jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Krystal A. Hughes | Bishal Misra | Maryam Maghareh | Parinya Samart | Ethan Nguyen | Salik Hussain | Werner J. Geldenhuys | Sharan Bobbala
Source: Discover Nano (article, 2024-01-04)
Field: Materials Science — Biomaterials

Flash nanoprecipitation allows easy fabrication of pH-responsive acetalated dextran nanoparticles for intracellular release of payloads Acetalated dextran (Ac-Dex) nanoparticles are currently of immense interest due to their sharp pH-responsive nature and high biodegradability. Ac-Dex nanoparticles are often formulated through single- or double-emulsion methods utilizing polyvinyl alcohol as the stabilizer. The emulsion methods utilize toxic organic solvents such as dichloromethane or chloroform and require multi-step processing to form stable Ac-Dex nanoparticles. Here, we introduce a simple flash nanoprecipitation (FNP) approach that utilizes a confined impinging jet mixer and a non-toxic solvent, ethanol, to form Ac-Dex nanoparticles rapidly. Ac-Dex nanoparticles were stabilized using nonionic PEGylated surfactants, D-α-Tocopherol polyethylene glycol succinate (TPGS), or Pluronic (F-127). Ac-Dex nanoparticles formed using FNP were highly monodisperse and stably encapsulated a wide range of payloads, including hydrophobic, hydrophilic, and macromolecules. When lyophilized, Ac-Dex TPGS nanoparticles remained stable for at least one year with greater than 80% payload retention. Ac-Dex nanoparticles were non-toxic to cells and achieved intracellular release of payloads into the cytoplasm. In vivo studies demonstrated a predominant biodistribution of Ac-Dex TPGS nanoparticles in the liver, lungs, and spleen after intravenous administration. Taken together, the FNP technique allows easy fabrication and loading of Ac-Dex nanoparticles that can precisely release payloads into intracellular environments for diverse therapeutic applications. pH-responsive Acetalateddextran can be formulated using nonionic surfactants, such as TPGS or F-127, for intracellular release of payloads. Highly monodisperse and stable nanoparticles can be created through the simple, scalable flash nanoprecipitation technique, which utilizes a confined impingement jet mixer. Nanoparticle ; Poloxamer ; Dispersity ; Emulsion ; Dextran ; Polyethylene glycol ; Materials science ; Drug carrier ; Chemistry ; Ethylene glycol ; Nanotechnology ; Chemical engineering ; Drug delivery ; Chromatography ; Organic chemistry ; Copolymer ; Polymer Nanoparticle-Based Drug Delivery ; Inhalation and Respiratory Drug Delivery ; Electrohydrodynamics and Fluid Dynamics
Authors: Yingwei Hu | Michael Schnaubelt | Li Chen | Bai Zhang | Trung Hoàng | T. Mamie Lih | Zhen Zhang | Hui Zhang
Source: Analytical Chemistry (article, 2024-06-13)
Field: Chemistry — Spectroscopy

MS-PyCloud: A Cloud Computing-Based Pipeline for Proteomic and Glycoproteomic Data Analyses Rapid development and wide adoption of mass spectrometry-based glycoproteomic technologies have empowered scientists to study proteins and protein glycosylation in complex samples on a large scale. This progress has also created unprecedented challenges for individual laboratories to store, manage, and analyze proteomic and glycoproteomic data, both in the cost for proprietary software and high-performance computing and in the long processing time that discourages on-the-fly changes of data processing settings required in explorative and discovery analysis. We developed an open-source, cloud computing-based pipeline, MS-PyCloud, with graphical user interface (GUI), for proteomic and glycoproteomic data analysis. The major components of this pipeline include data file integrity validation, MS/MS database search for spectral assignments to peptide sequences, false discovery rate estimation, protein inference, quantitation of global protein levels, and specific glycan-modified glycopeptides as well as other modification-specific peptides such as phosphorylation, acetylation, and ubiquitination. To ensure the transparency and reproducibility of data analysis, MS-PyCloud includes open-source software tools with comprehensive testing and versioning for spectrum assignments. Leveraging public cloud computing infrastructure via Amazon Web Services (AWS), MS-PyCloud scales seamlessly based on analysis demand to achieve fast and efficient performance. Application of the pipeline to the analysis of large-scale LC-MS/MS data sets demonstrated the effectiveness and high performance of MS-PyCloud. The software can be downloaded at https://github.com/huizhanglab-jhu/ms-pycloud. Cloud computing ; Computer science ; Pipeline (software) ; Software ; Database ; Proteomics ; Proteome ; Chemistry ; Data mining ; Operating system ; Biochemistry Advanced Proteomics Techniques and Applications ; Genomics and Phylogenetic Studies ; Glycosylation and Glycoproteins Research
Authors: Tianqing Zhou | Ze Luo | Yongzhou Zhang | B.L. Liu | Lan Li | Rong Wang | Haibo Huang | Hua Tang
Source: Surfaces and Interfaces (article, 2024-07-03)
Field: Chemistry — Inorganic Chemistry

