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Arrhenius, K., Fischer, A., Büker, O., Adrien, H., El Masri, A., Lestremau, F. & Robinson, T. (2020). Analytical methods for the determination of oil carryover from CNG/biomethane refueling stations recovered in a solvent. RSC Advances, 10(20), 11907-11917
Open this publication in new window or tab >>Analytical methods for the determination of oil carryover from CNG/biomethane refueling stations recovered in a solvent
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2020 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 10, no 20, p. 11907-11917Article in journal (Refereed) Published
Abstract [en]

Vehicle gas is often compressed to about 200 bar at the refueling station prior to charging to the vehicle's tank. If a high amount of oil is carried over to the gas, it may cause damage to the vehicles; it is therefore necessary to accurately measure oil carryover. In this paper, three analytical methods for accurate quantification of the oil content are presented whereby two methods are based on gas chromatography and one on FTIR. To better evaluate the level of complexity of the matrix, 10 different compressor oils in use at different refueling stations were initially collected and analysed with GC and FTIR to identify their analytical traces. The GC traces could be divided into three different profiles: oils exhibiting some well resolved peaks, oils exhibiting globally unresolved peaks with some dominant peaks on top of the hump and oils exhibiting globally unresolved peaks. After selection of three oils; one oil from each type, the three methods were evaluated with regards to the detection and quantification limits, the working range, precision, trueness and robustness. The evaluation of the three measurement methods demonstrated that any of these three methods presented were suitable for the quantification of compressor oil for samples. The FTIR method and the GC/MS method both resulted in measurement uncertainties close to 20% rel. while the GC/FID method resulted in a higher measurement uncertainty (U = 30% rel.).

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2020
Keywords
Gas chromatography, Vehicles, Accurate quantifications, Analytical method, Compressor oil, Detection and quantification limit, Measurement methods, Measurement uncertainty, Oil contents, Uncertainty analysis
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-44716 (URN)10.1039/d0ra01399d (DOI)2-s2.0-85082745947 (Scopus ID)
Available from: 2020-04-27 Created: 2020-04-27 Last updated: 2020-04-27Bibliographically approved
Arrhenius, K., Bohlen, H., Büker, O., de Krom, I., Heikens, D. & van Wijk, J. (2020). Hydrogen purity analysis: Suitability of sorbent tubes for trapping hydrocarbons, halogenated hydrocarbons and sulphur compounds. Applied Sciences, 10(1), Article ID 120.
Open this publication in new window or tab >>Hydrogen purity analysis: Suitability of sorbent tubes for trapping hydrocarbons, halogenated hydrocarbons and sulphur compounds
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2020 (English)In: Applied Sciences, E-ISSN 2076-3417, Vol. 10, no 1, article id 120Article in journal (Refereed) Published
Abstract [en]

The ISO 14687-2 standard sets requirements for the purity of the hydrogen that is delivered at refuelling stations. These specifications cover a wide range of impurities and include challenging measurements, mainly due to the very low levels of the required detection limits and the need for "total" measurements (total hydrocarbons, total sulphur compounds, halogenated compounds). Most of the compounds belonging to the species are organic. Thermal desorption often coupled with gas chromatography is a common speciation method used to determine the content of organic impurities. However, no existing sorbent tubes are sufficiently universal to trap all possible impurities; depending on the sorbents and the sampling volume, some compounds may irreversibly adsorb or may break through. It is therefore necessary to evaluate sorbents for the compounds targeted at the level required. In this study, the suitability of sorbent tubes for trapping organic impurities in hydrogen was investigated. Suitable sorbents were selected based on a literature review of suitable sorbent materials. Short-term stability studies for compounds among hydrocarbons, halogenated compounds and sulphurcompounds on the selected sorbents have then been performed for storage periods of two weeks since this is the period typically required to complete the collection, transport and analysis of hydrogen samples. The study clearly shows that the method is promising for total species, even through the results show that not all of the compounds belonging to the three total species to be analysed when performing hydrogen purity analysis can be quantified on one unique sorbent. A multibed sorbent consisting of Tenax TA (weak), Carboxen 1003 (medium), Carbograph 1 (strong) is shown to be a versatile sorbent suitable for the three "total species"; only a few compounds from each family would need to be analysed using other analytical methods. This method proposed here for total species will not only provide a sum of concentrations, but also an identification of which compound(s) is/are actually present in the hydrogen.

