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Suriyanarayanan, S., Olsson, G. D. & Nicholls, I. A. (2024). On-Surface Synthesis of Porosity-Controlled Molecularly Imprinted Polymeric Receptors for the Biotinyl Moiety. ACS Applied Polymer Materials, 6(2), 1470-1482
Open this publication in new window or tab >>On-Surface Synthesis of Porosity-Controlled Molecularly Imprinted Polymeric Receptors for the Biotinyl Moiety
2024 (English)In: ACS Applied Polymer Materials, E-ISSN 2637-6105, Vol. 6, no 2, p. 1470-1482Article in journal (Refereed) Published
Abstract [en]

Controlled on-surface synthesis of polymer films using amide-based, environmentally friendly, nonionic deep eutectic solvents (ni-DESs) has been developed to regulate the porous features of the films. An appropriate combination of acetamide (A), urea (U), and their methyl derivatives (N-methylacetamide (NMA) and N-methylurea (NMU)) was used to prepare ni-DES. Polymer films were electrosynthesized using 4-aminobenzoic acid (4-ABA) and pyrrole as monomers in ni-DESs. We presumed that the flickering-cluster-like complexes and the extended H-bond networks in ni-DESs enhance the porosity of the polymer films, thus improving permeability features, as reflected in sensor performance. Electrosynthesized polymer films, imprinted with biotin templates (MIPs), have been tested as receptors for biotinylated targets. Molecular dynamics simulations of the prepolymerization mixture revealed the formed complexes between 4-ABA and biotin comprising high-frequency H-bonds. X-ray photoelectron spectroscopy (XPS) and reflection absorption infrared spectroscopy (RAIRS) studies revealed the structural integrity in the polymer films irrespective of the medium. Scanning electron microscopy (SEM) and electrochemical impedance spectroscopy (EIS) measurements showed a highly corrugated and porous nature for MIPA-U and MIPNMU-U when prepared in A-U and NMU-U ni-DESs. Atomic force microscope (AFM) studies support these observations, displaying an enhancement in the surface roughness from 1.44 nm (MIPaqueous) to 23.6 nm (MIPNMU-U). QCM analysis demonstrated a remarkable improvement in sensitivity of MIPA-U (17.99 +/- 0.72 Hz/mM) and MIPNMU-U (18.40 +/- 0.81 Hz/mM) films toward the biotin methyl ester (BtOMe, biotin derivative) than the MIPaqueous film. The chemosensor devised with the above MIP recognition films selectively recognized BtOMe (LOD = 12.5 ng/mL) and biotinylated biomolecules, as shown by the stability constant K-s values (MIPA-U = 1442 and MIPNMU-U = 1502 M-1). The porous network generated in the polymer films by the flickering-cluster-like complexes present in the ni-DES facilitates the analyte diffusion and recognition. We propose this ni-DES as an economically advantageous and environmentally friendly alternative to conventional ionic liquids and organic solvents in polymer synthesis and to influence polymer morphology for developing hierarchical materials.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
Keywords
biotin biosensor, electropolymerization, molecularlyimprinted polymer, nonionic deep eutectic solvent, porous polymer films, quartz crystal microbalance
National Category
Polymer Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
urn:nbn:se:lnu:diva-127676 (URN)10.1021/acsapm.3c02655 (DOI)001152652200001 ()2-s2.0-85182006978 (Scopus ID)
Available from: 2024-02-14 Created: 2024-02-14 Last updated: 2024-02-14
Dhillon, P., Anaspure, P., Wiklander, J. G., Kathiravan, S. & Nicholls, I. A. (2023). Diyne-steered switchable regioselectivity in cobalt(ii)-catalysed C(sp(2))-H activation of amides with unsymmetrical 1,3-diynes. Organic and biomolecular chemistry, 21(9), 1942-1951
Open this publication in new window or tab >>Diyne-steered switchable regioselectivity in cobalt(ii)-catalysed C(sp(2))-H activation of amides with unsymmetrical 1,3-diynes
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2023 (English)In: Organic and biomolecular chemistry, ISSN 1477-0520, E-ISSN 1477-0539, Vol. 21, no 9, p. 1942-1951Article in journal (Refereed) Published
Abstract [en]

