Design of experiments in 241Am alpha source preparation by electrodeposition: an approach to process optimization

  • Matías Ezequiel CarranzaEmail author


This work describes a procedure to improve the quality of an 241Am alpha source obtained by means of electrodeposition. The technique of design of experiments (DoE) was applied in order to perform a multivariate analysis of the experimental variable effects taking into consideration the following: i—amperage, d—cathode–anode distance, t—time and PP—polishing process. A 34−2 fractional design was employed using four experimental factors, three levels per factor, and three response variables were studied: Harea = electrodeposited active area, %R = activity recovery percentage, and Δ1/2 = width at half-height. Thanks to this simple design, 9 experiments were enough, done in triplicate, to discern how Δ1/2 and %R are modified when experimental factors change. Additionally, this work provides tools to perform effect statistical analysis of experimental factors, and to pose linear models applying significant terms. The models obtained were validated by analysis of variance and they were of help to verify the choice of significant factors by means of DoE and to approximate to the optimization of the preparation method of a 241Am alpha source by means of contour plots of Δ1/2 and %R.


Design of experiments Optimization Alpha source 241Am Alpha spectrometry Electrodeposition 



This work would not have been done without the support and encouragement of the Nuclear Regulatory Authority (NRA), Argentina. The author would like to thank Mr. Hugo Equillor (NRA) for his productive talks and helpful contributions about detections by alpha spectrometry. Thanks must also be given to Dr. Jorge Magallanes (National Atomic Energy Commission) for his advice and comments on experimental design techniques, as well as for providing the linear model calculation tool in MatLab. The author once again wishes to thank Mr. Fabio Oscar López (NRA) and Ms. Cecilia Esther Lewis (NRA) for endorsing this work and showing special interest in the application of chemometric techniques in the Environmental Management Department of NRA. Finally, thanks are to the translator, María Laura Fauaz, for her work.


