; Isostructural ; Materials science ; Acceptor ; Covalent bond ; Molecule ; Photoluminescence ; Photochemistry ; Nanotechnology ; Chemistry ; Optoelectronics ; Crystal structure ; Crystallography ; Organic chemistry Covalent Organic Framework Applications ; Advanced Photocatalysis Techniques ; Metal-Organic Frameworks: Synthesis and Applications
Authors: Ana Yañez-Aulestia | Víctor M. Trejos | J. Marcos Esparza-Schulz | Ilich A. Ibarra | Elı́ Sánchez-González
Source: ACS Applied Materials & Interfaces (article, 2024-11-12)
Field: Chemistry — Inorganic Chemistry

Chemically Modified HKUST-1(Cu) for Gas Adsorption and Separation: Mixed-Metal and Hierarchical Porosity The archetypical metal-organic framework (MOF), HKUST-1, has been systematically modified in both its organic and inorganic building blocks to introduce diversity in the metal centers and create defects within the network, achieving a variety of bimetallic hierarchical structures. These modifications changed the affinity of the MOFs for acid gases. The introduction of bimetallic sites mostly affects CO<sub>2</sub> adsorption, while the hierarchical structure generates an increase in SO<sub>2</sub> uptake capacity, allowing better performance in the separation of binary mixtures of these gases near room temperature. Notably, the synthesized HH-Cu<sub>100</sub> material exhibited an exceptionally high IAST SO<sub>2</sub>/CO<sub>2</sub> (10:90) selectivity of 3420 at 298 K, outperforming benchmark MOFs with open metal sites. Materials science ; Porosity ; Adsorption ; Gas separation ; Chemical engineering ; Separation (statistics) ; Metal ; Composite material ; Metallurgy ; Membrane ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; Catalytic Processes in Materials Science ; Mesoporous Materials and Catalysis
Authors: Mohammad Jaber | Yasemin Ozbay | Emmanuel Chefdeville | Gaël Tran | Abderrahmane Amgoune
Source: ACS Catalysis (article, 2024-08-09)
Field: Chemistry — Organic Chemistry

Unified Photocatalytic Strategy for the Cross-Coupling of Alcohols with Aryl Halides Enabled by Synergistic Nickel and Iron LMCT Catalysis The use of alcohol feedstock as a coupling partner in cross-coupling reactions offers an extraordinary potential for the efficient synthesis of Csp3-rich complex molecular scaffolds. This prominent strategy relies on the generation of alkoxy radicals, which can react via various radical pathways to give carbon-centered radicals that can be engaged in C–C bond formation reactions. However, cross-coupling reactions involving catalytic generation of alkoxy radicals directly from native alcohols are highly challenging and the scope of existing catalytic methods remains particularly limited. Moreover, a unified strategy that can incorporate a broad range of alcohols in catalytic cross-coupling with aryl halides is currently unavailable. Herein, we report a general photocatalytic platform that combines nickel and iron ligand-to-metal charge transfer (LMCT) catalysis for the selective deconstructive Csp3–Csp3 bond cleavage and arylation of various unactivated alcohols. This protocol leverages the ability of photoinduced iron LMCT catalysis to generate radicals from diversely substituted alcohols, enabling implementation of various C–C bond-forming manifolds. These include dehydroxymethylative arylation of aliphatic alcohols, remote arylation of cyclic alcohols to yield alkyl ketones, and the methylation of aryl halides using tertiary alcohols as the methyl radical source. This methodology offers a practical and unified strategy for engaging a large variety of commercially available alcohols in cross-coupling reactions under mild conditions, using abundant nickel and iron catalysts. Mechanistic studies, including stoichiometric organometallic chemistry and cyclic voltammetry, provide insights into the crucial role of the ancillary ligand surrounding the iron catalyst in stabilizing both low- and high-valent iron catalytic intermediates. Chemistry ; Aryl ; Catalysis ; Radical ; Combinatorial chemistry ; Coupling reaction ; Nickel ; Alkoxy group ; Ligand (biochemistry) ; Photocatalysis ; Photochemistry ; Organic chemistry ; Alkyl Radical Photochemical Reactions ; Catalytic C–H Functionalization Methods ; Sulfur-Based Synthesis Techniques
Authors: Naznin Sultana | A.P. Cole | Francine Strachan
Source: Materials (review, 2024-11-15)
Field: Materials Science — Biomaterials

