Determining kinetic reaction parameters with great detail has been of utmost importance in the field of chemical reaction engineering. However, commonly used experimental and computational methods however are unable to provide sufficiently resolved spatiotemporal information that can aid in the process of understanding these chemical reactions. With our work, we demonstrate the use of a custom designed single-bounce ATR-integrated microfluidic reactor to obtain spatiotemporal resolution for monitoring of chemical reactions. Having a single-bounce ATR accessory allows us to individually address different sensing areas, thereby providing the ability to obtain spatially and temporally resolved information. To further enhance the spatial resolution, we utilize the benefits of synchrotron IR radiation with the smallest beam spot-size ∼150 μm. An on-flow modular microreactor additionally allows us to monitor the chemical reaction , where the temporal characterization can be controlled with the operational flowrate. With a unique combination of experimental measurements and numerical simulations, we characterize and analyse a model S2 reaction. For a chemical reaction between benzyl bromide (BB) and sodium azide (SA) to produce benzyl azide (BA), we successfully show the capability of our device to determine the diffusion coefficients of BB and SA as 0.367 ± 0.115 10 m s and 1.17 ± 0.723 10 m s, respectively. Finally, with the above characteristics of our device, we also calculate a reaction rate of for the given chemical reaction.
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http://dx.doi.org/10.1039/d3lc00521f | DOI Listing |
ACS Appl Mater Interfaces
January 2025
Key Laboratory of Low Carbon Energy and Chemical Engineering of Gansu Province, Lanzhou 730050, China.
Na superionic conductor (NASICON)-structure NaMnV(PO) (NVMP) electrode materials reveal highly attractive application prospects due to ultrahigh energy density originating from two-electron reactions. Nevertheless, NVMP also encounters challenges with its poor electronic conductivity, Mn dissolution, and Jahn-Teller distortion. To address this issue, utilizing N-doped carbon layers and carbon nanotubes (CNTs) for dual encapsulation enhances the material's electronic conductivity, creating an effective electron transport network that promotes the rapid diffusion and storage of Na.
View Article and Find Full Text PDFAnalyst
January 2025
Anhui Provincial Key Laboratory of Biomedical Materials and Chemical Measurement, Laboratory of Functionalized Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, P. R. China.
It is highly required to rationally design fluorescent probes a molecular engineering strategy with desired analytical performance for applications in sensing and imaging. Reaction-based fluorescent probes for highly selective sensing of cysteine (Cys) are mainly based on the participation of Cys in reactions such as, addition-cyclization with acrylates, cyclization with aldehydes, coordination displacement, Michael addition reactions, and cleavage reactions. Cys-triggered reactions with the O atoms of ether bonds has also been used to construct reaction-based fluorescent probes based on the substitution of the ether with the nucleophilic thiolate of Cys.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill 27599, United States.
Architecturally hindered crystallization of bottlebrush graft copolymers offers a reaction- and solvent-free pathway for creating injectable elastomers with tissue-mimetic softness. Currently, injectable materials involve solvents and chemical reactions, leading to uncontrolled swelling, leaching of unreacted moieties, and side reactions with tissue. To address this issue, bottlebrush copolymers with a poly(ethylene glycol) (PEG) amorphous block and crystallizable poly(lactic acid) (PLA) grafted chains (A--B) were synthesized, with grafted chains of controlled length arranged along the backbone at controlled spacing.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, People's Republic of China.
Symmetric functions, such as Permutationally Invariant Polynomials (PIPs) and Fundamental Invariants (FIs), are effective and concise descriptors for incorporating permutation symmetry into neural network (NN) potential energy surface (PES) fitting. The traditional algorithm for generating such symmetric polynomials has a factorial time complexity of , where is the number of identical atoms, posing a significant challenge to applying symmetric polynomials as descriptors of NN PESs for larger systems, particularly with more than 10 atoms. Herein, we report a new algorithm which has only linear time complexity for identical atoms.
View Article and Find Full Text PDFOrg Lett
January 2025
Department of Chemistry, Ben-Gurion University of the Negev, Beer-Sheva 8410501, Israel.
A novel class of bis-8-aryl-isoquinoline () bis-alkylamine iron complexes, Fe()(OTf) and Fe()(OTf) ( = dipyrrolidinyl or = ,'-dimethylcyclohexyl-diamine), for asymmetric oxidation reactions is reported. The scalable divergent synthesis of 8-aryl-3-formylisoquinolines (), the key intermediates in preparing these ligands, enables precise structural and electronic tuning around the metal center. The enantioselective epoxidation and hydroxy carbonylation of conjugated alkenes, mediated by the Fe() catalyst with HO as the oxidant, demonstrates the potential of these redox Fe[N] catalysts in inducing face selection in oxygen transfer transformations.
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