Imprinted Oxide and MIP/Oxide Hybrid Nanomaterials for Chemical Sensors †

Afzal, Adeel; Dickert, Franz L.

doi:10.3390/nano8040257

Cited by 17 publications

(6 citation statements)

References 197 publications

(228 reference statements)

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“… 20 Molecularly imprinted inorganic structures, although typically more difficult to prepare due to harsher synthetic conditions, making retention of the templated structure more challenging, have in fact been developed previously. 21 , 22 Imprinted oxides have been shown to induce spatial resolution for adsorptive, catalytic, and electronic applications. 23 , 24 A third group of processes, which can be employed either pre- or postsynthesis, is called kinetic resolution.…”

Section: Introductionmentioning

confidence: 99%

“…Chiral imprinting in organic polymers was proposed as an alternative approach to the common chiral chromatography columns, as well as to membrane-based and other retention-based separation techniques. ,− Chirally imprinted polymers have also been used for sensing applications. , Nevertheless, imprinted polymers may lack structural stability, especially at elevated temperatures . Molecularly imprinted inorganic structures, although typically more difficult to prepare due to harsher synthetic conditions, making retention of the templated structure more challenging, have in fact been developed previously. , Imprinted oxides have been shown to induce spatial resolution for adsorptive, catalytic, and electronic applications. , A third group of processes, which can be employed either pre- or postsynthesis, is called kinetic resolution. This is a group of many different reactions which selectively favor one enantiomer over the other, for either the production of the target molecule or its further reaction into easily separable products. , …”

Section: Introductionmentioning

confidence: 99%

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Kinetic Resolution of Racemic Mixtures via Enantioselective Photocatalysis

Arbell

Bauer

Paz

2021

ACS Appl. Mater. Interfaces

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Despite the increasing demand for enantiopure drugs in the pharmaceutical industry, currently available chiral separation technologies are still lagging behind, whether due to throughput or to operability considerations. This paper presents a new kinetic resolution method, based on the specific adsorption of a target enantiomer onto a molecularly imprinted surface of a photocatalyst and its subsequent degradation through a photocatalytic mechanism. The current model system is composed of an active TiO 2 layer, on which the target enantiomer is adsorbed. A photocatalytic suppression layer of Al 2 O 3 is then grown around the adsorbed target molecules by atomic layer deposition. Following the removal of the templating molecules, molecularly imprinted cavities that correspond to the adsorbed species are formed. The stereospecific nature of these pores encourages enantioselective degradation of the undesired species through its enhanced adsorption on the photocatalyst surface, while dampening nonselective photocatalytic activity around the imprinted sites. The method, demonstrated with the dipeptide leucylglycine as a model system, revealed a selectivity factor of up to 7 and an enrichment of a single enantiomer to 85% from an initially racemic mixture. The wide range of parameters that can be optimized (photocatalyst, concentration of imprinted sites, type of passivating layer, etc.) points to the great potential of this method for obtaining enantiomerically pure compounds, beginning from racemic mixtures.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Kinetic Resolution of Racemic Mixtures via Enantioselective Photocatalysis

Arbell

Bauer

Paz

2021

ACS Appl. Mater. Interfaces

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“…However, the MIPs are versatile robust polymers, which can be easily tailored for fast, selective separations. The imprinting technique was primarily introduced to improve selectivity in the chromatographic separations, but nowadays, the technique finds immense use in several toxic remediations such as heavy metal ion such as Cu(II), Hg(II), Pb(II), etc., or anions such as phosphate extraction from waste water by preparing their corresponding MIPs. − The MIPs can be used for recognition of not only metal ions (commonly called as ion imprinted polymers (IIPs)) but also for biological molecules such as proteins, amino acids, etc., , as sensors ,, and in drug delivery. , The selective recognition sites in MIPs/IIPs are based on the size, structure, and functional groups of the analyte of interest. The first step for MIP/IIPs synthesis requires bulk complex formation of the target analyte with the appropriate functional monomers, commonly referred to as the target specific template.…”

Section: Introductionmentioning

confidence: 99%

Phosphate-based Ce(IV) Ion-Imprinted Polymers for Separation of Berkelium: Testing the Homologue Imprinting Approach for Heavy Actinides

Mhatre

Agarwal

Nag

et al. 2021

ACS Appl. Polym. Mater.