Biocomposite Scaffolds for Tissue Engineering: Materials, Fabrication Techniques and Future Directions Tissue engineering is an interdisciplinary field that combines materials, methods, and biological molecules to engineer newly formed tissues to replace or restore functional organs. Biomaterials-based scaffolds play a crucial role in developing new tissue by interacting with human cells. Tissue engineering scaffolds with ideal characteristics, namely, nontoxicity, biodegradability, and appropriate mechanical and surface properties, are vital for tissue regeneration applications. However, current biocomposite scaffolds face significant limitations, particularly in achieving structural durability, controlled degradation rates, and effective cellular integration. These qualities are essential for maintaining long-term functionality in vivo. Although commonly utilized biomaterials can provide physical and chemical properties needed for tissue regeneration, inadequate biomimetic properties, as well as insufficient interactions of cells-scaffolds interaction, still need to be improved for the application of tissue engineering in vivo. It is impossible to achieve some essential features using a single material, so combining two or more materials may accomplish the requirements. In order to achieve a proper scaffold design, a suitable fabrication technique and combination of biomaterials with controlled micro or nanostructures are needed to achieve the proper biological responses. This review emphasizes advancements in scaffold durability, biocompatibility, and cellular responsiveness. It focuses on natural and synthetic polymer combinations and innovative fabrication techniques. Developing stimulus-responsive 3D scaffolds is critical, as these scaffolds enhance cell adhesion and promote functional tissue formation while maintaining structural integrity over time. This review also highlights the natural polymers, smart materials, and recent advanced techniques currently used to create emerging scaffolds for tissue regeneration applications. Tissue engineering ; Scaffold ; Nanotechnology ; Materials science ; Biocomposite ; Regeneration (biology) ; Biocompatibility ; Biomedical engineering ; Engineering Electrospun Nanofibers in Biomedical Applications ; Bone Tissue Engineering Materials ; Graphene and Nanomaterials Applications
Authors: Geethu Venugopal | V. Ravi Kumar | Ashok Badrinarayan Jadhav | Sangram D. Dongre | Abujunaid Habib Khan | Rajesh G. Gonnade | Jatish Kumar | Sukumaran Santhosh Babu
Source: Chemistry - A European Journal (article, 2024-01-25)
Field: Chemistry — Organic Chemistry

Boron‐ and Oxygen‐Doped π‐Extended Helical Nanographene with Circularly Polarised Thermally Activated Delayed Fluorescence Helical nanographenes have garnered substantial attention owing to their finely adjustable optical and semiconducting properties. The strategic integration of both helicity and heteroatoms into the nanographene structure, facilitated by a boron-oxygen-based multiple resonance (MR) thermally activated delayed fluorescence (TADF), elevates its photophysical and chiroptical features. This signifies the introduction of an elegant category of helical nanographene that combines optical (TADF) and chiroptical (CPL) features. In this direction, we report the synthesis, optical, and chiroptical properties of boron, oxygen-doped Π-extended helical nanographene. The π-extension induces distortion in the DOBNA-incorporated nanographene, endowing a pair of helicenes, (P)-B2NG, and (M)-B2NG exhibiting circularly polarized luminescence with g<sub>lum</sub> of -2.3×10<sup>-3</sup> and +2.5×10<sup>-3</sup>, respectively. B2NG exhibited MR-TADF with a lifetime below 5 μs, and a reasonably high fluorescence quantum yield (50 %). Our molecular design enriches the optical and chiroptical properties of nanographenes and opens up new opportunities in multidisciplinary fields. Materials science ; Fluorescence ; Quantum yield ; Boron ; Luminescence ; Circular dichroism ; Heteroatom ; Helicity ; Doping ; Photochemistry ; Crystallography ; Nanotechnology ; Optoelectronics ; Chemistry ; Optics ; Physics Synthesis and Properties of Aromatic Compounds ; Luminescence and Fluorescent Materials ; Organic Electronics and Photovoltaics
Authors: Mahmoud A.S. Sakr | Hazem Abdelsalam | Nahed H. Teleb | Omar H. Abd‐Elkader | Qinfang Zhang
Source: Scientific Reports (article, 2024-02-29)
Field: Materials Science — Materials Chemistry