  1. 1.
    Aggarwal SK (2016) Alpha-particle spectrometry for the determination of alpha emitting isotopes in nuclear, environmental and biological samples: past, present and future. Anal Methods 8:5353–5371CrossRefGoogle Scholar
  2. 2.
    Mola M, Palomo M, Peñalver A, Borrull F, Aguilar C (2013) Comparative study of different analytical methods for the determination of 238U, 234U, 235U, 230Th and 232Th in NORM samples (Southern Catalonia). J Environ Radioact 115:207–213CrossRefGoogle Scholar
  3. 3.
    Oliveira JM, Carvalho FP (2006) Sequential extraction procedure for determination of uranium, thorium, radium, lead and polonium radionuclides by alpha spectrometry in environmental samples. Czech J Phys 56:D545CrossRefGoogle Scholar
  4. 4.
    Vajda N, Kim C (2010) Determination of Pu isotopes by alpha spectrometry: a review of analytical methodology. J Radioanal Nucl Chem 283:203–223CrossRefGoogle Scholar
  5. 5.
    Manickam E, Straulig S, Tinker RA (2008) Method design and validation for the determination of uranium levels in human urine using high-resolution alpha spectrometry. J Environ Radioact 3:491–501CrossRefGoogle Scholar
  6. 6.
    Pöllänen R, Karhunen T, Siiskonen T, Toivonen H, Pelikan A (2009) Deconvolution of alpha spectra from hot particles. In: Oughton DH, Kashparov V (eds) Radioactive particles in the environment. NATO science for peace and security series C: environmental security. Springer, Dordrecht, pp 209–220Google Scholar
  7. 7.
    Ranebo Y, Pöllänen R, Eriksson M, Siiskonen T, Niagolova N (2010) Characterization of radioactive particles using non-destructive alpha spectrometry. Appl Radiat Isot 68:1754–1759CrossRefGoogle Scholar
  8. 8.
    Semkow TM, Khan AJ, Haines DK, Bari A (2009) Rapid alpha spectroscopy of evaporated liquid residues for emergency response. Health Phys 96:432–441CrossRefGoogle Scholar
  9. 9.
    Croudace IW, Warwick PE, Reading DG, Russell BC (2016) Recent contributions to the rapid screening of radionuclides in emergency responses and nuclear forensics. Trends Anal Chem 85:120–129CrossRefGoogle Scholar
  10. 10.
    Duval CE, Darge AW, Ruff CL, DeVol TA, Husson SM (2018) Rapid sample preparation for alpha spectroscopy with ultrafiltration membranes. Anal Chem 90:4144–4149CrossRefGoogle Scholar
  11. 11.
    Lee MH, Lee CW (2000) Preparation of alpha-emitting nuclides by electrodeposition. Nucl Instr Methods Phys Res A 447:593–600CrossRefGoogle Scholar
  12. 12.
    Crespo MT (2012) A review of electrodeposition methods for the preparation of alpha-radiation sources. Appl Radiat Isot 70:210–215CrossRefGoogle Scholar
  13. 13.
    Dumitru OA, Begy RC, Nita DC, Bobos LD, Cosma C (2013) Uranium electrodeposition for alpha spectrometric source preparation. J Radioanal Nucl Chem 298:1335–1339CrossRefGoogle Scholar
  14. 14.
    Trdin M, Benedik L, Samardžija Z, Pihlar B (2012) Investigation of factors affecting of americium electroplating. Appl Radiat Isot 70:2002–2005CrossRefGoogle Scholar
  15. 15.
    Krmpotić M, Rožmarić Benedik L (2018) Investigation of key factors in preparation of alpha sources by electrodeposition. Appl Radiat Isot 136:37–44CrossRefGoogle Scholar
  16. 16.
    Krmpotić M, Rožmarić Benedik L (2017) Evaluation of several electrolyte mixture-cathode material combinations in electrodeposition of americium radioisotopes for alpha-spectrometric measurements. Appl Radiat Isot 128:158–164CrossRefGoogle Scholar
  17. 17.
    Klemenčič H, Benedik L (2010) Alpha-spectrometric thin source preparation with emphasis on homogeneity. Appl Radiat Isot 68:1247–1251CrossRefGoogle Scholar
  18. 18.
    Janda J, Sládek P, Sas D (2010) Electrodeposition of selected alpha-emitting radionuclides from oxalate-ammonium sulfate electrolyte and measured by means of solid-state alpha spectrometry. J Radioanal Nucl Chem 286:687–691CrossRefGoogle Scholar
  19. 19.
    Leardi R (2009) Experimental design in chemistry: a tutorial. Anal Chim Acta 652:161–172CrossRefGoogle Scholar
  20. 20.
    Costa S, Barroso M, Castañera A, Dias M (2010) Design of experiments, a powerful tool for method development in forensic toxicology: application to the optimization of urinary morphine 3-glucuronide acid hydrolysis. Anal Bioanal Chem 396:2533–2542CrossRefGoogle Scholar
  21. 21.
