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Publications (10 of 21) Show all publications
Sandin, S., Hamad, A. A., Cuartero, M., de Marco, R., Crespo, G. A., Backström, J. & Cornell, A. M. (2020). Deactivation and selectivity for electrochemical ozone production at Ni- and Sb-doped SnO2 / Ti electrodes. Electrochimica Acta, 335, Article ID 135645.
Open this publication in new window or tab >>Deactivation and selectivity for electrochemical ozone production at Ni- and Sb-doped SnO2 / Ti electrodes
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2020 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 335, article id 135645Article in journal (Refereed) Published
Abstract [en]

This work reports on a time-resolved study of the deactivation of electrochemical ozone production (EOP) active anodes using a novel approach to measure total ozone production. The reproducibility and change of the electrodes over time have been investigated using a number of electrochemical and physical techniques. The dissolution of antimony from the surface of the nickel- and antimony-doped tin oxide (NATO) electrode is the main process behind the deactivation of the EOP. When surface antimony is depleted, the continued deactivation seems to be connected to the dissolution of nickel. Despite tin (from the coating) and titanium (from the substrate) continuously dissolving during galvanostatic polarization of the NATO electrode, our experiments point to no connection between these processes and the EOP activity. In addition, the selectivity of the electrode is affected by electrolyte penetration, accessing fresh reaction sites that are active on the EOP. The results indicate that both antimony (III) and nickel present at the surface of the NATO are responsible for the EOP activity.

Place, publisher, year, edition, pages
PERGAMON-ELSEVIER SCIENCE LTD, 2020
Keywords
Ozone, NATO, Tin oxide anode, Anode deactivation mechanisms, Selectivity
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-269023 (URN)10.1016/j.electacta.2020.135645 (DOI)000511293800020 ()2-s2.0-85078059874 (Scopus ID)
Note

QC 20200313

Available from: 2020-03-13 Created: 2020-03-13 Last updated: 2020-03-13Bibliographically approved
Ciftci, S., Cánovas, R., Neumann, F., Paulraj, T., Nilsson, M., Crespo, G. A. & Madaboosi, N. (2020). The sweet detection of rolling circle amplification: Glucose-based electrochemical genosensor for the detection of viral nucleic acid. Biosensors & bioelectronics, 151, Article ID 112002.
Open this publication in new window or tab >>The sweet detection of rolling circle amplification: Glucose-based electrochemical genosensor for the detection of viral nucleic acid
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2020 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 151, article id 112002Article in journal (Refereed) Published
Abstract [en]

Herein, an isothermal padlock probe-based assay for the simple and portable detection of pathogens coupled with a glucose oxidase (GOx)-based electrochemical readout is reported. Infectious diseases remain a constant threat on a global scale, as in recurring pandemics. Rapid and portable diagnostics hold the promise to tackle the spreading of diseases and decentralising healthcare to point-of-care needs. Ebola, a hypervariable RNA virus causing fatalities of up to 90% for recent outbreaks in Africa, demands immediate attention for bedside diagnostics. The design of the demonstrated assay consists of a rolling circle amplification (RCA) technique, responsible for the generation of nucleic acid amplicons as RCA products (RCPs). The RCPs are generated on magnetic beads (MB) and subsequently, connected via streptavidin-biotin bonds to GOx. The enzymatic catalysis of glucose by the bound GOx allows for an indirect electrochemical measurement of the DNA target. The RCPs generated on the surface of the MB were confirmed by scanning electron microscopy, and among other experimental conditions such as the type of buffer, temperature, concentration of GOx, sampling and measurement time were evaluated for the optimum electrochemical detection. Accordingly, 125 μg mL−1 of GOx with 5 mM glucose using phosphate buffer saline (PBS), monitored for 1 min were selected as the ideal conditions. Finally, we assessed the analytical performance of the biosensing strategy by using clinical samples of Ebola virus from patients. Overall, this work provides a proof-of-concept bioassay for simple and portable molecular diagnostics of emerging pathogens using electrochemical detection, especially in resource-limited settings.

