jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Zheren Wang | Yingzhi Sun | Kevin Cruse | Yan Zeng | Yuxing Fei | Zexuan Liu | Junyi Shangguan | Young‐Woon Byeon | KyuJung Jun | Tanjin He | Wenhao Sun | Gerbrand Ceder
Source: Nature Synthesis (article, 2024-01-30)
Field: Materials Science — Materials Chemistry

Optimal thermodynamic conditions to minimize kinetic by-products in aqueous materials synthesis Abstract Phase diagrams offer substantial predictive power for materials synthesis by identifying the stability regions of target phases. However, thermodynamic phase diagrams do not offer explicit information regarding the kinetic competitiveness of undesired by-product phases. Here we propose a quantitative and computable thermodynamic metric to identify synthesis conditions under which the propensity to form kinetically competing by-products is minimized. We hypothesize that thermodynamic competition is minimized when the difference in free energy between a target phase and the minimal energy of all other competing phases is maximized. We validate this hypothesis for aqueous materials synthesis through two empirical approaches: first, by analysing 331 aqueous synthesis recipes text-mined from the literature; and second, by systematic experimental synthesis of LiIn(IO 3 ) 4 and LiFePO 4 across a wide range of aqueous electrochemical conditions. Our results show that even for synthesis conditions that are within the stability region of a thermodynamic Pourbaix diagram, phase-pure synthesis occurs only when thermodynamic competition with undesired phases is minimized. Aqueous solution ; Metric (unit) ; Pourbaix diagram ; Chemical stability ; Thermodynamics ; Phase diagram ; Kinetic energy ; Stability (learning theory) ; Phase (matter) ; Materials science ; Chemistry ; Electrochemistry ; Computer science ; Physical chemistry ; Physics ; Organic chemistry Machine Learning in Materials Science ; Electrocatalysts for Energy Conversion ; Chalcogenide Semiconductor Thin Films
Authors: Chloe J. Balhatchet | Jamie W. Gittins | Seung‐Jae Shin | Kangkang Ge | Xinyu Liu | Teedhat Trisukhon | Shivani Sharma | Thomas Kress | Pierre‐Louis Taberna | Patrice Simon | Aron Walsh | Alexander C. Forse
Source: Journal of the American Chemical Society (article, 2024-08-12)
Field: Chemistry — Inorganic Chemistry

Revealing Ion Adsorption and Charging Mechanisms in Layered Metal–Organic Framework Supercapacitors with Solid-State Nuclear Magnetic Resonance Conductive layered metal-organic frameworks (MOFs) have demonstrated promising electrochemical performances as supercapacitor electrode materials. The well-defined chemical structures of these crystalline porous electrodes facilitate structure-performance studies; however, there is a fundamental lack in the molecular-level understanding of charge storage mechanisms in conductive layered MOFs. To address this, we employ solid-state nuclear magnetic resonance (NMR) spectroscopy to study ion adsorption in nickel 2,3,6,7,10,11-hexaiminotriphenylene, Ni<sub>3</sub>(HITP)<sub>2</sub>. In this system, we find that separate resonances can be observed for the MOF's in-pore and ex-pore ions. The chemical shift of in-pore electrolyte is found to be dominated by specific chemical interactions with the MOF functional groups, with this result supported by quantum mechanics/molecular mechanics (QM/MM) and density functional theory (DFT) calculations. Quantification of the electrolyte environments by NMR was also found to provide a proxy for electrochemical performance, which could facilitate the rapid screening of synthesized MOF samples. Finally, the charge storage mechanism was explored using a combination of <i>ex-situ</i> NMR and <i>operando</i> electrochemical quartz crystal microbalance (EQCM) experiments. These measurements revealed that cations are the dominant contributors to charge storage in Ni<sub>3</sub>(HITP)<sub>2</sub>, with anions contributing only a minor contribution to the charge storage. Overall, this work establishes the methods for studying MOF-electrolyte interactions via NMR spectroscopy. Understanding how these interactions influence the charging storage mechanism will aid the design of MOF-electrolyte combinations to optimize the performance of supercapacitors, as well as other electrochemical devices including electrocatalysts and sensors. Chemistry ; Electrolyte ; Supercapacitor ; Electrochemistry ; Density functional theory ; Solid-state nuclear magnetic resonance ; Adsorption ; Chemical physics ; Electrode ; Nanotechnology ; Physical chemistry ; Computational chemistry ; Materials science ; Nuclear magnetic resonance Metal-Organic Frameworks: Synthesis and Applications ; Conducting polymers and applications ; Supercapacitor Materials and Fabrication
Authors: Minlong Wang | Jiaman Hou | Hainam Do | Chao Wang | Xiaohe Zhang | Ying Du | Qixin Dong | Lijun Wang | Ke Ni | Fazheng Ren | Jie An
Source: Nature Communications (article, 2024-08-10)
Field: Chemistry — Organic Chemistry

