Rational design of a molecularly imprinted polymer for dinotefuran: theoretical and experimental studies aimed at the development of an efficient adsorbent for microextraction by packed sorbent

The Analyst ◽  
2018 ◽  
Vol 143 (1) ◽  
pp. 141-149 ◽  
Author(s):  
Camilla Fonseca Silva ◽  
Keyller Bastos Borges ◽  
Clebio Soares do Nascimento
Keyword(s):  
Molecularly Imprinted Polymer ◽  
Density Functional ◽  
Rational Design ◽  
Experimental Studies ◽  
Density Functional Theory Calculations ◽  
Imprinted Polymer ◽  
Functional Theory ◽  
Molecularly Imprinted ◽  
Functional Monomers ◽  
Packed Sorbent

In this work, we studied theoretically the formation process of a molecularly imprinted polymer (MIP) for dinotefuran (DNF), by testing distinct functional monomers (FM) in various solvents through density functional theory calculations.

Application of Response Surface Methodology to Synthesize Appropriate Molecularly Imprinted Polymer for Diazinon

2014 ◽  
Vol 605 ◽  
pp. 67-70 ◽  
Author(s):  
Mohsen Rahiminezhad ◽  
Seyed Jamaleddin Shahtaheri ◽  
Mohammad Reza Ganjali ◽  
Abbas Rahimi Rahimi Forushani
Keyword(s):  
Molecular Imprinting ◽  
Molecularly Imprinted Polymer ◽  
Binding Sites ◽  
Capillary Electrochromatography ◽  
Template Molecule ◽  
Imprinted Polymer ◽  
Molecularly Imprinted ◽  
Functional Monomers ◽  
Molecular Imprinting Technology ◽  
Cross Linker

Molecular imprinting technology has become an interesting research area to the preparation of specific sorbent material for environmental and occupational sample preparation techniques (1). In the molecular imprinting technology, specific binding sites have been formed in polymeric matrix, which often have an affinity and selectivity similar to antibody-antigen systems (2). In molecular imprinted technology, functional monomers are arranged in a complementary configuration around a template molecule, then, cross-linker and solvent are also added and the mixture is treated to give a porous material containing nono-sized binding sites. After extraction of the template molecule by washing, vacant imprinted sites will be left in polymer, which are available for rebinding of the template or its structural analogue (3). The stability, convention of preparation and low cost of these materials make them particularly attractive (4). These synthetic materials have been used for capillary electrochromatography (5), chromatography columns (6), sensors (7), and catalyze system (8). Depending on the molecular imprinting approach, different experimental variables such as the type and amounts of functional monomers, porogenic solvent, initiator, monomer to cross-linker ratio, temperature, and etc may alter the properties of the final polymeric materials. In this work, chemometric approach based on Central Composite Design (CCD) was used to design the experiments as well as to find the optimum conditions for preparing appropriate diazinon molecularly imprinted polymer.

scholarly journals Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts

2020 ◽  
Vol 6 (11) ◽  
pp. eaaz0510 ◽  
Author(s):  
Yonggang Yao ◽  
Zhenyu Liu ◽  
Pengfei Xie ◽  
Zhennan Huang ◽  
Tangyuan Li ◽  
...  
Keyword(s):  
Density Functional ◽  
Rational Design ◽  
Density Functional Theory Calculations ◽  
Great Promise ◽  
Alloy Formation ◽  
Functional Theory ◽  
Excellent Thermal Stability ◽  
Design And Synthesis ◽  
Highly Efficient ◽  
Computational Strategy

Multi-elemental alloy nanoparticles (MEA-NPs) hold great promise for catalyst discovery in a virtually unlimited compositional space. However, rational and controllable synthesize of these intrinsically complex structures remains a challenge. Here, we report the computationally aided, entropy-driven design and synthesis of highly efficient and durable catalyst MEA-NPs. The computational strategy includes prescreening of millions of compositions, prediction of alloy formation by density functional theory calculations, and examination of structural stability by a hybrid Monte Carlo and molecular dynamics method. Selected compositions can be efficiently and rapidly synthesized at high temperature (e.g., 1500 K, 0.5 s) with excellent thermal stability. We applied these MEA-NPs for catalytic NH3 decomposition and observed outstanding performance due to the synergistic effect of multi-elemental mixing, their small size, and the alloy phase. We anticipate that the computationally aided rational design and rapid synthesis of MEA-NPs are broadly applicable for various catalytic reactions and will accelerate material discovery.

