jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Dan Lai | Fuqiang Chen | Lidong Guo | Lihang Chen | Jie Chen | Qiwei Yang | Zhiguo Zhang | Yiwen Yang | Qilong Ren | Zongbi Bao
Source: Engineering (article, 2023-02-20)
Field: Chemistry — Inorganic Chemistry

Guest Solvent-Directed Isomeric Metal–Organic Frameworks for the Kinetically Favorable Separation of Carbon Dioxide and Methane The adsorptive separation of CH4 from CO2 is a promising process for upgrading natural gas. However, thermodynamically selective adsorbents exhibit a strong affinity for CO2 and thus require a high energy compensation for regeneration. Instead, kinetic separation is preferred for a pressure swing adsorption process, although precise control of the aperture size to achieve a tremendous discrepancy in diffusion rates remains challenging. Here, we report a guest solvent-directed strategy for fine-tuning the pore size at a sub-angstrom precision to realize highly efficient kinetic separation. A series of metal–organic frameworks (MOFs) with isomeric pore surface chemistry were constructed from 4,4′-(hexafluoroisopropyli-dene)-bis(benzoic acid) and dicopper paddlewheel notes. The resultant CuFMOF·CH3OH (CuFMOF-c) exhibits an excellent kinetic separation performance thanks to a periodically expanding and contracting aperture with the ideal bottleneck size, which enables the effective trapping of CO2 and impedes the diffusion of CH4, offering an ultrahigh kinetic selectivity (273.5) and equilibrium-kinetic combined selectivity (64.2). Molecular dynamics calculations elucidate the separation mechanism, and breakthrough experiments validate the separation performance. Adsorption ; Chemistry ; Selectivity ; Methane ; Diffusion ; Kinetic energy ; Separation process ; Chemical engineering ; Gas separation ; Chemical physics ; Nanotechnology ; Materials science ; Physical chemistry ; Catalysis ; Organic chemistry ; Thermodynamics ; Chromatography ; Membrane Metal-Organic Frameworks: Synthesis and Applications ; Carbon Dioxide Capture Technologies ; Carbon dioxide utilization in catalysis
Authors: Anis H. Fakeeha | Dharmesh M. Vadodariya | Mohammed F. Alotibi | Jehad K. Abu‐Dahrieh | Ahmed A. Ibrahim | Ahmed E. Abasaeed | Naif Alarifi | Rawesh Kumar | Ahmed S. Al‐Fatesh
Source: Catalysts (article, 2023-10-18)
Field: Materials Science — Materials Chemistry

Pd+Al2O3-Supported Ni-Co Bimetallic Catalyst for H2 Production through Dry Reforming of Methane: Effect of Carbon Deposition over Active Sites Dry reforming of methane (DRM) is gaining global attention due to its capacity to convert two greenhouse gases together. It proceeds through CH4 decomposition over active sites (into CH4−x) followed by CH4−x oxidation by CO2 (into syngas). Furthermore, CH4−x oligomerization into coke cannot be neglected. Herein, xNi(5−x)Co/Pd+Al2O3 (x = 5, 3.75, 2.5, 1.25, 0) catalysts are prepared, investigated for DRM, and characterized with X-ray diffraction, UV-Vis, transmission electron microscopy, temperature-programmed reduction/desorption techniques, and thermogravimetry. Fine-tuning among stable active sites, graphitic carbon deposits, and catalytic activity is noticed. The total reducibility and basicity are found to decrease upon increasing the Co proportion up to 2.5 wt% in the Ni-Co bimetallic Pd+Al2O3-supported catalyst. The active sites derived from strong metal–support interaction species (NiAl2Ox or dispersed CoOx) are found to be promising in higher levels of activity. However, activity is, again, limited by graphitic carbon which is increased with an increasing Co proportion in the Ni-Co bimetallic Pd+Al2O3-supported catalyst. The incorporation of 1.25 wt% Co along with 3.75 wt% Ni over Pd+Al2O3 results in the generation of fewer such active sites, extensive oxidizable carbon deposits, and inferior catalytic activity compared to 5Ni/Pd+Al2O3. The 2.5Ni2.5Co/Pd+Al2O3 catalyst has lower crystallinity, a relatively lower coke deposit (than the 3.75Ni1.25Co/Pd+Al2O3 catalyst), and a higher number of stable active sites. It attains a 54–51% H2 yield in 430 min TOS and 0.87 H2/CO (similar to 5Ni/Pd+Al2O3) Bimetallic strip ; Catalysis ; Carbon dioxide reforming ; Methane ; Syngas ; Crystallinity ; Coke ; Carbon fibers ; Materials science ; Inorganic chemistry ; Chemical engineering ; Chemistry ; Metallurgy ; Organic chemistry ; Composite material Catalytic Processes in Materials Science ; Catalysts for Methane Reforming ; Catalysis and Oxidation Reactions
Authors: Rosangela Mastrangelo | Claudio Resta | Emiliano Carretti | Emiliano Fratini | Piero Baglioni
Source: ACS Applied Materials & Interfaces (article, 2023-07-29)
Field: Materials Science — Materials Chemistry