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The present study focuses on the synthesis of phosphate-based ion imprinted polymers (IIPs) using a chemical homologue (cerium(IV)) for the fast and selective separation of Bk(IV) from a large number of fission products. Two imprinted phosphate-based gels, poly(bis[2-(methacryloyloxy)ethyl] phosphate) (poly-BMEP) and poly(bis[2-(methacryloyloxy)ethyl] phosphate-co-acrylic acid) (poly-(BMEP-AA)) have been prepared by in situ UV polymerization. The imprinting has been achieved by complexation of the phosphate-based monomers with the Ce(IV) ion. The desorption of Ce(IV) ions from the imprinted gels has been studied with H2O2. The prepared gels have been characterized by FE-SEM, FT-IR, XRD, and XPS. The imprinted gels have been shown to extract Ce(IV) ions selectively from an 8 mol L–1 HNO3 medium in the presence of fission products (Ba, Ru, Tb). DFT calculations show formation of a 1:4 Ce(IV):BMEP complex. The presence of acrylic acid (AA) has been shown to improve the kinetics of Ce(IV) uptake owing to the decrease in the tortuosity of the polymeric structure due to the AA presence. The imprinted gels though do not show kinetic selectivity toward Ce(IV) compared to non-imprinted gels; they show thermodynamic selectivity toward Ce(IV), indicating the inability of the non-imprinted gels to retain Ce(IV) for longer periods. Also, the imprinted gels have been found to be more selective compared to solvent extraction with BMEP as the complexing agent. These two imprinted gels were used to extract Bk, which was produced in 11B + 238U at a 66 MeV beam energy. The extraction by IIPs have been found to be much faster with the reduction in overall extraction time by ∼80% relative to the earlier reported method though with a lesser selectivity for some elements. The present approach, as guided by DFT calculations, offers a possibility of preparing IIPs for the selective extraction of heavy actinides and trans-actinides using their chemical homologues as the imprinting ion.

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“…MIPs were synthesized by non-covalent methods and implemented for the first time in the 1970s by Mosbach and his group [1]. MIPs as capable materials with high specificity, and their physical and chemical stability have been effectively used in the extraction, and microextraction fields and even in sensing applications [2,3,4,5,6,7,8,9,10,11,12,13,14,15]. The common MIP preparation methods require organic monomers (acrylates or acrylic acid) and an organic solution phase which represent limitations from environmental and biological points of view.…”

Section: Introductionmentioning

confidence: 99%

Recent Applications of Molecularly Imprinted Sol-Gel Methodology in Sample Preparation

2019

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Due to their selectivity and chemical stability, molecularly imprinted polymers have attracted great interest in sample preparation. Imprinted polymers have been applied for the extraction and the enrichment of different sorts of trace analytes in biological and environmental samples before their analysis. Additionally, MIPs are utilized in various sample preparation techniques such as SPE, SPME, SBSE and MEPS. Nevertheless, molecularly imprinted polymers suffer from thermal (stable only up to 150 °C) and mechanical stability issues, improper porosity and poor capacity. The sol-gel methodology as a promising alternative to address these limitations allowing the production of sorbents with controlled porosity and higher surface area. Thus the combination of molecularly imprinted technology and sol-gel technology can create influential materials with high selectivity, high capacity and high thermal stability. This work aims to present an overview of molecularly imprinted sol-gel polymerization methods and their applications in analytical and bioanalytical fields.

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Imprinted Oxide and MIP/Oxide Hybrid Nanomaterials for Chemical Sensors †

Cited by 17 publications

References 197 publications

Kinetic Resolution of Racemic Mixtures via Enantioselective Photocatalysis

Kinetic Resolution of Racemic Mixtures via Enantioselective Photocatalysis

Phosphate-based Ce(IV) Ion-Imprinted Polymers for Separation of Berkelium: Testing the Homologue Imprinting Approach for Heavy Actinides

Recent Applications of Molecularly Imprinted Sol-Gel Methodology in Sample Preparation

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