Exploring the structural, electronic, and hydrogen storage properties of hexagonal boron nitride and carbon nanotubes: insights from single-walled to doped double-walled configurations This study investigates the structural intricacies and properties of single-walled nanotubes (SWNT) and double-walled nanotubes (DWNT) composed of hexagonal boron nitride (BN) and carbon (C). Doping with various atoms including light elements (B, N, O) and heavy metals (Fe, Co, Cu) is taken into account. The optimized configurations of SWNT and DWNT, along with dopant positions, are explored, with a focus on DWNT-BN-C. The stability analysis, employing binding energies, affirms the favorable formation of nanotube structures, with DWNT-C emerging as the most stable compound. Quantum stability assessments reveal significant intramolecular charge transfer in specific configurations. Electronic properties, including charge distribution, electronegativity, and electrical conductivity, are examined, showcasing the impact of doping. Energy gap values highlight the diverse electronic characteristics of the nanotubes. PDOS analysis provides insights into the contribution of atoms to molecular orbitals. UV-Vis absorption spectra unravel the optical transitions, showcasing the influence of nanotube size, dopant type, and location. Hydrogen storage capabilities are explored, with suitable adsorption energies indicating favorable hydrogen adsorption. The desorption temperatures for hydrogen release vary across configurations, with notable enhancements in specific doped DWNT-C variants, suggesting potential applications in high-temperature hydrogen release. Overall, this comprehensive investigation provides valuable insights into the structural, electronic, optical, and hydrogen storage properties of BN and C nanotubes, laying the foundation for tailored applications in electronics and energy storage. Materials science ; Hydrogen storage ; Carbon nanotube ; Dopant ; Nanotube ; Nanotechnology ; Doping ; Optical properties of carbon nanotubes ; Electronegativity ; Electronic structure ; Selective chemistry of single-walled nanotubes ; Hydrogen ; Chemical physics ; Computational chemistry ; Optoelectronics ; Chemistry Boron and Carbon Nanomaterials Research ; Graphene research and applications ; Advancements in Battery Materials
Authors: Hua An | Yani Ding | Philippe Sautet | Geng Sun | Ning Yan
Source: Journal of the American Chemical Society (article, 2024-10-21)
Field: Chemistry — Organic Chemistry

Selective Reduction of Nitroarenes via Noncontact Hydrogenation In traditional hydrogenation, where H<sub>2</sub> and substrates with unsaturated bonds are activated on the same catalyst (contact mode), competitive hydrogenation of multiple reducible groups often occurs. We employ an unbiased H-cell for selective hydrogenation of the nitro group when multiple reducible groups are present. The setup spatially separates H<sub>2</sub> and nitroarenes into two chambers connected by a proton-exchange membrane, thus adding barriers for a Langmuir-Hinshelwood-type mechanism that is common in thermocatalytic hydrogenation. Through a unique proton/electron transfer pathway that is specific to nitro functional group reduction to hydroxylamine, side reactions like C═C, C═O, and C≡C bond hydrogenation are fully avoided. Using Pd/C for H<sub>2</sub> activation, and CNT for selective proton/electron transfer to -NO<sub>2</sub> groups while being inert to C≡C, C═C, and C═O hydrogenation, the system effectively eliminates the competitive hydrogenation, achieving 100% nitro-group reduction selectivity in the hydrogenation of various nitroarenes, in sharp contrast to negligible selectivity over the same catalysts in a batch reactor under contact mode. This device enables selectivity control in hydrogenation reactions, moving beyond the traditional focus on catalyst active site engineering. Chemistry ; Reduction (mathematics) ; Selective reduction ; Organic chemistry ; Catalysis Nanomaterials for catalytic reactions ; Asymmetric Hydrogenation and Catalysis ; Innovative Microfluidic and Catalytic Techniques Innovation
Authors: Yifan Hu | Liangli Dai | Bolin Li | Zesheng Li
Source: Advanced Sustainable Systems (article, 2024-06-06)
Field: Chemistry — Inorganic Chemistry