Innovative two-dimensional porphyrin-integrated metal-organic frameworks for enhanced photocatalytic hydrogen peroxide generation in pure water • The novel 2D-MOFs, specifically Ce-TCPP and La-TCPP, with a consistent topological framework, were successfully synthesized. • The architecture of 2D-MOFs fine-tunes the electron and hole transport pathways, thus enhancing the photocatalytic activity . • La-TCPP exhibited significant photocatalytic performance, achieving an H 2 O 2 yield of 79.75 μmol/g/h in pure water. In the quest for eco-friendly and efficient synthesis of hydrogen peroxide (H 2 O 2 ), a chemical with extensive applications, photocatalytic production emerges as a promising clean technique. Metal-organic frameworks (MOFs), known for their exceptional porosity and geometric customizability, stand at the forefront of potential photocatalytic materials. Yet, the conventional three-dimensional topologies of MOFs pose a challenge, impeding the swift transit of photogenerated electrons and thereby curbing performance enhancements. In this vein, we have engineered novel 2D porphyrin-based MOFs , specifically Ce-TCPP and La-TCPP, utilizing diverse metal sources while maintaining a consistent topological framework. This design strategy streamlines the electron and hole transport pathways, thus elevating the photocatalytic activity . Delving into the structural nuances of these MOFs , our research unveiled that the photocatalytic activity experienced a marked shift upon altering the metal cluster types. Notably, La-TCPP, as an efficacious catalyst, demonstrated an H 2 O 2 yield of 79.75 μmol/g/h in pure water, sans any sacrificial agents. Rigorous testing confirmed the robust stability of both MOFs . This study marks the inaugural design and synthesis of a single crystal structure of La-TCPP. By strategically varying metal cluster compositions, we have fine-tuned the architecture of two-dimensional MOFs. This approach sheds light on the intricate structure-activity relationship governing the photocatalytic synthesis of H 2 O 2 , paving the way for future advancements in the field. Photocatalysis ; Materials science ; Porphyrin ; Metal-organic framework ; Nanotechnology ; Catalysis ; Water splitting ; Hydrogen peroxide ; Porosity ; Metal ; Chemical engineering ; Photochemistry ; Organic chemistry ; Chemistry ; Adsorption ; Composite material Metal-Organic Frameworks: Synthesis and Applications ; Advanced Photocatalysis Techniques ; Covalent Organic Framework Applications
Authors: Givi Kalandia | Cui‐Lian Liu | David E. Salazar Marcano | Mhamad Aly Moussawi | Sem Bleus | Bart Van Meerbeek | Wim Dehaen | Tatjana N. Parac‐Vogt
Source: Angewandte Chemie International Edition (article, 2024-11-13)
Field: Materials Science — Materials Chemistry

Host‐Guest Assemblies of Polyoxovanadate Clusters as Supramolecular Catalysts Supramolecular functional materials can be used to overcome some of the most challenging tasks in materials science, where the dynamic nature of supramolecular interactions can be leveraged to fine-tune the properties of the material for a given task. The Lindqvist hexavanadate family of polyoxometalates (POMs) have emerged as particularly interesting candidates to be used in supramolecular materials due to their redox and Lewis acid properties that enable their application in the fields of energy conversion/storage or catalysis. Despite their promising potential, hexavanadate clusters are underrepresented in the field of supramolecular materials, mainly due to the synthetic challenges related to their inherent reactivity. In this work, pillar[5]arene was successfully grafted onto a Lindqvist hexavanadate and the resulting structure was confirmed by single crystal X-ray diffraction (SC-XRD), presenting the first example of a crystal structure of a POMcovalently functionalized with a pillar[5]arene. By introducing a ditopic guest molecule that could interlink pillar[5]arene moieties, host-guest interactions were leveraged as the driving force for the formation of supramolecular assemblies incorporating hexavanadate clusters in a controlled manner. The enhanced catalytic performance of the resulting aggregates confirmed their potential application as functional catalytic materials. This novel approach for developing hexavanadate-based catalysts reported here showcases the potential of using host-guest interactions as a means to introduce catalytically active metal-oxo clusters into supramolecular frameworks. Supramolecular chemistry ; Polyoxometalate ; Catalysis ; Nanotechnology ; Pillar ; Materials science ; Molecule ; Supramolecular assembly ; Reactivity (psychology) ; Covalent bond ; Chemistry ; Combinatorial chemistry ; Organic chemistry Polyoxometalates: Synthesis and Applications ; Metal-Organic Frameworks: Synthesis and Applications ; Nanocluster Synthesis and Applications
Authors: Antonio Angelastro | Alexey Barkhanskiy | Toby Journeaux | Rohan Sivapalan | Thomas A. King | Laura Rodríguez Pérez | William R. F. Goundry | Perdita E. Barran | Sabine L. Flitsch
Source: Nature Synthesis (article, 2024-06-14)
Field: Chemistry — Organic Chemistry