The regiochemical outcome of a cobalt(ii) catalysed C-H activation reaction of aminoquinoline benzamides with unsymmetrical 1,3-diynes under relatively mild reaction conditions can be steered through the choice of diyne. The choice of diyne provides access to either 3- or 4-hydroxyalkyl isoquinolinones, paving the way for the synthesis of more highly elaborate isoquinolines.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2023
National Category
Organic Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
urn:nbn:se:lnu:diva-119795 (URN)10.1039/d2ob02193e (DOI)000929089700001 ()36753336 (PubMedID)2-s2.0-85148443014 (Scopus ID)
Available from: 2023-03-16 Created: 2023-03-16 Last updated: 2023-05-31Bibliographically approved
Suriyanarayanan, S., Babu, M. P., Murugan, R., Muthuraj, D., Ramanujam, K. & Nicholls, I. A. (2023). Highly Efficient Recovery and Recycling of Cobalt from Spent Lithium-Ion Batteries Using an N-Methylurea-Acetamide Nonionic Deep Eutectic Solvent. ACS Omega, 8(7), 6959-6967
Open this publication in new window or tab >>Highly Efficient Recovery and Recycling of Cobalt from Spent Lithium-Ion Batteries Using an N-Methylurea-Acetamide Nonionic Deep Eutectic Solvent
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2023 (English)In: ACS Omega, E-ISSN 2470-1343, Vol. 8, no 7, p. 6959-6967Article in journal (Refereed) Published
Abstract [en]

The growing demand for lithium-ion batteries (LiBs) for the electronic and automobile industries combined with the limited availability of key metal components, in particular cobalt, drives the need for efficient methods for the recovery and recycling of these materials from battery waste. Herein, we introduce a novel and efficient approach for the extraction of cobalt, and other metal components, from spent LiBs using a nonionic deep eutectic solvent (ni-DES) comprised of N-methylurea and acetamide under relatively mild conditions. Cobalt could be recovered from lithium cobalt oxide-based LiBs with an extraction efficiency of >97% and used to fabricate new batteries. The N-methylurea was found to act as both a solvent component and a reagent, the mechanism of which was elucidated.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
National Category
Materials Chemistry Organic Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
urn:nbn:se:lnu:diva-120778 (URN)10.1021/acsomega.2c07780 (DOI)000964070600001 ()36844576 (PubMedID)2-s2.0-85148029223 (Scopus ID)
Available from: 2023-05-17 Created: 2023-05-17 Last updated: 2023-05-31Bibliographically approved
Kathiravan, S., Zhang, T. & Nicholls, I. A. (2023). Iridium catalysed C2 site-selective methylation of indoles using a pivaloyl directing group through weak chelation-assistance. RSC Advances, 13(17), 11291-11295
Open this publication in new window or tab >>Iridium catalysed C2 site-selective methylation of indoles using a pivaloyl directing group through weak chelation-assistance
2023 (English)In: RSC Advances, E-ISSN 2046-2069, Vol. 13, no 17, p. 11291-11295Article in journal (Refereed) Published
Abstract [en]

Here we present an iridium catalysed C2-selective methylation of indoles using methyltrifluoroborate as a source of methyl group. The iridium catalyst selectively discriminates the indole C2 and C4 C-H bonds by coordination with a pivaloyl directing group.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2023
National Category
Organic Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
urn:nbn:se:lnu:diva-120916 (URN)10.1039/d3ra02031b (DOI)000968938400001 ()37057266 (PubMedID)2-s2.0-85152919419 (Scopus ID)
Available from: 2023-05-26 Created: 2023-05-26 Last updated: 2023-09-07Bibliographically approved
Tasfaout, A., Ibrahim, F., Morrin, A., Brisset, H., Sorrentino, I., Nanteuil, C., . . . Branger, C. (2023). Molecularly imprinted polymers for per- and polyfluoroalkyl substances enrichment and detection. Talanta: The International Journal of Pure and Applied Analytical Chemistry, 258, Article ID 124434.
Open this publication in new window or tab >>Molecularly imprinted polymers for per- and polyfluoroalkyl substances enrichment and detection
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2023 (English)In: Talanta: The International Journal of Pure and Applied Analytical Chemistry, ISSN 0039-9140, E-ISSN 1873-3573, Vol. 258, article id 124434Article in journal (Refereed) Published
Abstract [en]

