ORCID Profile
0000-0002-1340-902X
Current Organisation
VitalTrace Pty Ltd
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Publisher: Elsevier BV
Date: 09-2015
Publisher: The Electrochemical Society
Date: 09-10-2022
DOI: 10.1149/MA2022-02542053MTGABS
Abstract: A sustainable future requires an energy sector led by renewable sources, especially energy conversion and storage (ECS). Advances in the design and synthesis of nanomaterials, like conducting polymers [1], are critical for future development. An ex le for this type of material is poly-(3,4-ethylenedioxythiophene) (PEDOT), ideally known for energy applications as a thin film due to its excellent properties (e.g., tunable conductivity, flexibility, and transparency) [2]. However, current manufacturing methods require additives, like surfactants, that affect their properties, leading to decreased performance [3]. The use of liquid-liquid interfaces continues to grow as a viable platform for nanomaterial film synthesis with impressive structural properties [4]. Since several such interfaces are electrochemically active [5], providing external stimulus at these interfaces can fine tune the electric field to enhance interfacial electrosynthesis or self-assembly. This has the potential to produce free-floating films that can be transferred to any solid support with ease for device fabrication. The ability to form thin films directly in a single step will eliminate the need for additives such as surfactants. To explore this, we have investigated the use of Fenton chemistry (H 2 O 2 in the presence of a ferrous compound) as the oxidant to polymerize PEDOT at the liquid-liquid interface. This combination offers the advantages of interfacial electropolymerization with a “greener” oxidant. We used cyclic voltammetry (CV) to study PEDOT formation at the interface under different pHs, molar ratios, and solvent conditions. Repetitive cycling at pH 1.5 - 2 (~10mM HCl) shows the growth of the electrical double layer with each successive cycle as a peak (around ca . -0.1 V vs Ag/AgCl) is growing accordingly until a blue material (PEDOT) is observed at the interface. This is liken to CVs observed for CP electropolymerization on typical solid electrodes [6]. However, this potentiodynamic method takes more than ~5 hours so we also explored chrono erometry to hasten the film formation and control film thickness. Applying constant potential ( ca . 1.25 V vs Ag/AgCl) allowed film formation even after ~60 mins, and the film thickness also varies with time. The properties of produced films were then characterized using electrochemistry, SEM, XPS, RAMAN, and ex-situ conductivity. As a proof-of-concept, we demonstrate that Fenton chemistry is a viable alternative to produce PEDOT at the liquid-liquid interface. The latest results on PEDOT interfacial electropolymerization using Fenton chemistry and its characterization will be presented and discussed. Literature: [1] Q. Meng, et. al., Nano Energy, 2017, 36, 268–285. [2] M. N. Gueye, et. al., Chem. Mater., 2016, 28, 3462–3468. [3] A. Köhler and H. Bässler, Electron. Struct. Org. Semicond., 2015, 307–388. [4] J. Forth, et. al., Adv. Mater., 2019, 1806370, 1806370. [5] L. Rivier, et. al., Angew. Chemie Int. Ed., 2017, 56, 2324–2327. [6] J. Heinze, et al., Chem. Rev. 2010, 110 (8), 4724–4771 Figure 1
Publisher: American Chemical Society (ACS)
Date: 12-06-2018
DOI: 10.1021/ACS.ANALCHEM.8B01172
Abstract: The electrochemical behavior of a synthetic oligonucleotide, thrombin-binding aptamer (TBA, 15-mer), was explored at a liquid-organogel microinterface array. TBA did not display any response when only background electrolytes were present in both phases. On the basis of literature reports that surfactants can influence nucleic acid detection, the response in the presence of cetyltrimethylammonium (CTA
Publisher: Elsevier BV
Date: 12-2019
DOI: 10.1016/J.ACA.2019.08.016
Abstract: This review critically discusses the developments on open-tubular liquid chromatography (OT-LC) and open-tubular capillary electrochromatography (OT-CEC) during 2014-2018. An appropriate Scopus search revealed 5 reviews, 4 theoretical papers on open-tubular format chromatography, 29 OT-LC articles, 68 OT-CEC articles and 4 OT-LC/OT-CEC articles, indicating a sustained interest in these areas. The open-tubular format typically uses a capillary column with inner walls that are coated with an le layer or coating of solid stationary phase material. The ratio between the capillary internal diameter and coating thickness (CID/CT) is ideally ≤ 100 for appropriate chromatographic retention. We, therefore, approximated the CID/CT ratios and found that 22 OT-LC papers have CID/CT ratios ≤100. The other 7 OT-LC papers have CID/CT ratio >100 but have clearly demonstrated chromatographic retention. These 29 papers utilised reversed phase or ion exchange mechanisms using known or innovative solid stationary phase materials (e.g. metal organic frameworks), stationary pseudophases from ionic surfactants or porous supports. On the other hand, we found that 68 OT-CEC papers, 7 OT-LC papers and 4 OT-LC & OT-CEC papers have CID/CT ratios >100. Notably, 44 papers (42 OT-CEC and 2 OT-LC & OT-CEC) did not report the retention factor and/or effective electrophoretic mobility of analytes. Considering all covered papers, the most popular activity was on the development of new chromatographic materials as coatings. However, we encourage OT-CEC researchers to not only characterise changes in the electroosmotic flow but also verify the interaction of the analytes with the coating. In addition, the articles reported were largely driven by stationary phase or support development and not by practical applications.
Publisher: American Chemical Society (ACS)
Date: 03-08-2018
DOI: 10.1021/ACS.ANALCHEM.8B01710
Abstract: The electrochemical behavior and detection of sulfated carbohydrates were investigated at an array of microinterfaces between two immiscible electrolyte solutions where the organic phase was gelled. It was found that the electrochemical signal was dependent on the organic phase electrolyte cation. Cyclic voltammetry (CV) of sucrose octasulfate (SOS) with bis(triphenylphosphoranylidene)ammonium BTPPA
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7AN00761B
Abstract: The electrochemical behaviour of fucoidan, a sulfated polysaccharide, was investigated, leading to a detection strategy by adsorptive stripping voltammetry.
Publisher: Elsevier BV
Date: 11-2021
Publisher: American Chemical Society (ACS)
Date: 08-04-2019
DOI: 10.1021/ACS.LANGMUIR.8B04227
Abstract: The electroadsorption of proteins at aqueous-organic interfaces offers the possibility to examine protein structural rearrangements upon interaction with lipophilic phases, without modifying the bulk protein or relying on a solid support. The aqueous-organic interface has already provided a simple means of electrochemical protein detection, often involving adsorption and ion complexation however, little is yet known about the protein structure at these electrified interfaces. This work focuses on the interaction between proteins and an electrified aqueous-organic interface via controlled protein electroadsorption. Four proteins known to be electroactive at such interfaces were studied: lysozyme, myoglobin, cytochrome c, and hemoglobin. Following controlled protein electroadsorption onto the interface, ex situ structural characterization of the proteins by FTIR spectroscopy was undertaken, focusing on secondary structural traits within the amide I band. The structural variations observed included unfolding to form aggregated antiparallel β-sheets, where the rearrangement was specifically dependent on the interaction with the organic phase. This was supported by MALDI ToF MS measurements, which showed the formation of protein-anion complexes for three of these proteins, and molecular dynamic simulations, which modeled the structure of lysozyme at an aqueous-organic interface. On the basis of these findings, the modulation of protein secondary structure by interfacial electrochemistry opens up unique prospects to selectively modify proteins.
No related grants have been discovered for Bren Mark Felisilda.