Place, publisher, year, edition, pages
Elsevier Ltd, 2020
Keywords
Chronoamperometric readout, Ebola virus, Glucose oxidase, Molecular diagnostics, Point-of-care, Rolling-circle-amplification (RCA), Diagnosis, Diseases, Glucose, Glucose sensors, Nucleic acids, Product design, Scanning electron microscopy, Viruses, Point of care, Rolling circle amplifications, Chemical detection, biotin, buffer, phosphate buffered saline, streptavidin, virus DNA, Africa, amplicon, analytical parameters, Article, bioassay, biological monitoring, catalysis, concentration (parameter), controlled study, Ebola hemorrhagic fever, Ebolavirus, electrochemical detection, enzyme binding, epidemic, gene targeting, isotherm, magnetism, measurement, molecular probe, nonhuman, nucleic acid amplification, pandemic, point of care testing, rolling circle amplification, sampling, surface property, temperature sensitivity
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-272254 (URN)10.1016/j.bios.2019.112002 (DOI)31999596 (PubMedID)2-s2.0-85077655413 (Scopus ID)
Note

QC 20200421

Available from: 2020-04-21 Created: 2020-04-21 Last updated: 2020-04-21Bibliographically approved
Liu, Y., Canovas, R., Crespo, G. A. & Cuartero, M. (2020). Thin-Layer Potentiometry for Creatinine Detection in Undiluted Human Urine Using Ion-Exchange Membranes as Barriers for Charged Interferences. Analytical Chemistry, 92(4), 3315-3323
Open this publication in new window or tab >>Thin-Layer Potentiometry for Creatinine Detection in Undiluted Human Urine Using Ion-Exchange Membranes as Barriers for Charged Interferences
2020 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 92, no 4, p. 3315-3323Article in journal (Refereed) Published
Abstract [en]

Herein, thin-layer potentiometry combined with ion-exchange membranes as barriers for charged interferences is demonstrated for the analytical detection of creatinine (CRE) in undiluted human urine. Briefly, CRE diffuses through an anion-exchange membrane (AEM) from a sample contained in one fluidic compartment to a second reservoir, containing the enzyme CRE deiminase. There, CRE reacts with the enzyme, and the formation of ammonium is dynamically monitored by potentiometric ammonium-selective electrodes. This analytical concept is integrated into a lab-on-a-chip microfluidic cell that allows for a high sample throughput and the operation under stop-flow mode, which allows CRE to passively diffuse across the AEM. Conveniently, positively charged species (i.e., potassium, sodium, and ammonium, among others) are repelled by the AEM and never reach the ammonium-selective electrodes; thus, possible interference in the response can be avoided. As a result, the dynamic potential response of the electrodes is entirely ascribed to the stoichiometric formation of ammonium. The new CRE biosensor exhibits a Nernstian slope, within a linear range of response from 1 to 50 mM CRE concentration. As expected, the response time (15-60 min) primarily depends on the CRE diffusion across the AEM. CRE analysis in urine samples displayed excellent results, without requiring sample pretreatment (before the introduction of the sample in the microfluidic chip) and with high compatibility with development into a potential point-of-care clinical tool. In an attempt to decrease the analysis time, the presented analytical methodology for CRE detection is translated into an all-solid-state platform, in which the enzyme is immobilized on the surface of the ammonium-selective electrode and with the AEM on top. While more work is necessary in this direction, the CRE sensor appears to be promising for CRE analysis in both urine and blood.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2020
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-271290 (URN)10.1021/acs.analchem.9b05231 (DOI)000514758900056 ()2-s2.0-85080930359 (Scopus ID)
Note

QC 20200402

Available from: 2020-04-02 Created: 2020-04-02 Last updated: 2020-04-02Bibliographically approved
Canovas, R., Sanchez, S. P., Parrilla, M., Cuartero, M. & Crespo, G. A. (2019). Cytotoxicity Study of Ionophore-Based Membranes: Toward On Body and in Vivo Ion Sensing. ACS SENSORS, 4(9), 2524-2535
Open this publication in new window or tab >>Cytotoxicity Study of Ionophore-Based Membranes: Toward On Body and in Vivo Ion Sensing
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2019 (English)In: ACS SENSORS, ISSN 2379-3694, Vol. 4, no 9, p. 2524-2535Article in journal (Refereed) Published
Abstract [en]

We present the most complete study to date comprising in vitro cytotoxicity tests of ion-selective membranes (ISMs) in terms of cell viability, proliferation, and adhesion assays with human dermal fibroblasts. ISMs were prepared with different types of plasticizers and ionophores to be tested in combination with assays that focus on the medium-term and long-term leaching of compounds. Furthermore, the ISMs were prepared in different configurations considering (i) inner-filling solution-type electrodes, (ii) all-solid-state electrodes based on a conventional drop-cast of the membrane, (iii) peeling after the preparation of a wearable sensor, and (iv) detachment from a microneedle-based sensor, thus covering a wide range of membrane shapes. One of the aims of this study, other than the demonstration of the biocompatibility of various ISMs and materials tested herein, is to create an awareness in the scientific community surrounding the need to perform biocompatibility assays during the the very first steps of any sensor development with an intended biomedical application. This will foster meeting the requirements for subsequent on-body application of the sensor and avoiding further problems during massive validations toward the final in vivo use and commercialization of such devices.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
Keywords
biocompatibility, cytotoxicity tests, ion-selective electrodes, biomedical applications, point-of-care
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-262801 (URN)10.1021/acssensors.9b01322 (DOI)000488424100039 ()31448593 (PubMedID)2-s2.0-85072673080 (Scopus ID)
Note

