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On-Line Monitoring of Radiocarbon Emissions in a Nuclear Facility with Cavity Ring-Down Spectroscopy.

ABSTRACT: There are currently no suitable methods for sensitive automated in situ monitoring of gaseous radiocarbon, one of the main sources of radioactive gas emissions from nuclear power plants. Here, we present a transportable instrument for in situ airborne radiocarbon detection based on mid-infrared cavity ring-down spectroscopy and report its performance in a 1-week field measurement at the Loviisa nuclear power plant. Radiocarbon is detected by measuring an absorption line of the ¹⁴CO₂ molecule. The time resolution of the measurements is 45 min, significantly less than the few days' resolution of the currently used technique, while maintaining a comparable sensitivity. The method can also assess the prevalence of radiocarbon in different molecular species in the airborne emissions. The optical in situ monitoring presented is a completely new method for monitoring emissions from nuclear facilities.

SUBMITTER: Lehmuskoski J

PROVIDER: S-EPMC8655739 | biostudies-literature | 2021 Dec

REPOSITORIES: biostudies-literature

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On-Line Monitoring of Radiocarbon Emissions in a Nuclear Facility with Cavity Ring-Down Spectroscopy.

Lehmuskoski Johannes J Vasama Hannu H Hämäläinen Jussi J Hokkinen Jouni J Kärkelä Teemu T Heiskanen Katja K Reinikainen Matti M Rautio Satu S Hirvelä Miska M Genoud Guillaume G

Analytical chemistry 20211123 48

There are currently no suitable methods for sensitive automated in situ monitoring of gaseous radiocarbon, one of the main sources of radioactive gas emissions from nuclear power plants. Here, we present a transportable instrument for in situ airborne radiocarbon detection based on mid-infrared cavity ring-down spectroscopy and report its performance in a 1-week field measurement at the Loviisa nuclear power plant. Radiocarbon is detected by measuring an absorption line of the <sup>14</sup>CO<su ...[more]

PMID: 34814685

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Project description:New therapeutic biological entities such as bispecific antibodies targeting tissue or specific cell populations form an increasingly important part of the drug development portfolio. However, these biopharmaceutical agents bear the risk of extensive target-mediated drug disposition or atypical pharmacokinetic properties as compared to canonical antibodies. Pharmacokinetics and bio-distribution studies become therefore more and more important during lead optimization. Biologics present, however, greater analytical challenges than small molecule drugs due to the mass and selectivity limitation of mass spectrometry and ligand-binding assay, respectively. Radiocarbon (14C) and its detection methods, such as the emerging 14C cavity ring down spectroscopy (CRDS), thus can play an important role in the large molecule quantitation where a 14C-tag is covalently bound through a stable linker. CRDS has the advantage of a simplified sample preparation and introduction system as compared to accelerator mass spectrometry (AMS) and can be accommodated within an ordinary research laboratory. In this study, we report on the labeling of an anti-IL17 IgG1 model antibody with 14C propionate tag and its detection by CRDS using it as nanotracer (2.1 nCi or 77.7 Bq blended with the therapeutic dose) in a pharmacokinetics study in a preclinical species. We compare these data to data generated by AMS in parallel processed samples. The derived concentration time profiles for anti-IL17 by CRDS were in concordance with the ones derived by AMS and ?-counting of an 125I-labeled anti-IL17 radiotracer and were well described by a 2-compartment population pharmacokinetic model. In addition, antibody tissue distribution coefficients for anti-IL17 were determined by CRDS, which proved to be a direct and sensitive measurement of the extravascular tissue concentration of the antibody when tissue perfusion was applied. Thus, this proof-of-concept study demonstrates that trace 14C-radiolabels and CRDS are an ultrasensitive approach in (pre)clinical pharmacokinetics and bio-distribution studies of new therapeutic entities.

Project description:RationaleThe recent development of cavity ring-down laser spectroscopy (CRDS) instruments capable of measuring (17) O-excess in water has created new opportunities for studying the hydrologic cycle. Here we apply this new method to studying the triple oxygen ((17) O/(16) O, (18) O/(16) O) and hydrogen ((2) H/(1) H) isotope ratios of gypsum hydration water (GHW), which can provide information about the conditions under which the mineral formed and subsequent post-depositional interaction with other fluids.MethodsWe developed a semi-automated procedure for extracting GHW by slowly heating the sample to 400°C in vacuo and cryogenically trapping the evolved water. The isotopic composition (δ(17) O, δ(18) O and δ(2) H values) of the GHW is subsequently measured by CRDS. The extraction apparatus allows the dehydration of five samples and one standard simultaneously, thereby increasing the long-term precision and sample throughput compared with previous methods. The apparatus is also useful for distilling brines prior to isotopic analysis. A direct comparison is made between results of (17) O-excess in GHW obtained by CRDS and fluorination followed by isotope ratio mass spectrometry (IRMS) of O2 .ResultsThe long-term analytical precision of our method of extraction and isotopic analysis of GHW by CRDS is ±0.07‰ for δ(17) O values, ±0.13‰ for δ(18) O values and ±0.49‰ for δ(2) H values (all ±1SD), and ±1.1‰ and ±8 per meg for the deuterium-excess and (17) O-excess, respectively. Accurate measurement of the (17) O-excess values of GHW, of both synthetic and natural samples, requires the use of a micro-combustion module (MCM). This accessory removes contaminants (VOCs, H2 S, etc.) from the water vapour stream that interfere with the wavelengths used for spectroscopic measurement of water isotopologues. CRDS/MCM and IRMS methods yield similar isotopic results for the analysis of both synthetic and natural gypsum samples within analytical error of the two methods.ConclusionsWe demonstrate that precise and simultaneous isotopic measurements of δ(17) O, δ(18) O and δ(2) H values, and the derived deuterium-excess and (17) O-excess, can be obtained from GHW and brines using a new extraction apparatus and subsequent measurement by CRDS. This method provides new opportunities for the application of water isotope tracers in hydrologic and paleoclimatologic research.

Dataset Information

On-Line Monitoring of Radiocarbon Emissions in a Nuclear Facility with Cavity Ring-Down Spectroscopy.

Publications

On-Line Monitoring of Radiocarbon Emissions in a Nuclear Facility with Cavity Ring-Down Spectroscopy.

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