Pd–Pb nanoscale films as surface modifiers of Pd,Cu alloy membranes used for hydrogen ultrapurification
Abstract
The purpose of the article is to reveal the role of the thickness of the layer of the lead-palladium alloy deposited on a copper-palladium membrane in the processes of cathodic injection and the anodic extraction of atomic hydrogen.
The objects of the study were ~ 4 μm thick copper-palladium film electrodes obtained by magnetron sputtering of a target with a composition of 56 at. % Cu and 44 at. % Pd. The studies were carried out by cyclic voltammetry and double step anodic-cathodic chronoamperometry in a deaerated 0.1 М H2SO4 aqueous solution. The calculation of the parameters of hydrogen permeability for samples of finite thickness was carried out by mathematical modelling.
Cathodic injection and anodic extraction of atomic hydrogen were used to study the effect of the surface modification of the foil membrane of a Pd-Cu solid solution on the diffusion and kinetic parameters of hydrogen permeability.
It was found that even a small addition of Pd-Pb (a 2 nm thick film) leads to a decrease in the concentration of atomic hydrogen and the diffusion coefficient in the foil. With an increase in the thickness of the coating there is an increase in the diffusion parameters of the hydrogen injection and extraction processes. However, the hydrogen permeability does not reach the level of the unmodified alloy. The main kinetic parameter, the hydrogen extraction rate constant, changes nonlinearly with an increase in the thickness of the coating.
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Al-Mufachi N. A., Steinberger-Wilckens R. Influence of temperature and pressure on surface modified Pd-Cu alloy foils for hydrogen purification applications. Thin Solid Films. 2018;646: 83–91. https://doi.org/10.1016/j.tsf.2017.11.032
Akamatsu T., Kume Y., Komiay K., Yukawa H., Morinaga M., Yamaguchi S. Electrochemical method for measuring hydrogen permeability through metals. Journal of Alloys and Compounds. 2005;393: 302–306. https://doi.org/10.1016/j.jallcom.2004.10.007
Gorbunov S. V., Kannykin S. V., Penkina T. N., Roshan N. R., Chustov E. M., Burkhanov G. S. Palladium-lead alloys for the purification of hydrogencontaining gas mixtures and the separation of hydrogen from them. Russian Metallurgy (Metally). 2017;2017(1): 54–59. https://doi.org/10.1134/S0036029517010050
Endo N., Furukawa Y., Goshome K., Yaegashi S., Mashiko K., Tetsuhiko M. Characterization of mechanical strength and hydrogen permeability of a Pd-Cu alloy film prepared by one-step electroplating for hydrogen separation and membrane reactors. International Journal of Hydrogen Energy. 2019;44(16): 8290–8297. https://doi.org/10.1016/j.ijhydene.2019.01.089
Gorbunov S. V. Dontsov A. I., Sinetskaya D. A Structure and orientation changes in the growth process of solid solution films Pd-5 (at%)Pb. Materials Science. 2019;5: 10–13. https://doi.org/10.31044/1684-579x-2019-0-5-10-13
Ievlev V. M., Solntsev K. A., Dontsov A. I., Maksimenko A. A., Kannykin S. V. Hydrogen permeability of thin condensed Pd–Cu foil: Dependence on temperature and phase composition. Technical Physics. 2016;61(3): 467–469. https://doi.org/10.1134/s1063784216030105
Ievlev V. M., Maksimenko A. A., Kannykin S. V., Belonogov E. K., Volodina M. S., Roshan N. R. Structure and mechanical properties of the condensed foil of Pd-Cu solid solution. Kondensirovannye sredy i mezhfaznye granitsy = Condensed Matter and Interphases. 2016;18(4): 521–529.
Available at: https://elibrary.ru/item.asp?id=27474855 (In Russ., abstract in Eng.)