QC 20191021

Available from: 2019-10-21 Created: 2019-10-21 Last updated: 2019-10-21Bibliographically approved
Meng, Q., Zhang, B., Fan, L., Liu, H., Valvo, M., Edström, K., . . . Sun, L. (2019). Efficient BiVO4 Photoanodes by Postsynthetic Treatment: Remarkable Improvements in Photoelectrochemical Performance from Facile Borate Modification. Angewandte Chemie International Edition, 58(52), 19027-19033
Open this publication in new window or tab >>Efficient BiVO4 Photoanodes by Postsynthetic Treatment: Remarkable Improvements in Photoelectrochemical Performance from Facile Borate Modification
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2019 (English)In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 58, no 52, p. 19027-19033Article in journal (Refereed) Published
Abstract [en]

Water-splitting photoanodes based on semiconductor materials typically require a dopant in the structure and co-catalysts on the surface to overcome the problems of charge recombination and high catalytic barrier. Unlike these conventional strategies, a simple treatment is reported that involves soaking a sample of pristine BiVO4 in a borate buffer solution. This modifies the catalytic local environment of BiVO4 by the introduction of a borate moiety at the molecular level. The self-anchored borate plays the role of a passivator in reducing the surface charge recombination as well as that of a ligand in modifying the catalytic site to facilitate faster water oxidation. The modified BiVO4 photoanode, without typical doping or catalyst modification, achieved a photocurrent density of 3.5 mA cm−2 at 1.23 V and a cathodically shifted onset potential of 250 mV. This work provides an extremely simple method to improve the intrinsic photoelectrochemical performance of BiVO4 photoanodes.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2019
Keywords
artificial photosynthesis, BiVO4, borate, photoelectrochemical cells, water oxidation
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-267868 (URN)10.1002/anie.201911303 (DOI)31617301 (PubMedID)2-s2.0-85075156952 (Scopus ID)
Note

QC 20200306

Available from: 2020-03-06 Created: 2020-03-06 Last updated: 2020-03-06Bibliographically approved
Cuartero, M., Chai, L., Zhang, B., De Marco, R. & Crespo, G. A. (2019). Ferrocene self assembled monolayer as a redox mediator for triggering ion transfer across nanometer-sized membranes. Electrochimica Acta, 315, 84-93
Open this publication in new window or tab >>Ferrocene self assembled monolayer as a redox mediator for triggering ion transfer across nanometer-sized membranes
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2019 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 315, p. 84-93Article in journal (Refereed) Published
Abstract [en]

Modulation of ion-transfer processes across nanometer-sized voltammetry membranes by ferrocene-based self-assembled monolayer on regular glassy carbon electrode is herein demonstrated. The composition of the membrane is advantageously tuned to promote either cation or anion transfer: the presence of an exchangeable cation results in cation transfer, whereas a lipophilic salt induces anion transfer through the fulfilment of the electroneutrality of the system. When an anodic scan oxidizes ferrocene moieties in the monolayer, these are stabilized by the pairing of lipophilic anions present in the membrane. As a result, either, hydrophilic cations present in the membrane are expelled into the solution or anions enter from the solution generating hence reversible and voltammetric waves for these transfers. The use of a redox active monolayer rather than a conducting polymer film or a redox active compound into the membrane overcomes a number of drawbacks previously manifested by these systems. The confinement of the redox process in a thin film at the immediate vicinity of the membrane allows to avoid the need of elevated number of redox moieties to be sued in the membrane, therefore suppressing its acute leaching and being compatible with the incorporation of both cation and anion ionophores for the first time. In this sense, assisted transfer of lithium and chloride are shown as proof-of-concept. Here, the peak potential of the associated voltammetric waves shifts according to the Nernst equation, in analogy to potentiometric sensors. Analytical detection of lithium and chloride ions in real samples is additionally presented.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Voltammetry membranes, Self-assembled monolayer, Ion transfer, Ionophores
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-254066 (URN)10.1016/j.electacta.2019.05.091 (DOI)000470108800011 ()2-s2.0-85066091769 (Scopus ID)
Note