Intramolecular chalcogen bonding activated SuFEx click chemistry for efficient organic-inorganic linking SuFEx click chemistry demonstrates remarkable molecular assembly capabilities. However, the effective utilization of alkyl sulfonyl fluoride hubs in SuFEx chemistry, particularly in reactions with alcohols and primary amines, presents considerable challenges. This study pioneers an intramolecular chalcogen bonding activated SuFEx (S-SuFEx) click chemistry employing alkyl sulfonyl fluorides with γ-S as the activating group. The ChB-activated alkyl sulfonyl fluorides can react smoothly with phenols, alcohols, and amines, exhibiting enhanced reactivity compared to SO<sub>2</sub>F<sub>2</sub>. Excellent yields have been achieved with all 75 tested substrates. Pioneering the application of S-SuFEx chemistry, we highlight its immense potential in organic-inorganic linking, considering the critical role of interfacial covalent bonding in material fabrication. The S-SuFEx hub 1c, incorporating a trialkoxy silane group has been specifically designed and synthesized for organic-inorganic linking. In a simple step, 1c efficiently anchors various organic compounds onto surfaces of inorganic materials, forming functionalized surfaces with properties such as antibacterial activity, hydrophobicity, and fluorescence. Chalcogen ; Intramolecular force ; Click chemistry ; Chemistry ; Combinatorial chemistry ; Organic chemistry Click Chemistry and Applications ; Chemical Synthesis and Analysis ; Advanced biosensing and bioanalysis techniques
Authors: Seunghyuck Chi | Chaehoon Kim | Yongjin Lee | Minkee Choi
Source: JACS Au (article, 2024-03-29)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Diversity in Atomic Structures of Zeolite-Templated Carbons and the Consequences for Macroscopic Properties Zeolite-templated carbons (ZTCs) are a family of ordered microporous carbons with extralarge surface areas and micropore volumes, which are synthesized by carbon deposition within the confined spaces of zeolite micropores. There has been great controversy regarding the atomic structures of ZTCs, which encompass two extremes: (1) three-dimensionally connected curved open-blade-type carbon moieties and (2) ideal tubular structures (commonly referred to as "Schwarzites"). In this study, through a combination of experimental analyses and theoretical calculations, we demonstrate that the atomic structure of ZTCs is difficult to define as a single entity, and it widely varies depending on their synthesis conditions. Carbon deposition using a large organic precursor and low-temperature framework densification generates ZTCs predominantly composed of open-blade-type moieties, characterized by low surface curvature and abundant H-terminated edge sites. Meanwhile, synthesis using a small precursor with high-temperature densification produces ZTCs with an increased portion of closed-strut carbon moieties (or closed-fullerene-like nodes), exhibiting large surface curvature and diminished edge sites. The variations in the atomic structure of ZTCs result in significant differences in their macroscopic properties, such as N<sub>2</sub>/CO<sub>2</sub> adsorption, oxidative stability, work function, and electrocatalytic properties, despite the presence of comparable pore structures. Therefore, ZTCs demonstrate the potential to synthesize ordered nanoporous carbons with tunable physicochemical properties. Microporous material ; Materials science ; Carbon fibers ; Nanoporous ; Adsorption ; Chemical engineering ; Zeolite ; Nanotechnology ; Curvature ; Graphyne ; Chemical physics ; Catalysis ; Graphene ; Chemistry ; Organic chemistry ; Composite material ; Geometry Supercapacitor Materials and Fabrication ; Graphene research and applications ; Zeolite Catalysis and Synthesis
Authors: Jesús Ferrando‐Soria | Antonio Herrera
Source: Nano-Micro Letters (review, 2024-01-12)
Field: Chemistry — Inorganic Chemistry