scholarly journals Influence of Varying Functionalization on the Peroxidase Activity of Nickel(II)–Pyridine Macrocycle Catalysts: Mechanistic Insights from Density Functional Theory

Computation ◽  
2020 ◽  
Vol 8 (2) ◽  
pp. 52
Author(s):  
Jerwin Jay E. Taping ◽  
Junie B. Billones ◽  
Voltaire G. Organo
Keyword(s):  
Density Functional Theory ◽  
Proton Transfer ◽  
Density Functional ◽  
Experimental Studies ◽  
Density Functional Theory Calculations ◽  
Catalytic Performance ◽  
Stoichiometric Ratio ◽  
Functional Theory ◽  
Pendant Arm ◽  
Spin Singlet

Nickel(II) complexes of mono-functionalized pyridine-tetraazamacrocycles (PyMACs) are a new class of catalysts that possess promising activity similar to biological peroxidases. Experimental studies with ABTS (2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid), substrate) and H2O2 (oxidant) proposed that hydrogen-bonding and proton-transfer reactions facilitated by their pendant arm were responsible for their catalytic activity. In this work, density functional theory calculations were performed to unravel the influence of pendant arm functionalization on the catalytic performance of Ni(II)–PyMACs. Generated frontier orbitals suggested that Ni(II)–PyMACs activate H2O2 by satisfying two requirements: (1) the deprotonation of H2O2 to form the highly nucleophilic HOO−, and (2) the generation of low-spin, singlet state Ni(II)–PyMACs to allow the binding of HOO−. COSMO solvation-based energies revealed that the O–O Ni(II)–hydroperoxo bond, regardless of pendant arm type, ruptures favorably via heterolysis to produce high-spin (S = 1) [(L)Ni3+–O·]2+ and HO−. Aqueous solvation was found crucial in the stabilization of charged species, thereby favoring the heterolytic process over homolytic. The redox reaction of [(L)Ni3+–O·]2+ with ABTS obeyed a 1:2 stoichiometric ratio, followed by proton transfer to produce the final intermediate. The regeneration of Ni(II)–PyMACs at the final step involved the liberation of HO−, which was highly favorable when protons were readily available or when the pKa of the pendant arm was low.

scholarly journals Cation Involvement in Telomestatin Binding to G-Quadruplex DNA

2010 ◽  
Vol 2010 ◽  
pp. 1-7 ◽  
Author(s):  
Frédéric Rosu ◽  
Valérie Gabelica ◽  
Nicolas Smargiasso ◽  
Gabriel Mazzucchelli ◽  
Kazuo Shin-Ya ◽  
...  
Keyword(s):  
Density Functional ◽  
Rational Design ◽  
Density Functional Theory Calculations ◽  
Binding Mode ◽  
Monovalent Cation ◽  
Ammonium Ion ◽  
Mass Measurements ◽  
Functional Theory ◽  
Quadruplex Dna ◽  
G Quadruplex

The binding mode of telomestatin to G-quadruplex DNA has been investigated using electrospray mass spectrometry, by detecting the intact complexes formed in ammonium acetate. The mass measurements show the incorporation of one extra ammonium ion in the telomestatin complexes. Experiments on telomestatin alone also show that the telomestatin alone is able to coordinate cations in a similar way as a crown ether. Finally, density functional theory calculations suggest that in the G-quadruplex-telomestatin complex, potassium or ammonium cations are located between the telomestatin and a G-quartet. This study underlines that monovalent cation coordination capabilities should be integrated in the rational design of G-quadruplex binding ligands.

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