Journal of the Korean Crystal Growth and Crystal Technology (한국결정성장학회지)

The Korea Association of Crystal Growth (한국결정성장학회)
권호 표지
DOI QR코드

DOI QR Code

Structural properties of Pd-barium zirconate dense membrane synthesized by dual sputtering method

동시 증착 스퍼터링 공정에 의해 증착된 Pd-barium zirconate membrane의 구조분석

  • Byeon, Myeong-Seop (School of Nano & Advanced Materials Engineering, Gyeongsang National University) ;
  • Kang, Eun-Tae (School of Nano & Advanced Materials Engineering, Gyeongsang National University) ;
  • Cho, Woo-Seok (Korea Institute of Ceramic Engineering and Technology) ;
  • Kim, Jin-Ho (Korea Institute of Ceramic Engineering and Technology) ;
  • Hwang, Kwang-Taek (Korea Institute of Ceramic Engineering and Technology)
  • Received : 2011.11.02
  • Accepted : 2011.12.23
  • Published : 2012.02.29
Download PDF
⟨ Previous Next ⟩

Abstract

Barium zirconate exhibits good thermo-chemical stability and proton conduction at high temperatures, but shows poor electron conductivity. Therefore, for high efficiency of hydrogen separation, a very thin and dense Pd-Barium zirconate membrane has to be coated on a porous substrate. A thin and dense Pd-Barium zirconate membrane was successfully synthesized on a porous substrate by means of dual sputtering method. The structural and chemical features of the $BaZr_{0.85}Y_{0.15}O_{3-{\delta}}$ membranes sputtered at $300^{\circ}C$ and $400^{\circ}C$ were investigated by X-ray diffractometry, and it was found that a well-crystallized membrane, Pm-3m space group of $BaZrO_3$, was synthesized. The surface and cross-sectional morphologies of membrane were assessed by SEM (scanning electron microscopy) and TEM(transmission electron microscopy) of the surface and of cross sections. The cross sectional observation of Pd-$BaZr_{0.85}Y_{0.15}O_{3-{\delta}}$ membrane by dual sputtering shows that the coating is quite dense with columnar structure.

Barium zirconate는 화학적 안정성이 우수하고 고온에서의 프로톤 전도성이 뛰어나지만, 프로톤 전도도에 비해 전자전도도가 현저히 떨어진다. 따라서 본 연구에서는 높은 수소 분리 특성을 위해 다공성 지지체 상에 Pd-Barium zirconate를 얇고 치밀한 박막으로 제조하고자 하였고, dual sputtering법을 이용하여 성공적으로 증착하였다. X-선 회절 분석을 통해 증착된 $BaZr_{0.85}Y_{0.15}O_{3-{\delta}}$ 박막은 300 이상에서부터 $BaZrO_3$(Pm-3m) 결정상으로 결정화됨을 확인할 수 있었으며 표면과 단면에 대한 구조적 형상은 SEM과 TEM을 통해 관찰하였다. 관찰 결과 증착된 분리막은 치밀하였고 부채꼴의 주상으로 결정이 성장함을 확인할 수 있었다.