Integrating Levels of Hierarchical Organization in Porous Organic Molecular Materials Porous organic molecular materials (POMMs) are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks, mainly held by non-covalent interactions. POMMs represent a variety of chemical families, such as hydrogen-bonded organic frameworks, porous organic salts, porous organic cages, C - H⋅⋅⋅π microporous crystals, supramolecular organic frameworks, π-organic frameworks, halogen-bonded organic framework, and intrinsically porous molecular materials. In some porous materials such as zeolites and metal organic frameworks, the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties. Therefore, considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials, we consider it appropriate to dedicate for the first time a critical review covering both topics. Herein, we will provide a summary of literature examples showcasing hierarchical POMMs, with a focus on their main synthetic approaches, applications, and the advantages brought forth by introducing hierarchy. Microporous material ; Porosity ; Supramolecular chemistry ; Porous medium ; Materials science ; Metal-organic framework ; Nanotechnology ; Hierarchy ; Molecule ; Organic chemistry ; Chemistry ; Composite material ; Adsorption Metal-Organic Frameworks: Synthesis and Applications ; Covalent Organic Framework Applications ; Luminescence and Fluorescent Materials
Authors: Nicolai Ree | Andreas H. Göller | Jan H. Jensen
Source: Digital Discovery (article, 2024-01-01)
Field: Chemistry — Organic Chemistry

Automated quantum chemistry for estimating nucleophilicity and electrophilicity with applications to retrosynthesis and covalent inhibitors Reactivity scales such as nucleophilicity and electrophilicity are valuable tools for determining chemical reactivity and selectivity. Nucleophile ; Electrophile ; Retrosynthetic analysis ; Covalent bond ; Chemistry ; Computational chemistry ; Computer science ; Stereochemistry ; Organic chemistry ; Total synthesis Chemical Reaction Mechanisms ; Organic Chemistry Cycloaddition Reactions ; Various Chemistry Research Topics
Authors: Selene Acosta | Mildred Quintana
Source: Sensors (article, 2024-03-12)
Field: Materials Science — Materials Chemistry

Chemically Functionalized 2D Transition Metal Dichalcogenides for Sensors The goal of the sensor industry is to develop innovative, energy-efficient, and reliable devices to detect molecules relevant to economically important sectors such as clinical diagnoses, environmental monitoring, food safety, and wearables. The current demand for portable, fast, sensitive, and high-throughput platforms to detect a plethora of new analytes is continuously increasing. The 2D transition metal dichalcogenides (2D-TMDs) are excellent candidates to fully meet the stringent demands in the sensor industry; 2D-TMDs properties, such as atomic thickness, large surface area, and tailored electrical conductivity, match those descriptions of active sensor materials. However, the detection capability of 2D-TMDs is limited by their intrinsic tendency to aggregate and settle, which reduces the surface area available for detection, in addition to the weak interactions that pristine 2D-TMDs normally exhibit with analytes. Chemical functionalization has been proposed as a consensus solution to these limitations. Tailored surface modification of 2D-TMDs, either by covalent functionalization, non-covalent functionalization, or a mixture of both, allows for improved specificity of the surface-analyte interaction while reducing van der Waals forces between 2D-TMDs avoiding agglomeration and precipitation. From this perspective, we review the recent advances in improving the detection of biomolecules, heavy metals, and gases using chemically functionalized 2D-TMDs. Covalent and non-covalent functionalized 2D-TMDs are commonly used for the detection of biomolecules and metals, while 2D-TMDs functionalized with metal nanoparticles are used for gas and Raman sensors. Finally, we describe the limitations and further strategies that might pave the way for miniaturized, flexible, smart, and low-cost sensing devices. Surface modification ; Nanotechnology ; Biomolecule ; Analyte ; Materials science ; Covalent bond ; Transition metal ; Chemistry ; Catalysis ; Organic chemistry 2D Materials and Applications ; Advanced biosensing and bioanalysis techniques ; MXene and MAX Phase Materials
Authors: M. Downes | Christopher E. Shuck | Ruocun Wang | Paweł Piotr Michałowski | Jonathan Shochat | Danzhen Zhang | Mikhail Shekhirev | Yizhou Yang | Nestor J. Zaluzec | Raúl Arenal | Steven J. May | Yury Gogotsi
Source: Journal of the American Chemical Society (article, 2024-10-31)
Field: Materials Science — Materials Chemistry