Per-and polyfluoroalkyl substances (PFAS) are highly toxic pollutants of significant concern as they are being detected in water, air, fish and soil. They are extremely persistent and accumulate in plant and animal tissues. Traditional methods of detection and removal of these substances use specialised instrumentation and require a trained technical resource for operation. Molecularly imprinted polymers (MIPs), polymeric materials with predetermined selectivity for a target molecule, have recently begun to be exploited in technologies for the selective removal and monitoring of PFAS in environmental waters. This review offers a comprehensive overview of recent developments in MIPs, both as adsorbents for PFAS removal and sensors that selectively detect PFAS at environmentally-relevant concentrations. PFAS-MIP adsorbents are classified according to their method of preparation (e.g., bulk or precipitation polymerization, surface imprinting), while PFAS-MIP sensing materials are described and discussed according to the transduction methods used (e.g., electrochemical, optical). This review aims to comprehensively discuss the PFAS-MIP research field. The efficacy and challenges facing the different applications of these materials in environmental water applications are discussed, as well as a perspective on challenges for this field that need to be overcome before exploitation of the technology can be fully realised.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Per-and polyfluoroalkyl substances (PFAS), Molecularly imprinted polymers (MIPs), Sensor, Adsorption, Environmental waters
National Category
Analytical Chemistry
Research subject
Chemistry, Analytical Chemistry
Identifiers
urn:nbn:se:lnu:diva-120766 (URN)10.1016/j.talanta.2023.124434 (DOI)000959279900001 ()36940572 (PubMedID)2-s2.0-85150281617 (Scopus ID)
Available from: 2023-05-17 Created: 2023-05-17 Last updated: 2023-05-31Bibliographically approved
Nilsson, P. H., Al-Majdoub, M., Ibrahim, A., Aseel, O., Suriyanarayanan, S., Andersson, L., . . . Nicholls, I. A. (2023). Quartz Crystal Microbalance Platform for SARS-CoV-2 Immuno-Diagnostics. International Journal of Molecular Sciences, 24(23), Article ID 16705.
Open this publication in new window or tab >>Quartz Crystal Microbalance Platform for SARS-CoV-2 Immuno-Diagnostics
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2023 (English)In: International Journal of Molecular Sciences, ISSN 1661-6596, E-ISSN 1422-0067, Vol. 24, no 23, article id 16705Article in journal (Refereed) Published
Abstract [en]

Rapid and accurate serological analysis of SARS-CoV-2 antibodies is important for assessing immune protection from vaccination or infection of individuals and for projecting virus spread within a population. The quartz crystal microbalance (QCM) is a label-free flow-based sensor platform that offers an opportunity to detect the binding of a fluid-phase ligand to an immobilized target molecule in real time. A QCM-based assay was developed for the detection of SARS-CoV-2 antibody binding and evaluated for assay reproducibility. The assay was cross-compared to the Roche electrochemiluminescence assay (ECLIA) Elecsys (R) Anti-SARS-CoV-2 serology test kit and YHLO's chemiluminescence immunoassay (CLIA). The day-to-day reproducibility of the assay had a correlation of r(2) = 0.99, p < 0.001. The assay linearity was r(2) = 0.96, p < 0.001, for dilution in both serum and buffer. In the cross-comparison analysis of 119 human serum samples, 59 were positive in the Roche, 52 in the YHLO, and 48 in the QCM immunoassay. Despite differences in the detection method and antigen used for antibody capture, there was good coherence between the assays, 80-100% for positive and 96-100% for negative test results. In summation, the QCM-based SARS-CoV-2 IgG immunoassay showed high reproducibility and linearity, along with good coherence with the ELISA-based assays. Still, factors including antibody titer and antigen-binding affinity may differentially affect the various assays' responses.

Place, publisher, year, edition, pages
MDPI, 2023
Keywords
chemiluminescence, COVID-19, electrochemiluminescence, quartz crystal microbalance, SARS-CoV-2
National Category
Immunology in the medical area
Research subject
Biomedical Sciences, Immunology
Identifiers
urn:nbn:se:lnu:diva-126262 (URN)10.3390/ijms242316705 (DOI)001117724600001 ()38069027 (PubMedID)2-s2.0-85179330180 (Scopus ID)
Available from: 2024-01-09 Created: 2024-01-09 Last updated: 2024-02-13Bibliographically approved
Durall, C., Wallinder, D., Ibrahim, A., Nolting, A., Almajdoub, M., Jones, N., . . . Aastrup, T. (2023). Robust QCM-Based Sensing and Assay Formats in Commercialized Systems. In: Springer Series on Chemical Sensors and Biosensors: Methods and Applications. Springer
Open this publication in new window or tab >>Robust QCM-Based Sensing and Assay Formats in Commercialized Systems
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2023 (English)In: Springer Series on Chemical Sensors and Biosensors: Methods and Applications, Springer, 2023Chapter in book (Refereed)
Abstract [en]