Place, publisher, year, edition, pages
MDPI AG, 2020
Keywords
Fuel cells, Hydrogen, Hydrogen quality, Hydrogen vehicle, Sorbent, Thermal desorption
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-43948 (URN)10.3390/app10010120 (DOI)2-s2.0-85079132423 (Scopus ID)
Available from: 2020-02-19 Created: 2020-02-19 Last updated: 2020-02-20Bibliographically approved
Bacquart, T., Arrhenius, K., Persijn, S., Rojo, A., Auprêtre, F., Gozlan, B., . . . Haloua, F. (2019). Hydrogen fuel quality from two main production processes: Steam methane reforming and proton exchange membrane water electrolysis. Journal of Power Sources, 444, Article ID 227170.
Open this publication in new window or tab >>Hydrogen fuel quality from two main production processes: Steam methane reforming and proton exchange membrane water electrolysis
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2019 (English)In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 444, article id 227170Article in journal (Refereed) Published
Abstract [en]

The absence of contaminants in the hydrogen delivered at the hydrogen refuelling station is critical to ensure the length life of FCEV. Hydrogen quality has to be ensured according to the two international standards ISO 14687–2:2012 and ISO/DIS 19880-8. Amount fraction of contaminants from the two hydrogen production processes steam methane reforming and PEM water electrolyser is not clearly documented. Twenty five different hydrogen samples were taken and analysed for all contaminants listed in ISO 14687-2. The first results of hydrogen quality from production processes: PEM water electrolysis with TSA and SMR with PSA are presented. The results on more than 16 different plants or occasions demonstrated that in all cases the 13 compounds listed in ISO 14687 were below the threshold of the international standards. Several contaminated hydrogen samples demonstrated the needs for validated and standardised sampling system and procedure. The results validated the probability of contaminants presence proposed in ISO/DIS 19880-8. It will support the implementation of ISO/DIS 19880-8 and the development of hydrogen quality control monitoring plan. It is recommended to extend the study to other production method (i.e. alkaline electrolysis), the HRS supply chain (i.e. compressor) to support the technology growth.

Place, publisher, year, edition, pages
Elsevier B.V., 2019
Keywords
Fuel cell electrical vehicles, Gas analysis, Hydrogen production, Hydrogen quality, ISO14687, Contamination, Electrolysis, Gas fuel analysis, ISO Standards, Methane, Proton exchange membrane fuel cells (PEMFC), Quality control, Steam reforming, Supply chains, Electrical vehicles, Hydrogen fuel qualities, Hydrogen production process, Hydrogen refuelling stations, International standards, Proton exchange membranes
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-40596 (URN)10.1016/j.jpowsour.2019.227170 (DOI)2-s2.0-85073687836 (Scopus ID)
Available from: 2019-11-12 Created: 2019-11-12 Last updated: 2019-11-12Bibliographically approved
Murugan, A., de Huu, M., Bacquart, T., van Wijk, J., Arrhenius, K., te Ronde, I. & Hemfrey, D. (2019). Measurement challenges for hydrogen vehicles. International journal of hydrogen energy, 44(35), 19326-19333
Open this publication in new window or tab >>Measurement challenges for hydrogen vehicles
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2019 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 44, no 35, p. 19326-19333Article in journal (Refereed) Published
Abstract [en]

Uptake of hydrogen vehicles is an ideal solution for countries that face challenging targets for carbon dioxide reduction. The advantage of hydrogen fuel cell electric vehicles is that they behave in a very similar way to petrol engines yet they do not emit any carbon containing products during operation. The hydrogen industry currently faces the dilemma that they must meet certain measurement requirements (set by European legislation) but cannot do so due to a lack of available methods and standards. This paper outlines the four biggest measurement challenges that are faced by the hydrogen industry including flow metering, quality assurance, quality control and sampling.

