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1.
Chemosphere ; 338: 139552, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37480948

ABSTRACT

Chlorinated paraffins (CPs) can be classified according to their length as short-chain (SC, C10-C13), medium-chain (MC, C14-C17) and long-chain (LC, C ≥ 18) CPs. Technical CP-mixtures can contain a wide range of carbon- (C-, nC = 10-30) and chlorine- (Cl-, nCl = 3-19) homologues. CPs are high-production volume chemicals (>106 t/y). They are used as flame-retardants, plasticizers and coolant fluids. Due to the persistence, bioaccumulation, long-range environmental transport potential and adverse effects, SCCPs are regulated as persistent organic pollutants (POPs) by the Stockholm Convention. Transformation of CPs can lead to the formation of unsaturated compounds such as chlorinated mono- (CO), di- (CdiO) and tri-olefins (CtriO). Such transformation reactions can occur at different stages of CP manipulation providing characteristic C-/Cl-homologue distributions. All this results in unique patterns that collectively create a fingerprint, which can be distinguished from CP-containing samples. Therefore, CP-fingerprinting can develop into a promising tool for future source apportionment studies and with it, the reduction of environmental burden of CPs and hazards to humans. Herein, CP-containing plastics were studied to establish fingerprints and develop this method. We analyzed four household items by reverse-phase liquid-chromatography coupled with a mass spectrometer with an atmospheric pressure chemical ionization source and an Orbitrap mass analyzer (RP-LC-APCI-Orbitrap-MS) operated at a resolution of 120000 (FWHM at m/z 200). MS-data of different CP-, CO-, CdiO- and CtriO-homologues were efficiently processed with an R-based automatic mass spectra evaluation routine (RASER). From the 16720 ions searched for, up to 4300 ions per sample were assigned to 340 C-/Cl-homologues of CPs and their transformation products. Specific fingerprints were deduced from the C-/Cl-homologues distributions, the carbon- (nC) and chlorine- (nCl) numbers and saturation degree. These fingerprints were compared with the ones obtained by a GC-ECNI-Orbitrap-MS method.


Subject(s)
Hydrocarbons, Chlorinated , Humans , Hydrocarbons, Chlorinated/analysis , Chlorine/analysis , Paraffin/analysis , Plastics , Environmental Monitoring/methods , China
2.
Sci Rep ; 10(1): 8100, 2020 May 12.
Article in English | MEDLINE | ID: mdl-32393805

ABSTRACT

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

3.
Sci Rep ; 9(1): 18805, 2019 Dec 11.
Article in English | MEDLINE | ID: mdl-31827132

ABSTRACT

X-ray phase contrast imaging (XPCI) is more sensitive to density variations than X-ray absorption radiography, which is a crucial advantage when imaging weakly-absorbing, low-Z materials, or steep density gradients in matter under extreme conditions. Here, we describe the application of a polychromatic X-ray laser-plasma source (duration ~0.5 ps, photon energy >1 keV) to the study of a laser-driven shock travelling in plastic material. The XPCI technique allows for a clear identification of the shock front as well as of small-scale features present during the interaction. Quantitative analysis of the compressed object is achieved using a density map reconstructed from the experimental data.

4.
J Synchrotron Radiat ; 24(Pt 1): 196-204, 2017 01 01.
Article in English | MEDLINE | ID: mdl-28009559

ABSTRACT

Direct metrology of coherent short-wavelength beamlines is important for obtaining operational beam characteristics at the experimental site. However, since beam-time limitation imposes fast metrology procedures, a multi-parametric metrology from as low as a single shot is desirable. Here a two-dimensional (2D) procedure based on high-resolution Fresnel diffraction analysis is discussed and applied, which allowed an efficient and detailed beamline characterization at the SACLA XFEL. So far, the potential of Fresnel diffraction for beamline metrology has not been fully exploited because its high-frequency fringes could be only partly resolved with ordinary pixel-limited detectors. Using the high-spatial-frequency imaging capability of an irradiated LiF crystal, 2D information of the coherence degree, beam divergence and beam quality factor M2 were retrieved from simple diffraction patterns. The developed beam metrology was validated with a laboratory reference laser, and then successfully applied at a beamline facility, in agreement with the source specifications.

5.
Chem Commun (Camb) ; 52(68): 10435-8, 2016 Aug 16.
Article in English | MEDLINE | ID: mdl-27488137

ABSTRACT

The extended electrochemical stability window offered by highly concentrated electrolytes allows the operation of aqueous batteries at voltages significantly above the thermodynamic stability limit of water, at which the stability of the current collector potentially limits the cell voltage. Here we report the observation of suppressed anodic dissolution of aluminum in "water-in-salt" electrolytes enabling roll-to-roll electrode fabrication for high-voltage aqueous lithium-ion batteries on cost-effective light-weight aluminum current collectors using established lithium-ion battery technology.

6.
Fresenius J Anal Chem ; 368(2-3): 221-6, 2000.
Article in English | MEDLINE | ID: mdl-11220583

ABSTRACT

A homogenized 193 nm ArF* laser ablation system coupled to an inductively coupled plasma-"Time of Flight"-mass spectrometer (LA-ICP-TOFMS) was tested for depth profiling analysis on different single-layer Ti based coatings on steel and W carbides. Laser parameters, such as repetition rate, pulse energy and spatial resolution were tested to allow optimum depth related calibration curves. The ablation process using a laser repetition rate of 3 Hz, 120 microm crater diameter, and 100 mJ output energy, leads to linear calibration curves independent of the drill time or peak area used for calibrating the thickness of the layer. The best depth resolution obtained (without beam splitter) was 0.20 microm per laser shot. The time resolution of the ICP-TOFMS of 102 ms integration time per isotope was sufficient for the determination of the drill time of the laser through the coatings into the matrix with better than 2.6% RSD (about 7 microm coating thickness, n = 7). Variation of the volume of the ablation cell was not influencing the depth resolution, which suggests that the depth resolution is governed by the ablation process. However, the application on the Ti(N,C) based single layer shows the potential of LA-ICP-TOFMS as a complementary technique for fast depth determinations on various coatings in the low to medium microm region.

7.
Fresenius J Anal Chem ; 368(1): 37-44, 2000 Sep.
Article in English | MEDLINE | ID: mdl-11220828

ABSTRACT

Simultaneous ion sampling and sequential detection offered by inductively coupled plasma 'time of flight' mass spectrometry (ICP-TOFMS) provides advantages for the analysis of short transient concentration-variable signals as produced in laser ablation. In order to investigate the capabilities of ICP-TOFMS in combination with an excimer laser ablation system, ablation studies on reference materials and geological samples were carried out. Various ICP-TOFMS parameters were optimized for laser-induced aerosols. Transverse rejection ion pulse was used to extend the dynamic range in concentration. A reduced volume ablation cell was designed and used in order to increase the sample density in the ICP. Results for 63 simultaneously measured isotopes (SRM 610 from NIST) lead to limits of detection in the 1-100 microg/g range for a 80 microm crater diameter (10 Hz, 1.2 mJ pulse energy). The reproducibility of signal ratios was determined to be better than 2% RSD for transient signals using 102 ms integration time. These optimized parameters were then used for the analysis of tin-rich fluid inclusions. Preliminary results of multielement analysis and isotopic ratio determinations on individual fluid inclusions (63 isotopes, 102 ms integration time) demonstrate the capabilities of ICP-TOFMS in combination with laser ablation.

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