Attana’s Quartz Crystal Microbalance (QCM) analytical instruments have been developed to study in vitro biological interactions, mimicking the in vivo conditions. Attana’s superior technology for kinetic interaction studies allows to perform different assays, including biochemical, crude, sera, cell, and tissue-based, in vitro diagnostic and material chemistry assays, in real time and label free. With the focus to validate, select, and optimize drug candidates prior to clinical trials, Attana has helped pharmaceutical companies to increase their efficiency and profitability. In addition, the Attana instruments and services have been used in many other applications and research as described in this chapter.

Place, publisher, year, edition, pages
Springer, 2023
Series
Springer Series on Chemical Sensors and Biosensors, ISSN 1612-7617
National Category
Analytical Chemistry
Research subject
Chemistry, Analytical Chemistry
Identifiers
urn:nbn:se:lnu:diva-126083 (URN)10.1007/5346_2023_29 (DOI)
Available from: 2023-12-20 Created: 2023-12-20 Last updated: 2024-02-06Bibliographically approved
Suriyanarayanan, S., Mandal, S., Ramanujam, K. & Nicholls, I. A. (2023). Smart bio-nano interface derived from zein protein as receptors for biotinyl moiety. Talanta: The International Journal of Pure and Applied Analytical Chemistry, 256, Article ID 124298.
Open this publication in new window or tab >>Smart bio-nano interface derived from zein protein as receptors for biotinyl moiety
2023 (English)In: Talanta: The International Journal of Pure and Applied Analytical Chemistry, ISSN 0039-9140, E-ISSN 1873-3573, Vol. 256, article id 124298Article in journal (Refereed) Published
Abstract [en]

Proteinaceous, tunable nanostructures of zein (prolamine of corn) were developed as biotinyl-specific receptors using a molecular imprinting technique. Sacrificial templates, such as latex beads (LB3) and anodized alumina membrane (AAM), have been used to control nanostructural patterns in biotin-imprinted zein (BMZ). Briefly, a methanolic solution of the zein-biotin complex was drop cast upon a self-organized LB3 and AAM templates on Au/quartz surfaces. Subsequent dissolution of these sacrificial templates affords highly oriented, predetermined, and uniformly grown hyperporous (300 nm) and nanowires (150 nm) motifs of zein (BMZ-LB3 and BMZ-AAM), as shown by scanning electron microscopy (SEM). Selective extraction of biotin molecular template cast-off site -selective biotin imprints within these zein nanostructures complementary to biotinyl moieties. Alternatively, biotin-imprinted zein nanoparticles (BMZ-Np) and thin film (BMZ-MeOH) were prepared by coacervation and drop casting methods, respectively. Density functional theoretical (DFT) studies reveal strong hydrogen-bonded interaction of biotin with serine and glutamine residues of zein. Quartz crystal microbalance (QCM) studies show remarkable sensitivity of the hyperporous-BMZ-LB3 and nanowires of BMZ-AAM towards biotin derivative (biotin methyl ester) by five (24.75 +/- 1.34 Hz/mM) and four (18.19 +/- 0.75 Hz/mM) times, respectively, higher than the BMZ-MeOH. Enhanced permeability features of the zein nanostructures, when templated with LB3, enable the QCM detection of biotin-or its derivatives down to 12.9 ng mL-1 from dairy products (Kefir). The outcome of this study shall be a key aspect in interfacing biological materials with micro-/nano-sensors and electronic devices for detecting pertinent analytes using sustainably developed biopolymer-based nanostructures.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Zein, Protein nanostructures, Sacrificial template, Biotin-biosensor, Quartz crystal microbalance, Imprinted biopolymer
National Category
Biochemistry and Molecular Biology
Research subject
Chemistry, Biochemistry
Identifiers
urn:nbn:se:lnu:diva-119764 (URN)10.1016/j.talanta.2023.124298 (DOI)000926449800001 ()36701858 (PubMedID)2-s2.0-85146919249 (Scopus ID)
Available from: 2023-03-16 Created: 2023-03-16 Last updated: 2023-05-31Bibliographically approved
Suriyanarayanan, S., Kandregula, G. R., Ramanujam, K. & Nicholls, I. A. (2023). Sustainable synthesis of hierarchically grown chloramphenicol-imprinted poly(caffeic acid) nanostructured films. Journal of Applied Polymer Science, 140(9), Article ID e53560.
Open this publication in new window or tab >>Sustainable synthesis of hierarchically grown chloramphenicol-imprinted poly(caffeic acid) nanostructured films
2023 (English)In: Journal of Applied Polymer Science, ISSN 0021-8995, E-ISSN 1097-4628, Vol. 140, no 9, article id e53560Article in journal (Refereed) Published
Abstract [en]