Sponge-like Cryogels from Liquid–Liquid Phase Separation: Structure, Porosity, and Diffusional Gel Properties Macroporous gels find application in several scientific fields, ranging from art restoration to wastewater filtration or cell entrapment. In this work, two-component sponge-like cryogels are challenged to assess their cleaning performances and to investigate how pores size and connectivity affect physico-chemical properties. The gels were obtained through a freeze-thaw process, exploiting a spontaneous polymer-polymer phase-separation occurring in the pre-gel solution. During the freezing step, a highly hydrolyzed polyvinyl alcohol (H-PVA) forms the hydrogel walls. The secondary components, namely a partially hydrolyzed polyvinyl alcohol (L-PVA) or polyvinyl pyrrolidone (PVP), act as modular porogens, being partially extracted during gel washing. H-PVA/L-PVA and H-PVA/PVP mixtures were studied by confocal laser scanning microscopy to unveil sols and gels morphology at the micron-scale, while small angle X-ray scattering was used to get insights about characteristic dimensions at the nanoscale. The gelation mechanism was investigated through rheology measurements, and the characteristic exponents were compared to De Gennes' scaling laws gathered from percolation. In the field of art conservation, these sponge-like gels are ideal systems for the cleaning of artistic painted surfaces. Their interconnected pores allow the diffusion of cleaning fluids at the painted interface, facilitating dirt uptake and/or detachment. This study uncovered a direct relationship linking a gel's cleaning performance to its apparent tortuosity. These findings can pave the way to fine-tuning systems with enhanced cleaning abilities, not restricted to the restoration of irreplaceable priceless works of art, but with possible application in diverse research fields. Polyvinyl alcohol ; Materials science ; Chemical engineering ; Polymer ; Phase (matter) ; Porosity ; Rheology ; Diffusion ; Composite material ; Chemistry ; Organic chemistry Pickering emulsions and particle stabilization ; Surface Modification and Superhydrophobicity ; Cultural Heritage Materials Analysis
Authors: Achilleas Savva | Janire Sáez | Aimee Withers | Chiara Barberio | Verena Stoeger | Shani Elias‐Kirma | Zixuan Lu | Chrysanthi‐Maria Moysidou | Konstantinos Kallitsis | Charalampos Pitsalidis | Róisı́n M. Owens
Source: Materials Horizons (article, 2023-01-01)
Field: Materials Science — Polymers and Plastics