QC 20190624

Available from: 2019-06-24 Created: 2019-06-24 Last updated: 2019-06-24Bibliographically approved
Xu, K., Cuartero, M. & Crespo, G. A. (2019). Lowering the limit of detection of ion-selective membranes backside contacted with a film of poly(3-octylthiophene). Sensors and actuators. B, Chemical, 297, Article ID UNSP 126781.
Open this publication in new window or tab >>Lowering the limit of detection of ion-selective membranes backside contacted with a film of poly(3-octylthiophene)
2019 (English)In: Sensors and actuators. B, Chemical, ISSN 0925-4005, E-ISSN 1873-3077, Vol. 297, article id UNSP 126781Article in journal (Refereed) Published
Abstract [en]

Nanometer-sized membranes (thickness of ca 200 nm) backside contacted with a film of poly(3-octylthiophene) (POT) are here interrogated by an electrochemical protocol based on the accumulation and stripping of the target ion aiming at lowering its limit of detection (i.e., in the sub-micromolar range). Thus, using a membrane based on silver ionophore IV (Sigma-Aldrich), which is one of the ionophores regularly used in ion-selective membranes presenting a large binding constant (log beta(Ag-)(ionophore )approximate to 12), it is possible to detect 5 nM concentration of silver with the established methodology. Importantly, this is a 1000-fold lower concentration of silver compared with the case in which the same membrane is subjected to traditional cyclic voltammetry. Essentially, the control of the oxidation state of the POT film by applying a constant potential during a certain period of time (i.e., E-app = 0 V for 720 s) in the presence of silver ions in the sample solution (from 5 to 100 nM) allows for an enrichment of the selective membrane in silver ions. As a result, a subsequent anodic linear sweep potential generates a voltammetric peak for silver transfer across the membrane that comprises a well-defined wave for such very low concentrations of silver in high sodium ion concentration background solution (10 mM NaNO3). Detection of nanomolar levels of silver in different types of natural and environmental waters is herein demonstrated and the results are validated using inductively coupled plasma mass spectrometry.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE SA, 2019
Keywords
Thin voltammetry membranes, Poly(3-octylthiophene), Silver ionophore, Nanomolar silver, Natural and environmental waters
National Category
Chemical Sciences
Research subject
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-256231 (URN)10.1016/j.snb.2019.126781 (DOI)000478562700061 ()2-s2.0-85068988928 (Scopus ID)
Note

QC 20191022

Available from: 2019-10-22 Created: 2019-10-22 Last updated: 2019-11-26Bibliographically approved
Cánovas, R., Cuartero, M. & Crespo, G. A. (2019). Modern creatinine (Bio)sensing: Challenges of point-of-care platforms. Biosensors & bioelectronics, 130, 110-124
Open this publication in new window or tab >>Modern creatinine (Bio)sensing: Challenges of point-of-care platforms
2019 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 130, p. 110-124Article, review/survey (Refereed) Published
Abstract [en]

The importance of knowing creatinine levels in the human body is related to the possible association with renal, muscular and thyroid dysfunction. Thus, the accurate detection of creatinine may indirectly provide information surrounding those functional processes, therefore contributing to the management of the health status of the individual and early diagnosis of acute diseases. The questions at this point are: to what extent is creatinine information clinically relevant?; and do modern creatinine (bio)sensing strategies fulfil the real needs of healthcare applications? The present review addresses these questions by means of a deep analysis of the creatinine sensors reported in the literature over the last five years. There is a wide range of techniques for detecting creatinine, most of them based on optical readouts (20 of the 33 papers collected in this review). However, the use of electrochemical techniques (13 of the 33 papers) is recently emerging in alignment with the search for a definitive and trustworthy creatinine detection at the point-of-care level. In this sense, biosensors (7 of the 33 papers) are being established as the most promising alternative over the years. While creatinine levels in the blood seem to provide better information about patient status, none of the reported sensors display adequate selectivity in such a complex matrix. In contrast, the analysis of other types of biological samples (e.g., saliva and urine) seems to be more viable in terms of simplicity, cross-selectivity and (bio)fouling, besides the fact that its extraction does not disturb individual's well-being. Consequently, simple tests may likely be used for the initial check of the individual in routine analysis, and then, more accurate blood detection of creatinine could be necessary to provide a more genuine diagnosis and/or support the corresponding decision-making by the physician. Herein, we provide a critical discussion of the advantages of current methods of (bio)sensing of creatinine, as well as an overview of the drawbacks that impede their definitive point-of-care establishment.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Blood analysis, Creatinine, Early diagnosis, Enzymatic biosensors, Healthcare, POC devices
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-246460 (URN)10.1016/j.bios.2019.01.048 (DOI)000461526200012 ()30731344 (PubMedID)2-s2.0-85060939971 (Scopus ID)
Note