Keywords

References

  1. H. Iwahara, "Technological challenges in the application of proton conducting ceramics", Solid State Ionics 77 (1995) 289. https://doi.org/10.1016/0167-2738(95)00051-7
  2. W.G. Coors, "Protonic ceramic fuel cells for high-efficiency operation with methane", J. Pow. Sour. 118 (2003) 150. https://doi.org/10.1016/S0378-7753(03)00072-7
  3. G. Zhang, S.E. Dorris, U. Balachandran and M. Liu, "Interfacial resistances of Ni-BCY mixed-conducting membranes for hydrogen separation", Solid State Ionics 159 (2003) 121. https://doi.org/10.1016/S0167-2738(02)00871-8
  4. Z. Zhong, "Stability and conductivity study of the $BaCe_{0.9-X}Zr_{X}Y_{0.1}O_{2.95}$ systems", Solid State Ionics 178 (2007) 213. https://doi.org/10.1016/j.ssi.2006.12.007
  5. F. Iguchi, N. Sata, T. Takao and H. Yugami, "Microstructures and grain boundary conductivity of $BaZr_{1-X}Y_{X}O_{3}$ (X = 0.05, 0.10, 0.15) ceramics", Solid State Ionics 178(7-10) (2007) 691. https://doi.org/10.1016/j.ssi.2007.02.019
  6. K. Katahira, Y. Kohchi, T. Shimura and H. Iwahara, "Protonic conduction in Zr-substituted $BaCeO_{3}$", Solid State Ionics 138(1-2) (2000) 91. https://doi.org/10.1016/S0167-2738(00)00777-3
  7. D.H. Kim, Y.C. Jeong, J.S. Park, B.K. Kim and Y.C. Kim "Transfer of Oxygen Vacancy and Proton in Ydoped $BaZrO_{3}$", J. Kor. Ceram. Soc. 46(6) (2009) 695. https://doi.org/10.4191/KCERS.2009.46.6.695
  8. K.D. Kreuer, "Proton-conducting oxides", Annu. Rev. Mater. Res. 33 (2003) 333. https://doi.org/10.1146/annurev.matsci.33.022802.091825
  9. M.A.P. Yazdi, P. Briois, S. Georges and A. Billard, "Electrical and structural investigations of perovskite structure reactively sputter deposited coatings", Solid State Ionics 180 (2009) 1246. https://doi.org/10.1016/j.ssi.2009.07.008
  10. H. Limage, F.D. Tichelaar, R. Closset, S. Delvaux, R. Cloots and S. Lucas, "Study of the effect of a silver nanoparticle seeding layer on the crystallisation temperature, photoinduced hydrophylic and catalytic properties of $TiO_{2}$ thin films deposited on glass by magnetron sputtering", Surf. Coat. Tech. 205(13-14) (2011) 3774. https://doi.org/10.1016/j.surfcoat.2011.01.022
  11. R. Thomas, S. Mochizuki, T. Mihara and T. Ishida, "Effect of substrate temperature on the crystallization of $Pb(Zr,Ti)O_{3}$ films on Pt/Ti/Si substrates prepared by radio frequency magnetron sputtering with a stoichiometric oxide target", Mat. Sci. Eng., B 95(1) (2002) 36. https://doi.org/10.1016/S0921-5107(02)00161-7
  12. I. Levin, T.G. Amos, S.M. Bell, L. Farber, T.A. Vanderah, R.S. Roth and B.H. Toby, "Phase equilibria, crystal structures, and dielectric anomaly in the $BaZrO_{3}-CaZrO_{3}$ system", J. Solid State Chem. 175(2) (2003) 170. https://doi.org/10.1016/S0022-4596(03)00220-2
  13. Y. Kuru, M. Wohlschlogel, U. Welzel and E.J. Mittemeijer, "Coefficients of thermal expansion of thin metal films investigated by non-ambient X-ray diffraction stress analysis", Surf. Coat. Tech. 202 (2008) 2306. https://doi.org/10.1016/j.surfcoat.2007.08.002
  14. W. Chen, X. Hu, R. Wang and Y. Huang, "On the assembling of Pd/ceramic composite membranes for hydrogen separation", Sep. Puri. Tech. 72 (2010) 92. https://doi.org/10.1016/j.seppur.2010.01.010
  15. S.K. Ryi, J.S. Parka, S.H. Kim, D.W. Kim and K.I. Cho, "Formation of a defect-free Pd-Cu-Ni ternary alloy membrane on a polished porous nickel support (PNS)", J. Memb. Sci. 318(1-2) (2008) 346. https://doi.org/10.1016/j.memsci.2008.02.055
  16. J. O'Brien, R. Hughes and J. Hisek, "Pd/Ag membranes on porous alumina substrates by unbalanced magnetron sputtering", Surf. Coat. Tech. 142-144 (2001) 253. https://doi.org/10.1016/S0257-8972(01)01198-7