3D organic bioelectronics for electrical monitoring of human adult stem cells Three-dimensional <i>in vitro</i> stem cell models have enabled a fundamental understanding of cues that direct stem cell fate. While sophisticated 3D tissues can be generated, technology that can accurately monitor these complex models in a high-throughput and non-invasive manner is not well adapted. Here we show the development of 3D bioelectronic devices based on the electroactive polymer poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)-(PEDOT:PSS) and their use for non-invasive, electrical monitoring of stem cell growth. We show that the electrical, mechanical and wetting properties as well as the pore size/architecture of 3D PEDOT:PSS scaffolds can be fine-tuned simply by changing the processing crosslinker additive. We present a comprehensive characterization of both 2D PEDOT:PSS thin films of controlled thicknesses, and 3D porous PEDOT:PSS structures made by the freeze-drying technique. By slicing the bulky scaffolds we generate homogeneous, porous 250 μm thick PEDOT:PSS slices, constituting biocompatible 3D constructs able to support stem cell cultures. These multifunctional slices are attached on indium-tin oxide substrates (ITO) with the help of an electrically active adhesion layer, enabling 3D bioelectronic devices with a characteristic and reproducible, frequency dependent impedance response. This response changes drastically when human adipose derived stem cells (hADSCs) grow within the porous PEDOT:PSS network as revealed by fluorescence microscopy. The increase of cell population within the PEDOT:PSS porous network impedes the charge flow at the interface between PEDOT:PSS and ITO, enabling the interface resistance (<i>R</i><sub>1</sub>) to be used as a figure of merit to monitor the proliferation of stem cells. The non-invasive monitoring of stem cell growth allows for the subsequent differentiation 3D stem cell cultures into neuron like cells, as verified by immunofluorescence and RT-qPCR measurements. The strategy of controlling important properties of 3D PEDOT:PSS structures simply by altering processing parameters can be applied for development of a number of stem cell <i>in vitro</i> models as well as stem cell differentiation pathways. We believe the results presented here will advance 3D bioelectronic technology for both fundamental understanding of <i>in vitro</i> stem cell cultures as well as the development of personalized therapies. PEDOT:PSS ; Bioelectronics ; Materials science ; Nanotechnology ; Indium tin oxide ; Conductive polymer ; Stem cell ; Polymer ; Thin film ; Layer (electronics) ; Composite material ; Biosensor Conducting polymers and applications ; Advanced Sensor and Energy Harvesting Materials ; Neuroscience and Neural Engineering
Authors: Li‐Xue Jiang | Matthias Polack | Xiangtang Li | Manxi Yang | Detlev Belder | Julia Laskin
Source: Lab on a Chip (article, 2023-01-01)
Field: Chemistry — Spectroscopy

A monolithic microfluidic probe for ambient mass spectrometry imaging of biological tissues Ambient mass spectrometry imaging (MSI) is a powerful technique that allows for the simultaneous mapping of hundreds of molecules in biological samples under atmospheric conditions, requiring minimal sample preparation. We have developed nanospray desorption electrospray ionization (nano-DESI), a liquid extraction-based ambient ionization technique, which has proven to be sensitive and capable of achieving high spatial resolution. We have previously described an integrated microfluidic probe, which simplifies the nano-DESI setup, but is quite difficult to fabricate. Herein, we introduce a facile and scalable strategy for fabricating microfluidic devices for nano-DESI MSI applications. Our approach involves the use of selective laser-assisted etching (SLE) of fused silica to create a monolithic microfluidic probe (SLE-MFP). Unlike the traditional photolithography-based fabrication, SLE eliminates the need for the wafer bonding process and allows for automated, scalable fabrication of the probe. The chamfered design of the sampling port and ESI emitter significantly reduces the amount of polishing required to fine-tune the probe thereby streamlining and simplifying the fabrication process. We have also examined the performance of a V-shaped probe, in which only the sampling port is fabricated using SLE technology. The V-shaped design of the probe is easy to fabricate and provides an opportunity to independently optimize the size and shape of the electrospray emitter. We have evaluated the performance of SLE-MFP by imaging mouse tissue sections. Our results demonstrate that SLE technology enables the fabrication of robust monolithic microfluidic probes for MSI experiments. This development expands the capabilities of nano-DESI MSI and makes the technique more accessible to the broader scientific community. Microfluidics ; Fabrication ; Nanotechnology ; Materials science ; Wafer ; Fluidics ; Mass spectrometry imaging ; Mass spectrometry ; Chemistry ; Chromatography Mass Spectrometry Techniques and Applications ; Microfluidic and Capillary Electrophoresis Applications ; Advanced Chemical Sensor Technologies
Authors: Aviva Levina | Canan Uslan | Heide A. Murakami | Debbie C. Crans | Peter A. Lay
Source: Inorganic Chemistry (article, 2023-10-20)
Field: Chemistry — Inorganic Chemistry