QC 20190320

Available from: 2019-03-20 Created: 2019-03-20 Last updated: 2019-04-05Bibliographically approved
Wiorek, A., Cuartero, M., De Marco, R. & Crespo, G. A. (2019). Polyaniline Films as Electrochemical-Proton Pump for Acidification of Thin Layer Samples. Analytical Chemistry, 91(23), 14951-14959
Open this publication in new window or tab >>Polyaniline Films as Electrochemical-Proton Pump for Acidification of Thin Layer Samples
2019 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, no 23, p. 14951-14959Article in journal (Refereed) Published
Abstract [en]

Here, we provide the first experimental evidence of proton release from polyaniline (PANT) films subjected to anodic potentials at environmental pHs. We conducted an extensive characterization of unpolarized/polarized PANI film-synthesized by traditional sequential voltammetric scanning by using spectroelectrochemistry, synchrotron radiation-X-ray photoelectron spectroscopy, near edge X-ray absorption fine structure, and potentiometric pH sensing in the vicinity of the PANI layer. This new insight enables the utilization of PANI as a proton pump, which is actively tuned through an electrochemical pulse, so as to controllably acidify well-confined thin layer samples. Furthermore, we demonstrate the analytical significance of this system by measuring the alkalinity of artificial and natural water samples by using two faced planar PANI electrodes, one working as a proton source and the other one as pH electrode. Finally, the impact of this approach is 2-fold: (i) all-solid-state electrode materials may be used with devisible consequences in miniaturized and implementable submersible probes, and (ii) rapid determination of alkalinity as compared to traditional approaches together with a versatility in pH adjustment in any kind of sample, among other applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-266192 (URN)10.1021/acs.analchem.9b03402 (DOI)000500838600027 ()31691565 (PubMedID)2-s2.0-85075424423 (Scopus ID)
Note

QC 20200108

Available from: 2020-01-08 Created: 2020-01-08 Last updated: 2020-01-08Bibliographically approved
Endrodi, B., Stojanovic, A., Cuartero, M., Simic, N., Wildlock, M., de Marco, R., . . . Cornell, A. M. (2019). Selective Hydrogen Evolution on Manganese Oxide Coated Electrodes: New Cathodes for Sodium Chlorate Production. ACS Sustainable Chemistry & Engineering, 7(14), 12170-12178
Open this publication in new window or tab >>Selective Hydrogen Evolution on Manganese Oxide Coated Electrodes: New Cathodes for Sodium Chlorate Production
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2019 (English)In: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 7, no 14, p. 12170-12178Article in journal (Refereed) Published
Abstract [en]

The safety and feasibility of industrial electrochemical production of sodium chlorate, an important chemical in the pulp and paper industry, depend on the selectivity of the electrode processes. The cathodic reduction of anodic products is sufficiently suppressed in the current technology by the addition of chromium(VI) to the electrolyte, but due to the high toxicity of these compounds, alternative pathways are required to maintain high process efficiency. In this paper, we evaluate the electrochemical hydrogen evolution reaction kinetics and selectivity on thermally formed manganese oxide-coated titanium electrodes in hypochlorite and chlorate solutions. The morphology and phase composition of manganese oxide layers were varied via alteration of the annealing temperature during synthesis, as confirmed by scanning electron microscopy, X-ray diffraction, synchrotron radiation X-ray photoelectron spectroscopy, and near-edge X-ray absorption fine structure spectroscopy measurements. As shown in mass spectroscopy coupled electrochemical measurements, the hydrogen evolution selectivity in hypochlorite and chlorate solutions is dictated by the phase composition of the coating. Importantly, a hydrogen evolution efficiency of above 95% was achieved with electrodes of optimized composition (annealing temperature, thickness) in hypochlorite solutions. Further, these electrode coatings are nontoxic and Earth-abundant, offering the possibility of a more sustainable chlorate production.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
Keywords
Cathode selectivity, HER, Industrial electrochemistry, Chemical technology, Dichromate
National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-255559 (URN)10.1021/acssuschemeng.9b01279 (DOI)000475838100027 ()2-s2.0-85073662618 (Scopus ID)
Note

QC 20190805

Available from: 2019-08-05 Created: 2019-08-05 Last updated: 2020-03-09Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-1221-3906

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