Place, publisher, year, edition, pages
Elsevier Ltd, 2019
Keywords
Flow metering, Fuel cell, Hydrogen, ISO 14687, Measurement, Metrology, Quality control, Vehicles, Carbon dioxide, Chemical industry, Flow measurement, Flowmeters, Fuel cells, Pollution control, Quality assurance, Carbon dioxide reduction, Carbon-containing products, European legislation, Hydrogen vehicles, Ideal solutions, Petrol engine
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-38502 (URN)10.1016/j.ijhydene.2019.03.190 (DOI)2-s2.0-85064398363 (Scopus ID)
Available from: 2019-05-03 Created: 2019-05-03 Last updated: 2020-01-10Bibliographically approved
Arrhenius, K., Fischer, A. & Büker, O. (2019). Methods for sampling biogas and biomethane on adsorbent tubes after collection in gas bags. Applied Sciences, 9(6), Article ID 1171.
Open this publication in new window or tab >>Methods for sampling biogas and biomethane on adsorbent tubes after collection in gas bags
2019 (English)In: Applied Sciences, E-ISSN 2076-3417, Vol. 9, no 6, article id 1171Article in journal (Refereed) Published
Abstract [en]

Biogas is a renewable energy source with many different production pathways and numerous excellent opportunities for use; for example, as vehicle fuel after upgrading (biomethane). Reliable analytical methodologies for assessing the quality of the gas are critical for ensuring that the gas can be used technically and safely. An essential part of any procedure aimed at determining the quality is the sampling and transfer to the laboratory. Sampling bags and sorbent tubes are widely used for collecting biogas. In this study, we have combined these two methods, i.e., sampling in a gas bag before subsequent sampling onto tubes in order to demonstrate that this alternative can help eliminate the disadvantages associated with the two methods whilst combining their advantages; with expected longer storage stability as well as easier sampling and transport. The results of the study show that two parameters need to be taken into account when transferring gas from a bag on to an adsorbent; the water content of the gas and the flow rate used during transfer of the gas on to the adsorbent. © 2019 by the authors.

Place, publisher, year, edition, pages
MDPI AG, 2019
Keywords
Bags, Biogas, Biomethane, Flow rate, Sampling
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-38460 (URN)10.3390/app9061171 (DOI)2-s2.0-85063743716 (Scopus ID)
Available from: 2019-05-06 Created: 2019-05-06 Last updated: 2019-05-06Bibliographically approved
Anyangwe Nwaboh, J., Persijn, S., Arrhenius, K., Bohlen, H., Werhahn, O. & Ebert, V. (2018). Metrological quantification of CO in biogas using laser absorption spectroscopy and gas chromatography. Measurement science and technology, 29(9), Article ID 095010.
Open this publication in new window or tab >>Metrological quantification of CO in biogas using laser absorption spectroscopy and gas chromatography
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2018 (English)In: Measurement science and technology, ISSN 0957-0233, E-ISSN 1361-6501, Vol. 29, no 9, article id 095010Article in journal (Refereed) Published
Abstract [en]