Horner–Wadsworth–Emmons olefination of proteins and glycoproteins Abstract Chemo-selective modifications of proteins are fundamental to the advancement of biological and pharmaceutical sciences. The search for biocompatible chemical reactions has prompted us to investigate Horner–Wadsworth–Emmons (HWE) olefinations, iconic reactions in organic synthesis that would give rise to new selective protein olefinations. Our choice of HWE olefinations was inspired by the growing number of methods for generating aldehydes as transient reactive groups in proteins and the potential for mild and simple reaction conditions. Here we show that HWE olefination reactions on aldehydes, produced by both chemical and enzymatic methods, are compatible with physiological conditions and highly selective in small and large proteins, including therapeutic antibodies and stable recombinant proteins exemplified by green fluorescent protein. Reaction kinetics can be fine-tuned over orders of magnitude both by judicious use of substituents and pH regulation. The electrophilic nature of the HWE olefination products can be tuned to allow for subsequent nucleophilic additions, including thiol- and phospha-Michael additions. Our results demonstrate that HWE olefination of aldehydes in proteins provides efficient and selective bioconjugation chemistries that are orthogonal to existing methods. Chemistry ; Bioconjugation ; Electrophile ; Nucleophile ; Organic chemistry ; Thiol ; Combinatorial chemistry ; Biochemistry ; Catalysis Click Chemistry and Applications ; Chemical Synthesis and Analysis ; Monoclonal and Polyclonal Antibodies Research
Authors: Sen Xiang | Jinbo Zhang | Shaofeng Liu | Pierre Braunstein | Zhibo Li
Source: Macromolecules (article, 2024-04-02)
Field: Materials Science — Biomaterials

Aluminum Complexes Bearing Aminoquinoline Ligands with Different Pendant Donors: Remarkable Impact of Hemilability on the Ring-Opening Polymerization of ε-Caprolactone Hemilabile ligands are highly promising components of advanced catalysts because their switchable coordination modes can trigger novel activation and stabilization mechanisms. Their increasing use has led to the successful development of stable, active, and selective catalysts. In this study, new aluminum complexes bearing aminoquinoline ligands with different potential hemilabile thiophenyl (Al1), phenoxyl (Al2), or benzyl (Al3) donor arms have been synthesized and used for the ring-opening polymerization (ROP) of ε-caprolactone (ε-CL). X-ray diffraction analysis revealed that the distance between the Al center and the pendant donor decreased in the order Al3 > Al1 > Al2, consistent with the 31P NMR spectroscopic evaluations of their relative donor capacities by the Gutmann–Beckett method. ROP of ε-CL under otherwise identical conditions revealed that Al1 with a hemilabile thiophenyl donor displayed both higher activity and stability than the complexes with a phenoxyl (Al2) or benzyl (Al3) group. The catalytic properties of the Al complexes were further enhanced by fine-tuning the S substituents. Remarkably, ultrahigh-molecular-weight polycaprolactones (PCLs; Mn up to 41.2 × 104 g·mol–1) were readily synthesized, and immortal catalysis with a catalyst loading as low as 0.01 mol % relative to monomer and a large excess BnOH (up to 100 equiv to Al) was achieved as a result of hemilabile ligand coordination. Chemistry ; Monomer ; Polymerization ; Catalysis ; Ligand (biochemistry) ; Ring (chemistry) ; Polymer chemistry ; Ring-opening polymerization ; Caprolactone ; Aluminium ; Stereochemistry ; Medicinal chemistry ; Organic chemistry ; Polymer ; Receptor biodegradable polymer synthesis and properties ; Carbon dioxide utilization in catalysis ; Polyoxometalates: Synthesis and Applications
Authors: Filippo Bodo | Alessandro Erba | Elfi Kraka | Renaldo T. Moura
Source: Journal of Computational Chemistry (article, 2024-01-26)
Field: Chemistry — Inorganic Chemistry