Wang Y., Nguyen T. S., Liu X. W., Wang X. Novel palladium–lead (Pd–Pb/C) bimetallic catalysts for electrooxidation of ethanol in alkaline media. Journal of Power Sources. 2010;195(9): 2619–2622. https://doi.org/10.1016/j.jpowsour.2009.11.072
Diao Y. Y., Yan R. Y., Zhang S. J., Yang P., Li Z. X., Wang L., Dong H. F. Effects of Pb and Mg doping in Al2O3-upported Pd catalyst on direct oxidative esterification of aldehydes with alcohols to esters. Journal of Molecular Catalysis A: Chemical. 2009;303: 35–42. https://doi.org/10.1016/j.molcata.2008.12.023
Anderson J. A., Richard J. M., Wells P. K. Pd catalysed hexyne hydrogenation modified by Bi and by Pb. Journal of Catalysis. 2009;261(2): 208–216. https://doi.org/10.1016/j.jcat.2008.11.023
Xingwen Y., Peter G.P. Novel Pd–Pb/C bimetallic catalysts for direct formic acid fuel cells. Journal of Power Sources. 2009;192(2): 279–284. https://doi.org/10.1016/j.jpowsour.2009.03.036
Faroppa M. L., Muscia J. J., Chiossoab M. E., Caggianoa C. G., Bideberripebc H. P., Garacia Fierro J. L., Siri G. J., Casella M. L. Oxidation of glycerol with H2O2 on Pb-promoted Pd/G-Al2O3 catalysts. Chinese Journal of Catalysis. 2016;37(11): 1982–1990. https://doi.org/10.1016/S1872-2067(16)62531-7
Khawar A., Aslam Z., Zahir A., Akbar I., Abbas A. Synthesis of Femur extracted hydroxyapatite reinforced nanocomposite and its application for Pb (II) ions abatement from aqueous phase. International Journal Biological Macromolecules. 2019;122: 667–676. https://doi.org/10.1016/j.ijbiomac.2018.10.223
Wei L., Yao X., Tian X., Cao M., Chen W., She Y., Zhang, S. DFT investigation of the effects of doped Pb atoms on Pdn clusters (13 ≤ n ≤ 116). Computational and Theoretical Chemistry. 2011;966(1-3): 375–382. https://doi.org/10.1016/j.comptc.2011.03.041
Morozova N. B., Vvedenskii A. V., Beredina I. P. Katodic injection, anodic extraction and hydrogen diffusion in metallurgic Cu, Pd and Ag, Pd-alloys. I. Theoretical model. Kondensirovannye sredy i mezhfaznye granitsy = Condensed Matter and Interphases. 2014;16(2): 178–188. Available at: https://elibrary.ru/item.asp?id=21785796 (In Russ., abstract in Eng.)
Abiyev R. Sh., et al. Novyy spravochnik khimika i tekhnologa. Elektrodnyye protsessy. Khimicheskaya kinetika i diffuziya. Kolloidnaya khimiya [A new reference book of a chemist and technologist. Electrode processes. hemical kinetics and diffusion. Colloidal chemistry]. St. Petersburg: Mir i Semia Publ.; 2004. 837 p. (In Russ.)
Morozova N. B., Vvedenskii A. V., Maksimenko А. А., Dontsov А. I. Thin layer multicycle cathodic-anodic chronoamperometry of atomic hydrogen injection-extraction into metals with regard to the stage of phase oundary exchange. Russian Journal of Electrochemistry. 2018;54(4): 344–354. https://doi.org/10.1134/s1023193518040067
Barlag H., Opara L., Züchner H. Hydrogen diffusion in palladium based f.c.c. alloys. Journal of Alloys and Compounds. 2002;330-332: 434–437. https://doi.org/10.1016/S0925-8388(01)01459-1
Morozova N. B., Vvedenskii A. V. Cathodic injection, anodic extraction and hydrogen diffusion in metallurgical Cu, Pd- and Ag, Pd-alloys. III. Accounting irreversible hydrogen sorption. Kondensirovannye sredy i mezhfaznye granitsy = Condensed Matter and Interphases. 2016;18(1): 81–90.
Available at: https://elibrary.ru/item.asp?id=25946624(In Russ., abstract in Eng.)
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