Substitution Kinetics, Albumin and Transferrin Affinities, and Hypoxia All Affect the Biological Activities of Anticancer Vanadium(V) Complexes Limited stability of most transition-metal complexes in biological media has hampered their medicinal applications but also created a potential for novel cancer treatments, such as intratumoral injections of cytotoxic but short-lived anticancer drugs. Two related V(V) complexes, [VO(Hshed)(dtb)] (<b>1</b>) and [VO(Hshed)(cat)] (<b>2</b>), where H<sub>2</sub>shed = <i>N</i>-(salicylideneaminato)-<i>N'</i>-(2-hydroxyethyl)-1,2-ethanediamine, H<sub>2</sub>dtb = 3,5-di-<i>tert</i>-butylcatechol, and H<sub>2</sub>cat = 1,2-catechol, decomposed within minutes in cell culture medium at 310 K (<i>t</i><sub>1/2</sub> = 43 and 9 s for <b>1</b> and <b>2</b>, respectively). Despite this, both complexes showed high antiproliferative activities in triple-negative human breast cancer (MDA-MB-231) cells, but the mechanisms of their activities were radically different. Complex <b>1</b> formed noncovalent adducts with human serum albumin, rapidly entered cells via passive diffusion, and was nearly as active in a short-term treatment (IC<sub>50</sub> = 1.9 ± 0.2 μM at 30 min) compared with a long-term treatment (IC<sub>50</sub> = 1.3 ± 0.2 μM at 72 h). The activity of <b>1</b> decreased about 20-fold after its decomposition in cell culture medium for 30 min at 310 K. Complex <b>2</b> showed similar activities (IC<sub>50</sub> ≈ 12 μM at 72 h) in both fresh and decomposed solutions and was inactive in a short-term treatment. The activity of <b>2</b> was mainly due to the reactions among V(V) decomposition products, free catechol, and O<sub>2</sub> in cell culture medium. As a result, the activity of <b>1</b> was less sensitive than that of <b>2</b> to the effects of hypoxic conditions that are characteristic of solid tumors and to the presence of apo-transferrin that acts as a scavenger of V(V/IV) decomposition products in blood serum. In summary, complex <b>1</b>, but not <b>2</b>, is a suitable candidate for further development as an anticancer drug delivered via intratumoral injections. These results demonstrate the importance of fine-tuning the ligand properties for the optimization of biological activities of metal complexes. Chemistry ; Kinetics ; Stereochemistry ; Human serum albumin ; Adduct ; IC50 ; Medicinal chemistry ; Biochemistry ; In vitro ; Organic chemistry Vanadium and Halogenation Chemistry ; Metal-Catalyzed Oxygenation Mechanisms ; Metal complexes synthesis and properties
Authors: Julianna S. Doll | Felix J. Becker | Dragoş‐Adrian Roşca
Source: ACS Organic & Inorganic Au (article, 2023-10-23)
Field: Chemistry — Inorganic Chemistry