    Tripathi J, Gupta S, Mishra PK, Variyar PS, Sharma A (2014) Optimization of radiation dose and quality parameters for development of ready-to-cook (RTC) pumpkin cubes using a statistical approach. Innov Food Sci Emerg Technol 26:248–256CrossRefGoogle Scholar
  22. 22.
    Hodek O, Křížek T, Coufal P, Ryšlavá H (2017) Design of experiments for amino acid extraction from tobacco leaves and their subsequent determination by capillary zone electrophoresis. Anal Bioanal Chem 9:2383–2391CrossRefGoogle Scholar
  23. 23.
    Carranza ME (2018) Application of an experimental design to optimize a segregation method of 129I and 14C. J Radioanal Nucl Chem 317:787–799CrossRefGoogle Scholar
  24. 24.
    Vera Candioti L, De Zan MM, Cámara MS, Goicoechea HC (2014) Experimental design and multiple response optimization. Using the desirability function in analytical methods development. Talanta 124:123–138CrossRefGoogle Scholar
  25. 25.
    Goos P, Jones B (2011) Optimal design of experiments. A case study approach. Wiley, New YorkCrossRefGoogle Scholar
  26. 26.
    Furlanetto S, Orlandini S, Mura P, Sergent M, Pinzauti S (2003) How experimental design can improve the validation process. Studies in pharmaceutical analysis. Anal Bioanal Chem 377:937–944CrossRefGoogle Scholar
  27. 27.
    Bärring N-E (1966) Electrodeposition of actinide and lanthanide elements. AB Atomenergi, NyköpingGoogle Scholar
  28. 28.
    Talvitie NA (1972) Electrodeposition of actinides for alpha spectrometric determination. Anal Chem 44:280–283CrossRefGoogle Scholar
  29. 29.
    Weissman S, Anderson NG (2015) Design of experiments (DoE) and process optimization. A review of recent publications. Org Process Res Dev 11:1605–1633CrossRefGoogle Scholar
  30. 30.
    Izadiyan P, Hemmateenejad B (2016) Multi-response optimization of factors affecting ultrasonic assisted extraction from Iranian basil using central composite design. Food Chem 190:864–870CrossRefGoogle Scholar
  31. 31.
    Dejaegher B, Vander Heyden Y (2011) Experimental designs and their recent advances in set-up, data interpretation, and analytical applications. J Pharm Biomed Anal 56(2):141–158CrossRefGoogle Scholar
  32. 32.
    Gorry PA (1990) General least-squares smoothing and differentiation by the convolution (Savitzky–Golay) method. Anal Chem 62:570–573CrossRefGoogle Scholar
  33. 33.
    Hund E, Vander Heyden Y, Haustein M, Massart DL, Smeyers-Verbeke J (2000) Comparison of several criteria to decide on the significance of effects in a robustness test with an asymmetrical factorial design. Anal Chim Acta 404:257–271CrossRefGoogle Scholar
  34. 34.
    Hund E, Vander Heyden Y, Haustein M, Massart DL, Smeyers-Verbeke J (2000) Robustness testing of a reversed-phase high-performance liquid chromatographic assay: comparison of fractional and asymmetrical factorial designs. J Chromatogr A 874:167–185CrossRefGoogle Scholar
  35. 35.
    Khuri AI, Mukhopadhyay S (2010) Response surface methodology. WIREs Comput Stat 2:128–149CrossRefGoogle Scholar
  36. 36.
    Massart DL, Vandeginste BGM, Buydens LMC, De Jong S, Lewi PJ, Smeyers-Verbeke J (1997) Handbook of chemometrics and qualimetrics: part A and B. Elsevier, AmsterdanGoogle Scholar
  37. 37.
    Montgomery DC (2013) Design and analysis of experiments, 8th edn. Wiley, New YorkGoogle Scholar
  38. 38.
    ISO norm 2854-1976 (E) (1976) Statistical interpretation of data. Techniques of estimation and tests relating to means and variancesGoogle Scholar
  39. 39.
    Glover SE, Filby RH, Clark SB, Grytdal SP (1998) Optimization and characterization of a sulfate based electrodeposition method for alpha-spectroscopy of actinide elements using chemometric analysis. J Radioanal Nucl Chem 234:213–220CrossRefGoogle Scholar
  40. 40.
    Tibshirani R (1996) Regression and selection via the lasso. J R Stat Soc B 58:267–288Google Scholar
  41. 41.
    Brath R, Banissi E (2017) Stem and leaf plots extended for text visualizations. In: 14th international conference on computer graphics, imaging and visualization, Marrakesh, MoroccoGoogle Scholar

Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2019

Authors and Affiliations

  1. 1.Ezeiza Atomic CenterRadiological Protection Measurements and Evaluations, Nuclear Regulatory AuthorityEzeiza, Buenos AiresArgentina

Personalised recommendations