Single‐Atom Long‐Range Interaction: Basic Principles and Applications Abstract Single‐atom catalysis involves loading the active metal onto the carrier's surface as a single‐atom. This atom is primarily bonded to the carrier surface through hetero‐atom bonding. It is important to note that the coordination environment of the metal atoms may not be the same when each dispersed active metal atom has an identical coordination environment on the carrier's surface. The utilization of single‐atom catalysts (SACs) doesn't strictly imply that a solitary metal atom with zero valency functions as the active core. Singular atoms can also engage in distant interactions with other atoms or clusters of atoms on the substrate, like electron transfer, and frequently demonstrate specific charges. The main reason for the high activity of the catalyst is the remote (i.e., long‐range) interaction of the active atom with the surrounding coordination atoms. For this reason, the study of the mechanism of long‐range interactions between multiple single‐atom sites and between single‐atom sites and atomic cluster sites has become an important and urgent task in the design and regulation of single‐atom catalyst performance. Range (aeronautics) ; Atom (system on chip) ; Computer science ; Materials science ; Embedded system Radioactive element chemistry and processing ; Electrocatalysts for Energy Conversion ; Machine Learning in Materials Science
Authors: Abir Das | Subramani Kumaran | Harihara Subramanian Ravi Sankar | J. Richard Premkumar | Basker Sundararaju
Source: Angewandte Chemie International Edition (article, 2024-06-19)
Field: Chemistry — Organic Chemistry

A Dual Cobalt‐Photoredox Catalytic Approach for Asymmetric Dearomatization of Indoles with Aryl Amides via C−H Activation In this study, we unveil a novel method for the asymmetric dearomatization of indoles under cobalt/photoredox catalysis. By strategically activating C-H bonds of amides and subsequent migratory insertion of π-bonds present in indole as reactive partner, we achieve syn-selective tetrahydro-5H-indolo[2,3-c]isoquinolin-5-one derivatives with excellent yields and enantiomeric excesses of up to >99 %. The developed method operates without a metal oxidant, relying solely on oxygen as the oxidant and employing an organic dye as a photocatalyst under irradiation. Control experiments and stoichiometric studies elucidate the reversible nature of the enantiodetermining C-H activation step, albeit not being rate-determining. This study not only expands the horizon of cobalt-catalyzed asymmetric C-H bond functionalization, but also showcases the potential synergy between cobalt and photoredox catalysis in enabling asymmetric synthesis of complex molecules. Cobalt ; Aryl ; Catalysis ; Dual (grammatical number) ; Chemistry ; Combinatorial chemistry ; Dual role ; Organic chemistry Catalytic C–H Functionalization Methods ; Oxidative Organic Chemistry Reactions ; Radical Photochemical Reactions
Authors: Ze-quan Wang | Xue Feng | Liang Qiu | Zhe Wang | Ruqian Wu | Yusheng Hou
Source: Nano Letters (preprint, 2024-03-20)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Switching Intrinsic Magnetic Skyrmions with Controllable Magnetic Anisotropy in van der Waals Multiferroic Heterostructures Magnetic skyrmions, topologically nontrivial whirling spin textures at nanometer scales, have emerged as potential information carriers for spintronic devices. The ability to efficiently create and erase magnetic skyrmions is vital yet challenging for such applications. Based on first-principles studies, we find that switching between intrinsic magnetic skyrmion and high-temperature ferromagnetic states can be achieved in the two-dimensional van der Waals (vdW) multiferroic heterostructure CrSeI/In<sub>2</sub>Te<sub>3</sub> by reversing the ferroelectric polarization of In<sub>2</sub>Te<sub>3</sub>. The core mechanism of this switching is traced to the controllable magnetic anisotropy of CrSeI influenced by the ferroelectric polarization of In<sub>2</sub>Te<sub>3</sub>. We propose a useful descriptor linking the presence of magnetic skyrmions to magnetic parameters and validate this connection through studies of a variety of similar vdW multiferroic heterostructures. Our work demonstrates that manipulating magnetic skyrmions via tunable magnetic anisotropies in vdW multiferroic heterostructures represents a highly promising and energy-efficient strategy for the future development of spintronics. Multiferroics ; Condensed matter physics ; Skyrmion ; van der Waals force ; Anisotropy ; Materials science ; Magnetic anisotropy ; Physics ; Magnetic field ; Magnetization ; Quantum mechanics ; Optoelectronics ; Ferroelectricity Multiferroics and related materials ; Advanced Materials and Mechanics ; Metamaterials and Metasurfaces Applications
Authors: Z.W. Li | Zhaosong Huang | Pengfei Gu
Source: Microorganisms (review, 2024-08-28)
Field: Chemistry — Physical and Theoretical Chemistry