Diazines and Triazines as Building Blocks in Ligands for Metal-Mediated Catalytic Transformations Pyridine is a ubiquitous building block for the design of very diverse ligand platforms, many of which have become indispensable for catalytic transformations. Nevertheless, the isosteric pyrazine, pyrimidine, and triazine congeners have enjoyed thus far a less privileged role in ligand design. In this review, several applications of such fragments in the design of new catalysts are presented. In a significant number of cases described, diazine- and triazine-based ligands either outperform their pyridine congeners or offer alternative catalytic pathways which enable new reactivities. The potential opportunities unlocked by using these building blocks in ligand design are discussed, and the origin of the enhanced catalytic activity is highlighted where mechanistic studies are available. Diazine ; Triazine ; Pyrazine ; Catalysis ; Ligand (biochemistry) ; Combinatorial chemistry ; Pyridine ; Chemistry ; Rational design ; Block (permutation group theory) ; Pyrimidine ; Nanotechnology ; Stereochemistry ; Organic chemistry ; Materials science ; Mathematics ; Receptor ; Biochemistry Asymmetric Hydrogenation and Catalysis ; Nanomaterials for catalytic reactions ; Catalytic C–H Functionalization Methods
Authors: Cătălin Păun | Ludmila Motelică | Denisa Ficai | Anton Ficai | Ecaterina Andronescu
Source: Materials (review, 2023-09-09)
Field: Chemistry — Inorganic Chemistry

Metal-Organic Frameworks: Versatile Platforms for Biomedical Innovations This review article explores the multiple applications and potential of metal-organic frameworks (MOFs) in the biomedical field. With their highly versatile and tunable properties, MOFs present many possibilities, including drug delivery, biomolecule recognition, biosensors, and immunotherapy. Their crystal structure allows precise tuning, with the ligand typology and metal geometry playing critical roles. MOFs' ability to encapsulate drugs and exhibit pH-triggered release makes them ideal candidates for precision medicine, including cancer treatment. They are also potential gene carriers for genetic disorders and have been used in biosensors and as contrast agents for magnetic resonance imaging. Despite the complexities encountered in modulating properties and interactions with biological systems, further research on MOFs is imperative. The primary focus of this review is to provide a comprehensive examination of MOFs in these applications, highlighting the current achievements and complexities encountered. Such efforts will uncover their untapped potential in creating innovative tools for biomedical applications, emphasizing the need to invest in the continued exploration of this promising field. Nanotechnology ; Metal-organic framework ; Drug delivery ; Biosensor ; Computer science ; Engineering ethics ; Materials science ; Biochemical engineering ; Engineering ; Chemistry Metal-Organic Frameworks: Synthesis and Applications ; Nanoplatforms for cancer theranostics ; Dendrimers and Hyperbranched Polymers
Authors: Cristina Negro | Héctor Martínez-Pérez-Cejuela | Ernesto Francisco Simó‐Alfonso | Waseem Iqbal | José Manuel Herrero‐Martínez | Donatella Armentano | Jesús Ferrando‐Soria | Emilio Pardo
Source: ACS Applied Materials & Interfaces (article, 2023-01-04)
Field: Chemistry — Inorganic Chemistry

(Multivariate)-Metal–Organic Framework for Highly Efficient Antibiotic Capture from Aquatic Environmental Matrices Contamination of aquatic environments by pharmaceuticals used by modern societies has become a serious threat to human beings. Among them, antibiotics are of particular concern due to the risk of creating drug-resistant bacteria and, thus, developing efficient protocols for the capture of this particular type of drug is mandatory. Herein, we report a family of three isoreticular MOFs, derived from natural amino acids, that exhibit high efficiency in the removal of a mixture of four distinct families of antibiotics, such as fluoroquinolones, penicillins, lincomycins, and cephalosporins, as solid-phase extraction (SPE) sorbents. In particular, a multivariate (MTV)-MOF, prepared using equal percentages of amino acids l-serine and l-methionine, also exhibits outstanding recyclability, surpassing the benchmark material activated carbon. The good removal performance of the MTV-MOF was rationalized by means of single-crystal X-ray diffraction. These results highlight the situation of MOFs as a real and promising alternative for the capture of antibiotics from environmental matrices, especially wastewater streams. Antibiotics ; Materials science ; Metal-organic framework ; Combinatorial chemistry ; Contamination ; Environmental chemistry ; Organic chemistry ; Chemistry ; Biology ; Microbiology ; Ecology ; Adsorption Metal-Organic Frameworks: Synthesis and Applications ; Covalent Organic Framework Applications ; Advanced Photocatalysis Techniques
Authors: Giacomo Filippini | Jacopo Dosso | Maurizio Prato
Source: Helvetica Chimica Acta (article, 2023-06-12)
Field: Chemistry — Organic Chemistry