Hierarchically nanostructured chloramphenicol (CLP) imprinted thin polymer films have been developed using a renewable monomer, the antioxidant caffeic acid (CA), using sacrificial nanostructures to induce porosity into the films. The poly(caffeic acid) (PCA) films were synthesized on Au/quartz resonators via greener polymerization conditions (clean energy electropolymerization in aqueous buffer or a non-ionic deep eutectic solvent). The sacrificial nanostructures explored included zein-based protein nanobeads, anodized alumina membrane, and Tween 20-derived polysorbate micelles, where dissolution of the sacrificial nanostructure templates from the PCA films afforded uniform long-range hyperporous networks, nanowires and nanoparticles, respectively, as revealed by SEM studies. Selective extraction of the CLP template from PCA films, was monitored by XPS, and afforded CLP selective cavities. The CLP-imprinted PCA(zein) films demonstrated eight- to 25-fold higher sensitivity than the other nanostructures in a QCM-sensor format, the limit of detection (LOD) under optimized FIA conditions was 50 mM. Significant sensitivities for CLP in milk were observed (1.5 mu g/ml to 3 mg/ml), covering the clinically relevant concentration range. The PCA(zein) thin films selectively differentiate CLP from structurally related antibiotics and are robust. Their production from renewable feedstocks of biological origin highlights the potential of this class of nanostructured materials for applications utilizing thin films.

Place, publisher, year, edition, pages
John Wiley & Sons, 2023
Keywords
chloramphenicol chemosensor, electropolymerization, molecularly imprinted polymer, Polycaffeic acid nanostructures, template directed synthesis
National Category
Materials Chemistry Polymer Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
urn:nbn:se:lnu:diva-118827 (URN)10.1002/app.53560 (DOI)000908053900001 ()2-s2.0-85146071440 (Scopus ID)
Available from: 2023-01-30 Created: 2023-01-30 Last updated: 2023-02-21Bibliographically approved
Mahajan, R., Suriyanarayanan, S., Olsson, G. D., Wiklander, J. G., Aastrup, T., Sellergren, B. & Nicholls, I. A. (2022). Oxytocin-Selective Nanogel Antibody Mimics. International Journal of Molecular Sciences, 23(5), Article ID 2534.
Open this publication in new window or tab >>Oxytocin-Selective Nanogel Antibody Mimics
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2022 (English)In: International Journal of Molecular Sciences, ISSN 1661-6596, E-ISSN 1422-0067, Vol. 23, no 5, article id 2534Article in journal (Refereed) Published
Abstract [en]

Oxytocin imprinted polymer nanoparticles were synthesized by glass bead supported solid phase synthesis, with NMR and molecular dynamics studies used to investigate monomer-template interactions. The nanoparticles were characterized by dynamic light scattering, scanning- and transmission electron microscopy and X-ray photoelectron spectroscopy. Investigation of nanoparticle-template recognition using quartz crystal microbalance-based studies revealed sub-nanomolar affinity, k(d) approximate to 0.3 +/- 0.02 nM (standard error of the mean), comparable to that of commercial polyclonal antibodies, k(d) approximate to 0.02-0.2 nM.

Place, publisher, year, edition, pages
MDPI, 2022
Keywords
molecular dynamics, molecularly imprinted polymer, nanoparticle, NMR, peptide imprinting, plastic antibody, oxytocin, solid-phase synthesis, QCM
National Category
Biochemistry and Molecular Biology
Research subject
Chemistry, Biochemistry
Identifiers
urn:nbn:se:lnu:diva-111046 (URN)10.3390/ijms23052534 (DOI)000769325200001 ()35269677 (PubMedID)2-s2.0-85125062528 (Scopus ID)2022 (Local ID)2022 (Archive number)2022 (OAI)
Available from: 2022-03-30 Created: 2022-03-30 Last updated: 2023-02-21Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0002-0407-6542

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