Synthesis of Three Isoelemental MXenes and Their Structure–Property Relationships The MXene family has rapidly expanded since its discovery in 2011 to include nearly 50 unique MXenes, not accounting for solid solutions and diverse surface terminations. However, a question raised since their discovery has been: What is the effect of <i>n</i>? In other words, how does the number of layers affect the MXene properties? To date, no direct study of the impact of <i>n</i> has been conducted due to the lack of isoelemental MXene compositions spanning more than two <i>n</i> values. Herein, we report on a system of three MXenes with identical M-site chemistries, (Mo<sub>2/3</sub>V<sub>1/3</sub>)<sub><i>n</i>+1</sub>C<sub><i>n</i></sub>T<sub><i>x</i></sub> (<i>n</i> = 1, 2, and 3), allowing for the study of MXene structure-property relationships across <i>n</i>, for the first time. Chemical analysis of the samples shows complete and partial ordering of the M-elements in the <i>n</i> = 2 and 3 samples, respectively. We show that sample stability gradually evolves as <i>n</i> is increased from 1 to 3, while electronic and electrochemical properties exhibit more significant changes in going from <i>n</i> = 1 to 2 than from <i>n</i> = 2 to 3. MXenes ; Chemistry ; Property (philosophy) ; Electrochemistry ; Physical chemistry ; Organic chemistry MXene and MAX Phase Materials ; 2D Materials and Applications ; Advanced Photocatalysis Techniques
Authors: Matthias Quintelier | Amirhossein Hajizadeh | Alexander Zintler | Bruna F. Gonçalves | Roberto Fernández de Luis | Leili Esrafili Dizaji | Christophe M. L. Vande Velde | Stefan Wuttke | Joke Hadermann
Source: Chemistry of Materials (article, 2024-07-22)
Field: Chemistry — Inorganic Chemistry

<i>In Situ</i> Study of the Activation Process of MOF-74 Using Three-Dimensional Electron Diffraction Metal-organic framework (MOF)-74 is known for its effectiveness in selectively capturing carbon dioxide (CO<sub>2</sub>). Especially the Zn and Cu versions of MOF-74 show high efficiency of this material for CO<sub>2</sub>. However, the activation of this MOF, which is a crucial step for its utilization, is so far not well understood. Here, we are closing the knowledge gap by examining the activation using, for the first time in the MOF, three-dimensional electron diffraction (3DED) during <i>in situ</i> heating. The use of state-of-the-art direct electron detectors enables rapid acquisition and minimal exposure times, therefore minimizing beam damage to the very electron beam-sensitive MOF material. The activation process of Zn-MOF-74 and Cu-MOF-74 is systematically studied <i>in situ</i>, proving the creation of open metal sites. Differences in thermal stability between Zn-MOF-74 and Cu-MOF-74 are attributed to the strength of the metal-oxygen bonds and Jahn-Teller distortions. In the case of Zn-MOF-74, we observe previously unknown remaining electrostatic potentials inside the MOF pores, which indicate the presence of remaining atoms that might impede gas flow throughout the structure when using the MOF for absorption purposes. We believe our study exemplifies the significance of employing advanced characterization techniques to enhance our material understanding, which is a crucial step for unlocking the full potential of MOFs in various applications. In situ ; Electron diffraction ; Materials science ; Diffraction ; Process (computing) ; Electron ; Chemical engineering ; Crystallography ; Nanotechnology ; Chemistry ; Computer science ; Physics ; Engineering ; Optics ; Organic chemistry ; Nuclear physics Metal-Organic Frameworks: Synthesis and Applications ; Inorganic Fluorides and Related Compounds ; Machine Learning in Materials Science
Authors: Zabiholah Damiri | Saeed Jafari | Saeed Yousefinejad | Hossein Kazemian
Source: Heliyon (article, 2024-05-01)
Field: Chemistry — Inorganic Chemistry