Biogas has a vital role in the future market of renewable energy. When upgraded to biomethane, it can be injected into natural gas grids if the level of certain impurities complies with the specifications in EN16723. For some of these impurities, suitable measurement methods are lacking which hampers the quality control of biomethane to be injected into natural gas networks. Here, we report the evaluation of three detection methods suitable for carbon monoxide (CO) in biogas and biomethane applications for which EN16723 specifies an upper limit of 0.1% (1000 µmol/mol). Two of these methods are based on laser absorption spectroscopy (LAS) and one on gas chromatography (GC). Both LAS spectrometers are employing direct absorption spectroscopy and operating at 4.6µm, probing a single CO absorption line in the fundamental CO band: One – called dTDLAS (direct tunable diode laser absorption spectroscopy)- is based on a new Interband Cascade Laser specially designed for biogas and biomethane applications, while the other is based on Quantum Cascade Laser Absorption Spectroscopy (QCLAS). The GC is equipped with two packed columns (Hayesep Q and Molecular Sieve 5A) and a thermal conductivity detector. Carbon monoxide amount fraction results in biogas matrices derived using these three measurement methods are compared to amount fraction values of different, gravimetrically prepared reference gas standards of CO in biogas. These were used to validate the measurement capabilities. The measured CO amount fraction results from LAS and GC covered 10 µmol/mol to 30000 µmol/mol (system measurement ranges, LAS: 3 µmol/mol - 1000 µmol/mol, GC: 500 µmol/mol - 30000 µmol/mol) and were in excellent agreement with the gravimetric values of the gas standards. At 400 µmol/mol, the guide to the expression of uncertainty in measurement (GUM) compliant relative standard uncertainties of our calibration-free dTDLAS and the gas-calibrated QCLAS systems are estimated to be 1.4 % vs 0.5 %, respectively. The relative standard uncertainty of the GC CO measurements at 5075 µmol/mol is 1.3 %. This work demonstrates that, by means of GC and LAS, relative standard uncertainties of 1.4 % and below can be reached for CO measurements in biogas and that cost-optimized calibration-free approaches not requiring frequent use of gas standards have become available.

National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-34113 (URN)10.1088/1361-6501/aad116 (DOI)2-s2.0-85051718594 (Scopus ID)
Available from: 2018-07-11 Created: 2018-07-11 Last updated: 2019-01-10Bibliographically approved
Haloua, F., Bacquart, T., Arrhenius, K., Delobelle, B. & Ent, H. (2018). Metrology for hydrogen energy applications: a project to address normative requirements. Paper presented at 18th International Congress of Metrology (CIM 2017). Measurement science and technology, 29(3), Article ID Special Section on the 18th International Congress of Metrology (CIM 2017).
Open this publication in new window or tab >>Metrology for hydrogen energy applications: a project to address normative requirements
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2018 (English)In: Measurement science and technology, ISSN 0957-0233, E-ISSN 1361-6501, Vol. 29, no 3, article id Special Section on the 18th International Congress of Metrology (CIM 2017)Article in journal (Refereed) Published
Abstract [en]

Hydrogen represents a clean and storable energy solution that could meet worldwide energy demands and reduce greenhouse gases emission. The joint research project (JRP) ‘Metrology for sustainable hydrogen energy applications’ addresses standardisation needs through pre- and co-normative metrology research in the fast emerging sector of hydrogen fuel that meet the requirements of the European Directive 2014/94/EU by supplementing the revision of two ISO standards that are currently too generic to enable a sustainable implementation of hydrogen. The hydrogen purity dispensed at refueling points should comply with the technical specifications of ISO 14687-2 for fuel cell electric vehicles. The rapid progress of fuel cell technology now requires revising this standard towards less constraining limits for the 13 gaseous impurities. In parallel, optimized validated analytical methods are proposed to reduce the number of analyses. The study aims also at developing and validating traceable methods to assess accurately the hydrogen mass absorbed and stored in metal hydride tanks; this is a research axis for the revision of the ISO 16111 standard to develop this safe storage technique for hydrogen. The probability of hydrogen impurity presence affecting fuel cells and analytical techniques for traceable measurements of hydrogen impurities will be assessed and new data of maximum concentrations of impurities based on degradation studies will be proposed. Novel validated methods for measuring the hydrogen mass absorbed in hydrides tanks AB, AB2 and AB5 types referenced to ISO 16111 will be determined, as the methods currently available do not provide accurate results. The outputs here will have a direct impact on the standardisation works for ISO 16111 and ISO 14687-2 revisions in the relevant working groups of ISO/TC 197 ‘Hydrogen technologies’.