Chemical bonding in Uranium‐based materials: A local vibrational mode case study of Cs 2UO 2Cl 4 and UCl 4 crystals The Local Vibrational Mode Analysis, initially applied to diverse molecular systems, was extended to periodic systems in 2019. This work introduces an enhanced version of the LModeA software, specifically designed for the comprehensive analysis of two and three-dimensional periodic structures. Notably, a novel interface with the Crystal package was established, enabling a seamless transition from molecules to periodic systems using a unified methodology. Two distinct sets of uranium-based systems were investigated: (i) the evolution of the Uranyl ion (UO <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow><mml:msubsup><mml:mo> </mml:mo> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> <mml:mrow><mml:mn>2</mml:mn> <mml:mo>+</mml:mo></mml:mrow> </mml:msubsup> </mml:mrow> </mml:math> ) traced from its molecular configurations to the solid state, exemplified by Cs <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow><mml:msub><mml:mo> </mml:mo> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> </mml:msub> </mml:mrow> </mml:math> UO <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow><mml:msub><mml:mo> </mml:mo> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> </mml:msub> </mml:mrow> </mml:math> Cl <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow><mml:msub><mml:mo> </mml:mo> <mml:mrow><mml:mn>4</mml:mn></mml:mrow> </mml:msub> </mml:mrow> </mml:math> and (ii) Uranium tetrachloride (UCl <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow><mml:msub><mml:mo> </mml:mo> <mml:mrow><mml:mn>4</mml:mn></mml:mrow> </mml:msub> </mml:mrow> </mml:math> ) in both its molecular and crystalline forms. The primary focus was on exploring the impact of crystal packing on key properties, including IR and Raman spectra, structural parameters, and an in-depth assessment of bond strength utilizing local mode perspectives. This work not only demonstrates the adaptability and versatility of LModeA for periodic systems but also highlights its potential for gaining insights into complex materials and aiding in the design of new materials through fine-tuning. Uranyl ; Uranium ; Raman spectroscopy ; Molecule ; Crystal (programming language) ; Molecular vibration ; Materials science ; Chemistry ; Chemical physics ; Crystallography ; Computer science ; Physics ; Metallurgy Radioactive element chemistry and processing ; Solid-state spectroscopy and crystallography ; Nuclear Materials and Properties
Authors: Meng Xu | Eun Ji Kim | Young Jun Lee | Hyunsoo Lee | Kyunghyun Jung | Jaeyoung Choi | Shin‐Hyun Kim | YongJoo Kim | Hongseok Yun | Bumjoon J. Kim
Source: Science Advances (article, 2024-06-14)
Field: Materials Science — Materials Chemistry

Icosahedral supracrystal assembly from polymer-grafted nanoparticles via interplay of interfacial energy and confinement effect Self-assembly of nanoparticles (NPs) in drying emulsion droplets paves the way for intricate three-dimensional (3D) superstructures, given the myriad of control parameters for fine-tuning assembly conditions. With their substantial energetic dynamics that are acutely responsive to emulsion confinements, polymeric ligands incorporated into a system can enrich its structural diversity. Here, we demonstrate the assembly of soft polymer-grafted NPs into Mackay icosahedrons beyond spherical body-centered cubic (BCC) packing structures commonly observed for these soft spheres. This behavior is governed by the free energy minimization within emulsions through the interplay of the oil-water interfacial energy and confinement effect as demonstrated by the experimental observations of structural transitions between icosahedrons and BCC crystals and by corresponding free energy calculations. The anisotropic surface of the icosahedral supracrystals provides the capability of guiding the position of a secondary constituent, creating unique hybrid patchy icosahedrons with the potential to develop into multifunctional 3D clusters that combine the benefits of both polymers and conventional colloids. Icosahedral symmetry ; Materials science ; Nanoparticle ; Polymer ; Chemical physics ; Nanotechnology ; Self-assembly ; Colloid ; Emulsion ; Surface energy ; SPHERES ; Molecular dynamics ; Chemical engineering ; Crystallography ; Composite material ; Chemistry ; Physics ; Computational chemistry Pickering emulsions and particle stabilization ; Surfactants and Colloidal Systems ; Proteins in Food Systems
Authors: Man Pang Tang | Lihui Zhu | Yulin Deng | Yi‐Xiang Shi | Samuel Kin‐Man Lai | Xiaoyong Mo | Xin‐Yu Pang | Chunyu Liu | Wei Jiang | Edmund C. M. Tse | Ho Yu Au‐Yeung
Source: Angewandte Chemie International Edition (article, 2024-04-25)
Field: Chemistry — Organic Chemistry