Enhanced adsorption of toluene on thermally activated ZIF-67: Characterization, performance, and modeling insights The zeolitic imidazolate framework-67 (ZIF-67) has been explored for the dynamic adsorption of toluene vapor. We synthesized ZIF-67 through a straightforward room-temperature process and characterized it using XRD, FT-IR, DLS, and SEM techniques. The synthesized ZIF-67 possessed a Brunauer-Emmett-Teller (BET) surface area of 1578.7 m<sup>2</sup>/g and 0.76 μm particle size. Thermal activation under various conditions revealed that ZIF-67, activated in dry air at 250 °C, demonstrated optimal adsorption efficacy. Its adsorption capacity, time of breakthrough, and time of equilibration were 414.5 mg/g, 420 min, and 795 min, respectively. We investigated the impact of diverse operational parameters on adsorption through breakthrough curve analysis. An increase in the toluene concentration from 100 to 1000 ppm enhanced the adsorption capacity from 171 to 414 mg/g, while breakthrough time decreased from 1260 min to 462 min, respectively. Our findings show that increasing relative humidity from 0 to 70 % reduced 53.7 % in adsorption capacity and 46.3 % in breakthrough time. The competitive adsorption of toluene and ethylbenzene revealed that ZIF-67 had a higher selectivity for toluene adsorption. A 98 % adsorbent's regeneration efficiency at the first cycle reveals its reusability. The experimental data were successfully fitted to the Yan, Thomas, and Yoon-Nelson models to describe the adsorption process. The statistical validation of the model parameters confirms their reliability for estimating adsorption parameters, thus facilitating the design of fixed-bed adsorption columns for practical applications. Adsorption ; Toluene ; Zeolitic imidazolate framework ; Ethylbenzene ; Chemical engineering ; Mesoporous material ; Materials science ; Chemistry ; Chromatography ; Metal-organic framework ; Organic chemistry ; Catalysis Metal-Organic Frameworks: Synthesis and Applications ; Covalent Organic Framework Applications ; Membrane Separation and Gas Transport
Authors: Christina Tang
Source: Materials (review, 2024-08-10)
Field: Chemistry — Organic Chemistry

Fundamental Aspects of Stretchable Mechanochromic Materials: Fabrication and Characterization Mechanochromic materials provide optical changes in response to mechanical stress and are of interest in a wide range of potential applications such as strain sensing, structural health monitoring, and encryption. Advanced manufacturing such as 3D printing enables the fabrication of complex patterns and geometries. In this work, classes of stretchable mechanochromic materials that provide visual color changes when tension is applied, namely, dyes, polymer dispersed liquid crystals, liquid crystal elastomers, cellulose nanocrystals, photonic nanostructures, hydrogels, and hybrid systems (combinations of other classes) are reviewed. For each class, synthesis and processing, as well as the mechanism of color change are discussed. To enable materials selection across the classes, the mechanochromic sensitivity of the different classes of materials are compared. Photonic systems demonstrate high mechanochromic sensitivity (Δnm/% strain), large dynamic color range, and rapid reversibility. Further, the mechanochromic behavior can be predicted using a simple mechanical model. Photonic systems with a wide range of mechanical properties (elastic modulus) have been achieved. The addition of dyes to photonic systems has broadened the dynamic range, i.e., the strain over which there is an optical change. For applications in which irreversible color change is desired, dye-based systems or liquid crystal elastomer systems can be formulated. While many promising applications have been demonstrated, manufacturing uniform color on a large scale remains a challenge. Standardized characterization methods are needed to translate materials to practical applications. The sustainability of mechanochromic materials is also an important consideration. Materials science ; Characterization (materials science) ; Fabrication ; Elastomer ; Nanotechnology ; Structural coloration ; Photonics ; Photonic crystal ; Composite material ; Optoelectronics Polydiacetylene-based materials and applications ; Nonlinear Optical Materials Studies ; Photochromic and Fluorescence Chemistry
Authors: Nerea Jiménez | Nicholas Ballard | José M. Asúa
Source: Macromolecular Materials and Engineering (review, 2024-02-27)
Field: Materials Science — Polymers and Plastics

Hard Coatings from Soft Latexes: A Review of Routes to Overcome the Film Formation Dilemma Abstract The use of polymer latexes for high‐performance coatings is challenging as the properties required to allow for film formation at reasonable temperatures tend to result in films with relatively poor mechanical properties. In this review, routes to overcome this so‐called film‐formation dilemma are discussed. First, the use of coalescing agents, focusing in particular on more recent approaches to minimize the use of volatile organic compounds (VOCs), is reviewed. Subsequently, approaches that utilize hybrid latexes are considered. This includes the use of high/low T g latex blends, nanocomposites that include a second, non‐polymeric phase, and multiphase latexes. Finally, the use of crosslinking technologies is considered, with a focus on necessary developments to reduce environmental impact. The review concludes with a summary and a discussion of possible future directions for research. Materials science ; Dilemma ; Nanocomposite ; Polymer ; Nanotechnology ; Phase (matter) ; Polymer science ; Composite material ; Organic chemistry Polymer composites and self-healing ; Polymer crystallization and properties ; Advanced Polymer Synthesis and Characterization