Oxidation-state-specific detection of uranium in aqueous solution by photoacoustic spectroscopy

Schrepp, W.; Stumpe, R.; Kim, J. I.; Walther, H.

doi:10.1007/bf00688289

Cited by 38 publications

(16 citation statements)

References 8 publications

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“…This work builds on the LPAS studies carried out by PATEL and ΤΑΜ [2] who first demonstrated high LPAS sensitivity in aqueous solution using microsecond excitation [3]and on actinide LPAS studies carried out by KIM and coworkers [4,5,6,7] who demonstrated high LPAS sensitivity at ambient temperature using nanosecond excitation. A significant advance reported here is achievement of high LPAS sensitivity at 90°C in carrying out speciation studies of Am 3+ in a carbonate solution.…”

Section: Introductionmentioning

confidence: 98%

Detection and Speciation of Transuranium Elements in Synthetic Groundwater via Pulsed-Laser Excitation

et al. 1988

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High-sensitivity methods for detection and speciation of complexed transuranium ions in synthetic basalt groundwater, and simplified analogs, are being developed which exploit advances in pulsed laser technology. The first demonstration of high sensitivity detection of a transuranium ion at temperatures significantly above ambient is reported using laser photoacoustic spectroscopy (LPAS). The existence of enhanced LPAS signal amplitudes with increasing temperature in aqueous solution is confirmed in LPAS spectra recorded at 30°C, 60°C and 90°C using micromolar concentrations of Am 3+ . A detection sensitivity of 8.5 parts per trillion (weight basis) of 144 Cm 3 + in a synthetic basalt groundwater at 22°C has been achieved using laser-induced fluorescence spectroscopy (LIF). This corresponds to 1 X 10* Cm 3 + ions in the laser beam. The detailed spectroscopic information obtained by this method points to the existence of previously unobserved Cm 3 + species. A brief assessment of the applicability and sensitivity of LPAS and LIF methods for speciating transuranium ions in near-neutral pH aqueous solution, such as the groundwater expected in a basalt nuclear waste repository, is presented.

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Section: Introductionmentioning

confidence: 98%

Detection and Speciation of Transuranium Elements in Synthetic Groundwater via Pulsed-Laser Excitation

et al. 1988

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“…On the other hand, the photoacoustic detection can also be used for measuring the nonradiative energies. The photoacoustic method, established hundred years ago by A. G. BELL [3], determines acoustic waves which are generated by the volume expansion of a heated absorber. In laser induced photoacoustic spectroscopy, the absorbed light is detected only; fluorescence and scattering lights will not contribute directly to the main acoustic signals but increase somewhat background signals.…”

Section: Introductionmentioning

confidence: 99%

A Direct Speciation of Transuranium Elements in Natural Aquatic Systems by Laser-Induced Photoacoustic Spectroscopy

Klenze¹,

Kim²

1988

Radiochimica Acta

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A laser induced photoacoustic spectroscopic (LPAS) method has been developed for the direct speciation of actinides in natural aquatic systems. This method provides spectroscopic information comparable to that of conventional absorption spectroscopy, but with much higher sensitivity. Speciation sensitivities for actinides in solution are attained in the sub-μηιοΐ range, e. g. for Am (III) down to 10" 8 mol L" 1 . The paper describes the basic principle and instrumentation as well as some applications to the speciation of transuranic ions, i. e. Pu and Am. Particular emphasis is made on the complexation reaction, the characterization of colloids and the chemical behaviour of actinides in natural groundwaters.

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“…The observed increase in wavelength of the absorption peak with increased carbonate concentration, at a fixed pH, as shown in Table 1, is reflected in the predicted increase in the number of carbonate ions complexed with an americium ion as indicated in Table 2. The formation of mixed hydroxyl/carbonate complexes is confirmed by the increase in peak wavelength [0][1][2][3][4][5] with increased pH at a fixed carbonate concentration again indicated in Table 1. The highest peak wavelength observed was 507.8 nm, shown in Figure 4, for a solution at pH 11.5 and 1 M in CO3 " (Table 1), and is probably associated with the presence of Am (OH) (CO 3)2 ~ ( Table 2).…”

Section: Americium Speciationmentioning

confidence: 59%

“…'Direct' methods are essentially non-invasive causing minimal disturbance of species equilibria, and are consequently more reliable though less sensitive. A survey of speciation methods [1] identified laser induced photoacoustic spectroscopy, LIPAS, as a highly sensitive 'direct' method capable of measuring actinide spectra down to ca 10" 8 M [2][3][4][5][6] and hence providing information on oxidation states and complexation. Consequently, it was selected at the Harwell Laboratory for further development and installation as the principal 'direct' speciation method.…”

Section: Introductionmentioning

confidence: 99%

Some Actinide Spec¡ation Using Laser Induced Photoacoustic Spectroscopy

et al. 1988

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Laser induced photoacoustic spectroscopy is an attractive method for the speciation of actinides in solutions from nuclear waste disposal studies because it is essentially non-invasive and has a reasonably high sensitivity, down to ca 10"' M. A novel true dual beam system has been constructed and commissioned at Harwell with a performance at least equal to any others in existence. It is based on a XeCl excimer laser and a dye laser, beam splitter, two laser power monitors and photoacoustic cells. The wavelength scanning, data collection, and spectra processing and display are controlled by an Apricot computer. The sample and reference cells are housed in an inert atmosphere glove box. Early applications of the equipment described include measurements of Am and Np species under varying conditions of pH, Eh and carbonate concentration. The observations show some correlation with predictions made using the geochemical modelling code PHREEQE.

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Oxidation-state-specific detection of uranium in aqueous solution by photoacoustic spectroscopy

Cited by 38 publications

References 8 publications

Detection and Speciation of Transuranium Elements in Synthetic Groundwater via Pulsed-Laser Excitation

Detection and Speciation of Transuranium Elements in Synthetic Groundwater via Pulsed-Laser Excitation

A Direct Speciation of Transuranium Elements in Natural Aquatic Systems by Laser-Induced Photoacoustic Spectroscopy

Some Actinide Spec¡ation Using Laser Induced Photoacoustic Spectroscopy

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