Phenols as Novel Photocatalytic Platforms for Organic Synthesis Abstract In recent years, organic chemists have devoted a great deal of effort towards the implementation of novel green photocatalytic synthetic protocols. To this end, the development of new effective, non‐toxic, inexpensive photocatalysts, which are capable of driving value‐added chemical transformations, is highly desirable. Interestingly, phenols fulfill all these requirements due to their outstanding physicochemical features, therefore emerging as promising metal‐free photocatalytic platforms for organic synthesis. This Perspective aims at highlighting the most recent applications of phenols in organic photocatalysis. More specifically, phenolate anions, formed upon deprotonation of phenols, are photo‐active organic intermediates that may absorb light within the visible region. Thus, when in the excited states, these anions may be used as reductants to generate reactive open shell species from suitable precursors under mild operative conditions. Alternatively, phenolate anions and suitable radical precursors can form electron donor‐acceptor (EDA) complexes. Specifically, the photochemical activity of these molecular aggregates can be used to initiate organic radical reactions. Lastly, forward‐looking opportunities within this research field have been discussed. Chemistry ; Photocatalysis ; Deprotonation ; Phenols ; Organic synthesis ; Photochemistry ; Combinatorial chemistry ; Organic chemistry ; Catalysis ; Ion Radical Photochemical Reactions ; Sulfur-Based Synthesis Techniques ; Catalytic C–H Functionalization Methods
Authors: Ana M. Pérez‐López | Adam Belsom | Linus Fiedler | Xiaoyi Xin | Juri Rappsilber
Source: Journal of Medicinal Chemistry (article, 2023-02-23)
Field: Chemistry — Organic Chemistry

Dual-Bioorthogonal Catalysis by a Palladium Peptide Complex Artificial metalloenzymes (ArMs) enrich bioorthogonal chemistry with new-to-nature reactions while limiting metal deactivation and toxicity. This enables biomedical applications such as activating therapeutics <i>in situ</i>. However, while combination therapies are becoming widespread anticancer treatments, dual catalysis by ArMs has not yet been shown. We present a heptapeptidic ArM with a novel peptide ligand carrying a methyl salicylate palladium complex. We observed that the peptide scaffold reduces metal toxicity while protecting the metal from deactivation by cellular components. Importantly, the peptide also improves catalysis, suggesting involvement in the catalytic reaction mechanism. Our work shows how a palladium-peptide homogeneous catalyst can simultaneously mediate two types of chemistry to synthesize anticancer drugs in human cells. Methyl salicylate palladium LLEYLKR peptide (<b>2-Pd</b>) succeeded to simultaneously produce paclitaxel by depropargylation, and linifanib by Suzuki-Miyaura cross-coupling in cell culture, thereby achieving combination therapy on non-small-cell lung cancer (NSCLC) A549 cells. Bioorthogonal chemistry ; Chemistry ; Peptide ; Palladium ; Combinatorial chemistry ; Catalysis ; Ligand (biochemistry) ; Peptide synthesis ; Biochemistry ; Click chemistry ; Receptor Click Chemistry and Applications ; Chemical Synthesis and Analysis ; Advanced biosensing and bioanalysis techniques