Water and Air Stable Copper(I) Complexes of Tetracationic Catenane Ligands for Oxidative C−C Cross‐Coupling Aqueous soluble and stable Cu(I) molecular catalysts featuring a catenane ligand composed of two dicationic, mutually repelling but mechanically interlocked macrocycles are reported. The ligand interlocking not only fine-tunes the coordination sphere and kinetically stabilizes the Cu(I) against air oxidation and disproportionation, but also buries the hydrophobic portions of the ligands and prevents their dissociation which are necessary for their good water solubility and a sustained activity. These catenane Cu(I) complexes can catalyze the oxidative C-C coupling of indoles and tetrahydroisoquinolines in water, using H<sub>2</sub>O<sub>2</sub> as a green oxidant with a good substrate scope. The successful use of catenane ligands in exploiting aqueous Cu(I) catalysis thus highlights the many unexplored potential of mechanical bond as a design element for exploring transition metal catalysis under challenging conditions. Copper ; Catenane ; Coupling (piping) ; Chemistry ; Oxidative phosphorylation ; Polymer chemistry ; Stereochemistry ; Materials science ; Organic chemistry ; Metallurgy ; Molecule ; Biochemistry Catalytic C–H Functionalization Methods ; Catalytic Cross-Coupling Reactions ; Oxidative Organic Chemistry Reactions
Authors: Xinyi Zhang | Zhikang Han | Tianle Cao | Yue Zhu | Zengrong Wang | Zhaoyang Zhang | Zhaohui Zhou | Dongqing Zhang | Ni Yan | Yueyan Zhang | Gang He
Source: Chemical Engineering Journal (article, 2024-12-10)
Field: Materials Science — Polymers and Plastics

Multi-responsive thiazolothiazole viologen-based electrochromic materials for smart windows and electronic displays Electrochromism ; Viologen ; Materials science ; Electronic materials ; Nanotechnology ; Computer science ; Optoelectronics ; Chemistry ; Photochemistry ; Physical chemistry ; Electrode Transition Metal Oxide Nanomaterials ; Conducting polymers and applications ; Polyoxometalates: Synthesis and Applications
Authors: Baptiste Amouroux | Ali Eftekhari | Clément Roux | J. C. Micheau | Pierre Roblin | Mathieu Pasturel | Fabienne Gauffre | Christian Würth | Ute Resch‐Genger | Michel Sliwa | Aude Bouchet | Christophe Coudret
Source: Advanced Optical Materials (article, 2024-06-26)
Field: Materials Science — Materials Chemistry

Synthesis and Emission Dynamics of Sub‐3 nm Upconversion Nanoparticles Abstract Reducing the size of upconversion nanoparticles (UCNPs) down to a few nm yields luminescent materials containing a very small number of emitters. Considering the bottom limit of one activator per particle ultrasmall UCNPs offer an unprecedented platform to study the contributions of the different energy transfers at play in upconversion luminescence. Maintaining detectable emission despite the limited number of emitting ions and the high surface‐to‐volume ratio requires suitable particle architectures. Na(Gd‐Yb)F 4 :Tm 3+ emissive sub‐3 nm diameter β‐phase UCNPs are prepared using a gadolinium‐rich composition in situ mixing of the precursors and a microwave high‐temperature cycling sequence allowing precise control of the particle size and dispersity. These cores are coated with a NaGdF 4 inert shell to minimize the deleterious influence of surface quenching (SQ). Time‐resolved luminescence measurements combining standard NIR excitation of the Yb 3+ sensitizer and direct UV excitation of the Tm 3+ activator are performed to quantify cross relaxation and surface quenching processes. The fine tuning of the number of activators per particle via an optimized synthesis pathway along with the use of an appropriate excitation scheme enabled to provide an accurate analysis of the different mechanisms at play in these model nanoparticles and to characterize the structure of the core‐shell architecture. Materials science ; Luminescence ; Photon upconversion ; Nanoparticle ; Activator (genetics) ; Quenching (fluorescence) ; Particle size ; Ion ; Excitation ; Dispersity ; Fluorescence ; Analytical Chemistry (journal) ; Particle (ecology) ; Nanotechnology ; Chemical engineering ; Optoelectronics ; Optics ; Chemistry Luminescence Properties of Advanced Materials ; Nuclear materials and radiation effects ; Radiation Detection and Scintillator Technologies