분광광도법에 의한 Ni(Ⅱ)-8-Hydroxyquinolinate의 용매추출 반응속도론

A Study on the Solvent Extraction Kinetics of Complex Nickel(Ⅱ) 8-Hydroxyquinolinate by Spectrophotometry

  • 이흥락 (경북대학교 자연과학대학 화학과) ;
  • 오인경 (경북대학교 자연과학대학 화학과)
  • Heung Lark Lee (Department of Chemistry, College of Natural Science, Kyungpook National University) ;
  • Oh In-Gyung (Department of Chemistry, College of Natural Science, Kyungpook National University)
  • 발행 : 1992.08.20

초록

Nickel(Ⅱ)-8-hydroxyquinolinate의 용매추출에 대한 반응속도와 메카니즘을 분광광도법으로 연구하였다. 유기상 chloroform에 있는 8-hydroxyquinoline(HOx) 농도와 물층의 pH값을 변화시켜 가면서 흡광도를 측정하였으며, 흡광도 데이터를 해석하여 반응속도가 oxine농도에 대하여는 1차, [$H^+$]에 대하여는 -1차임을 알 수 있었다. 따라서 추출 반응의 속도결정단계는 1 : 1 금속킬레이트인 $NiOx^+$의 생성단계이며, 속도식은 다음과 같다. -d[$Ni^{2+}$]/dt = k[Ni$^{2+}$][Ox$^-$]=k'[Ni$^{2+}$][HOx]$_0$/[H$^+$]. 이 식의 k'값은 log [Ni$^{2+}$]$_0$/[Ni$^{2+}$]$_t$와 시간을 도시한 기울기로부터 구하였으며, 속도상수 k값은 k' = k ${\times}$ K$_{HOx}$ / K$_{D,HOx}$를 써서 계산하였다. 온도에 따른 속도상수의 변화로부터 계산한 활성화에너지 $E_a$ = 6.26 kcal/mol이었고, 활성화 파라미터인 ${\Delta}$G$^{\neq}_{298}$ = 6.59 kcal/mol, ${\Delta}$H$^{\neq}_{298}$ = 5.67 kcal/mol, ${\Delta}$S$^{\neq}_{298}$8 = -3.09 eu/mol이었다.

Kinetics and mechanism on the solvent extraction of nickel(Ⅱ) with 8-hydroxyquinoline (HOx) was studied spectrophotometrically. Absorbance variation was measured by changing the 8-hydroxyquinoline concentration in the chloroform organic phase and the pH values in the aquous phase. By analyzing absorbance data the reaction rate was found to be the first order for 8-hydroxyquinoline concentration and the inverse first one for [H$^+$]. Therefore the rate determining step of the extraction reaction is the formation of the one-to-one metal chelate NiOx$^+$ and the rate equation is as follows; -d[Ni$^{2+}$]/dt = k[Ni$^{2+}$][Ox$^-$] = k'[Ni$^{2+}$][HOx]$_0$/[H$^+$]. The value of k' was evaluated from the slope of plot of log [Ni$^{2+}$]$_0$/[Ni$^{2+}$]$_t$ versus time and the rate constant k was calculated according to the equation k' = k ${\times}$ K$_{HOx}$ / K$_{D,HOx}$. From the temperature dependence of the extraction rate, the activation energy E$_a$ = 6.26 kcal/mol is calculated, and activation parameters, ${\Delta}$G$^{\neq}_{298}$ = 6.59 kcal/mol, ${\Delta}$H$^{\neq}_{298}$ = 5.68 kcal/mol, ${\Delta}$S$^{\neq}_{298}$ = -3.09 eu/mol are estimated.

키워드

참고문헌

  1. Solvent Extraction of Metals A. K. De;S. M. Khopker;R. A. Chalmers
  2. J. Am. Chem. v.63 I. M. Kolthoff;E. B. Sandell
  3. J. Chem. Soc. H. M. Irving;R. J. P. Williams
  4. J. Phys. Chem. v.66 C. B. Honaker;H. Freiser
  5. Anal. Chem. v.36 B. E. McClellan;H. Freiser
  6. Anal. Chem. v.39 J. S. Oh;H. Freiser
  7. Acc. Chem. Res. v.17 H. Freiser
  8. CRC Crit. Rev. Anal. Chem. v.10 P. R. Danesl;R. Chiarizia
  9. Anal. Chem. v.61 W. Yu;H. Freiser
  10. Techiniques of Chemistry v.II Organic Solvents, physical properties and methods of purification(3rd ed.) J. A. Riddick;W. B. Bunger
  11. Anal. Chim. Acta v.28 J. Stary
  12. Anal. Chim. Acta v.8 R. W. Geigen
  13. J. Am. Chem. Soc. v.69 K. G. Stone;l. Friedman
  14. 分析化學 李興洛
  15. J. Am. Chem. Soc. v.75 T. Moeller;F. L. Pundsack
  16. The Solvent Extraction of Metal Chelates J. Stary
  17. Solvent Extraction of Metals A. K. De;S. M. Khopker;R. A. Chalmers
  18. Anal. Chim. Acta v.28 J. Stary;E. Hladky
  19. 日本化學會誌 v.84 和田弘子;中川元吉
  20. Nippon Kagaku Zasshi S. Ito;K. Haraguchi;K. Nakayama;K. Yamada
  21. J. Inorg. Nuci. Chem. v.37 D. S. Flett;M. Cox;J. D. Heels
  22. Anal. Chem. v.47 G. Colovos;A. Yokoyama;H. Freiser
  23. Anal. Chem. v.52 K. Ohashi;H. Freiser
  24. J. Am. Chem. Soc. v.105 H. Watari;H. Freiser
  25. Anal. Chem. v.52 J. F. Coetzee;C. G. Karakatsanis
  26. Anal. Chem. v.52 J. F. Coetzee;C. G. Karakatsanis
  27. Anal. Chem. v.52 K. Ohashi;H. Freiser