Keywords
fuel cell electric vehicles; analytical methods; hydrogen storage; metal hydrides; ISO standards; hydrogen purity
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-33368 (URN)10.1088/1361-6501/aa99ac (DOI)2-s2.0-85042548528 (Scopus ID)
Conference
18th International Congress of Metrology (CIM 2017)
Available from: 2018-03-05 Created: 2018-03-05 Last updated: 2019-01-22Bibliographically approved
Hakonen, A., Karlsson, A., Lindman, L., Büker, O. & Arrhenius, K. (2018). Particles in fuel-grade Liquefied Natural Gas. Journal of Natural Gas Science and Engineering, 55, 350-353
Open this publication in new window or tab >>Particles in fuel-grade Liquefied Natural Gas
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2018 (English)In: Journal of Natural Gas Science and Engineering, ISSN 1875-5100, E-ISSN 2212-3865, Vol. 55, p. 350-353Article in journal (Refereed) Published
Abstract [en]

The utilization of Liquefied Natural Gas (LNG) in the heavy-duty transport sector is a convenient and cost-effective step towards a sustainable future. However, there are questions regarding LNG fuel quality and destructive particles for engines. Basically nothing is known about particles in the commercial LNG being fueled today. The gravimetric and SEM-EDX results here demonstrates that there are precarious metal and silicon dioxide particles in fuel-grade LNG that can clog and erode engine parts. Considering these results further research in the direction of this study, including standardized method development, is highly motivated.

Place, publisher, year, edition, pages
Elsevier B.V., 2018
Keywords
Fuel, Liquefied natural gas, LNG, Microscopy, Particles, SEM-EDX, Cost effectiveness, Elementary particles, Engines, Fueling, Gas fuel purification, Microscopic examination, Natural gas transportation, Silica, Cost effective, Engine parts, Fuel grade, Heavy duty, Liquefied Natural Gas (LNG), Standardized methods, Transport sectors
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-34306 (URN)10.1016/j.jngse.2018.05.005 (DOI)2-s2.0-85048716515 (Scopus ID)
Available from: 2018-08-06 Created: 2018-08-06 Last updated: 2018-08-14Bibliographically approved
Arrhenius, K., Karlsson, A., Hakonen, A., Ohlson, L., Yaghooby, H. & Büker, O. (2018). Variations of fuel composition during storage at Liquefied Natural Gas refuelling stations. Journal of Natural Gas Science and Engineering, 49, 317-323
Open this publication in new window or tab >>Variations of fuel composition during storage at Liquefied Natural Gas refuelling stations
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2018 (English)In: Journal of Natural Gas Science and Engineering, ISSN 1875-5100, E-ISSN 2212-3865, Vol. 49, p. 317-323Article in journal (Refereed) Published
Abstract [en]

Liquefied Natural Gas (LNG) and Liquefied Biogas (LBG) utilization within the heavy duty transport sector is today a sustainable alternative to the use of oil. However, in spite of the high degree of insulation in the storage tank walls, it is impossible to fully avoid any net heat input from the surroundings. Due to some degree of vaporization this results in variation in gas composition during storage at refuelling stations, potentially leading to engine failures. Within this study, a vaporizer/sampler has been built and tested at a station delivering liquefied biomethane (LBG) and occasionally; such in this case, LNG to heavy and medium duty trucks. The vaporizer/sampler has then been used to study the variation of the LNG composition in the storage tank during a two weeks period. The results clearly underline a correlation between the gas phase and the liquid phase as the concentration changes follow the same trend in both phases. Two opposite effects are assumed to influence the concentration of methane, ethane and propane in the liquid and in the gas phase. On one hand, because of the probable presence of not fully mixed layers in the storage tank and due to vehicles being refuelled, both liquid and gas phases are enriched in methane at the expense of ethane and propane. On the other hand, due to boil-off effect towards the end of the storage period, both liquid and gas phases are enriched in ethane and propane at the expense of methane.