Response of Escherichia coli to Acid Stress: Mechanisms and Applications—A Narrative Review Change in pH in growth conditions is the primary stress for most neutralophilic bacteria, including model microorganism <i>Escherichia coli</i>. However, different survival capacities under acid stress in different bacteria are ubiquitous. Research on different acid-tolerance mechanisms in microorganisms is important for the field of combating harmful gut bacteria and promoting fermentation performance of industrial strains. Therefore, this study aimed to carry out a narrative review of acid-stress response mechanism of <i>E. coli</i> discovered so far, including six AR systems, cell membrane protection, and macromolecular repair. In addition, the application of acid-tolerant <i>E. coli</i> in industry was illustrated, such as production of industrial organic acid and developing bioprocessing for industrial wastes. Identifying these aspects will open the opportunity for discussing development aspects for subsequent research of acid-tolerant mechanisms and application in <i>E. coli</i>. Escherichia coli ; Narrative ; Chemistry ; Microbiology ; Computational biology ; Biology ; Biochemistry ; Literature ; Art ; Gene thermodynamics and calorimetric analyses ; Microbial Metabolic Engineering and Bioproduction ; Bacterial Genetics and Biotechnology
Authors: Winnie S. Liang | Brett K. Beaulieu‐Jones | Susan L. Smalley | M Snyder | Laura H. Goetz | Nicholas J. Schork
Source: Frontiers in Pharmacology (review, 2024-03-13)
Field: Chemistry — Analytical Chemistry

Emerging therapeutic drug monitoring technologies: considerations and opportunities in precision medicine In recent years, the development of sensor and wearable technologies have led to their increased adoption in clinical and health monitoring settings. One area that is in early, but promising, stages of development is the use of biosensors for therapeutic drug monitoring (TDM). Traditionally, TDM could only be performed in certified laboratories and was used in specific scenarios to optimize drug dosage based on measurement of plasma/blood drug concentrations. Although TDM has been typically pursued in settings involving medications that are challenging to manage, the basic approach is useful for characterizing drug activity. TDM is based on the idea that there is likely a clear relationship between plasma/blood drug concentration (or concentration in other matrices) and clinical efficacy. However, these relationships may vary across individuals and may be affected by genetic factors, comorbidities, lifestyle, and diet. TDM technologies will be valuable for enabling precision medicine strategies to determine the clinical efficacy of drugs in individuals, as well as optimizing personalized dosing, especially since therapeutic windows may vary inter-individually. In this mini-review, we discuss emerging TDM technologies and their applications, and factors that influence TDM including drug interactions, polypharmacy, and supplement use. We also discuss how using TDM within single subject (N-of-1) and aggregated N-of-1 clinical trial designs provides opportunities to better capture drug response and activity at the individual level. Individualized TDM solutions have the potential to help optimize treatment selection and dosing regimens so that the right drug and right dose may be matched to the right person and in the right context. Therapeutic drug monitoring ; Dosing ; Medicine ; Precision medicine ; Personalized medicine ; Drug ; Polypharmacy ; Drug development ; Intensive care medicine ; Pharmacology ; Bioinformatics ; Biology Analytical Methods in Pharmaceuticals ; Attention Deficit Hyperactivity Disorder ; Pharmaceutical Practices and Patient Outcomes