Keywords
Ageing, Composition, LBG, LNG, Refuelling station, Chemical analysis, Ethane, Fuel storage, Gas fuel purification, Gases, Liquefied natural gas, Liquids, Methane, Natural gas, Natural gas transportation, Propane, Tanks (containers), Vaporization, Concentration change, Fuel compositions, Gas compositions, Liquefied Natural Gas (LNG), Liquid and gas phasis, Transport sectors, Gas fuel storage
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-33264 (URN)10.1016/j.jngse.2017.11.014 (DOI)2-s2.0-85035751251 (Scopus ID)
Note

 Funding details: EURAMET, European Association of National Metrology Institutes; Funding details: ENG 60 LNG; Funding text: This paper is written under the European Metrology Research Programme (EMRP) project ENG 60 LNG II Metrological support for LNG custody transfer and transport fuel applications , and the authors would like to acknowledge the funding of this Programme by EURAMET (European Association of National Metrology Institutes) and the European Commission . In addition, the authors are grateful to Fordonsgas AB who made their station available for the tests performed in this study.

Available from: 2018-02-12 Created: 2018-02-12 Last updated: 2018-08-14Bibliographically approved
Földváry, V., Bekö, G., Langer, S., Arrhenius, K. & Petráš, D. (2017). Effect of energy renovation on indoor air quality in multifamily residential buildings in Slovakia. Building and Environment, 122, 363-372
Open this publication in new window or tab >>Effect of energy renovation on indoor air quality in multifamily residential buildings in Slovakia
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2017 (English)In: Building and Environment, ISSN 0360-1323, E-ISSN 1873-684X, Vol. 122, p. 363-372Article in journal (Refereed) Published
Abstract [en]

Buildings are responsible for a substantial portion of the global energy consumption. Most of the multifamily residential buildings built in the 20th century in Central and Eastern Europe do not satisfy the current requirements on energy efficiency. Nationwide measures taken to improve the energy efficiency of these buildings rarely consider their impact on the indoor air quality (IAQ). The objective of the present study was to evaluate the impact of simple energy renovation on IAQ, air exchange rates (AER) and occupant satisfaction in Slovak residential buildings. Three pairs of identical naturally ventilated multifamily residential buildings were examined. One building in each pair was newly renovated, the other was in its original condition. Temperature, relative humidity (RH) and the concentration of carbon dioxide (CO2) were measured in 94 apartments (57%) during one week in the winter. A questionnaire related to perceived air quality, sick building syndrome symptoms and airing habits was filled by the occupants. In a companion experiment, the IAQ was investigated in 20 apartments (50%) of a single residential building before and after its renovation. In this experiment, concentrations of nitrogen dioxide (NO2), formaldehyde and total and individual volatile organic compounds (VOC) were also measured. CO2 concentrations were significantly higher and AERs were lower in the renovated buildings. Formaldehyde concentrations increased after renovation and were positively correlated with CO2 and RH. Energy renovation was associated with lower occupant satisfaction with IAQ. Energy retrofitting efforts should be complemented with improved ventilation in order to avoid adverse effects on IAQ.

Keywords
Air exchange rate, Apartment buildings, Natural ventilation, Occupant perception, Retrofitting, Air, Air quality, Apartment houses, Carbon, Carbon dioxide, Energy efficiency, Energy utilization, Finance, Formaldehyde, Housing, Indoor air pollution, Intelligent buildings, Nitrogen compounds, Nitrogen oxides, Ventilation, Volatile organic compounds, Air exchange rates, Central and Eastern Europe, Formaldehyde concentrations, Sick building syndrome symptoms, Volatile organic compound (VOC), Buildings
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-30814 (URN)10.1016/j.buildenv.2017.06.009 (DOI)2-s2.0-85021204935 (Scopus ID)
Available from: 2017-09-06 Created: 2017-09-06 Last updated: 2019-02-05Bibliographically approved
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-4037-3106

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