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  1. B100 理学部/理学研究科
  2. B100b 刊行物
  3. The Journal of earth and planetary sciences
  4. 53

Hydration change reaction of light REE^3+(aq) series-II:Contrasting nephelauxetic effects between hydrated [REE(H_2O)_9]^3+ and [REE(H_2O)_8]^3+ series and the tetrad effects in their hydration enthalpies and REE-OH_2 distances

https://doi.org/10.18999/joueps.53.51
https://doi.org/10.18999/joueps.53.51
5bb8745f-263e-4b70-9f7b-edc768e3a6ef
名前 / ファイル ライセンス アクション
KJ00004741140.pdf KJ00004741140.pdf (1.6 MB)
Item type 紀要論文 / Departmental Bulletin Paper(1)
公開日 2008-02-19
タイトル
タイトル Hydration change reaction of light REE^3+(aq) series-II:Contrasting nephelauxetic effects between hydrated [REE(H_2O)_9]^3+ and [REE(H_2O)_8]^3+ series and the tetrad effects in their hydration enthalpies and REE-OH_2 distances
言語 en
著者 KAWABE, Iwao

× KAWABE, Iwao

WEKO 21843

en KAWABE, Iwao

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TAKAHASHI, Takafumi

× TAKAHASHI, Takafumi

WEKO 21844

en TAKAHASHI, Takafumi

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TANAKA, Kazuya

× TANAKA, Kazuya

WEKO 21845

en TANAKA, Kazuya

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OHTA, Atsuyuki

× OHTA, Atsuyuki

WEKO 21846

en OHTA, Atsuyuki

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アクセス権
アクセス権 open access
アクセス権URI http://purl.org/coar/access_right/c_abf2
抄録
内容記述タイプ Abstract
内容記述 Light REE^3+(aq) is a mixture of two distinguishable species of nonahydrate and octahydrate in equilibrium with respect the hydration change reaction that [REE(H_2O_8]^3+(aq)+H_2O(I)=[REE(H_2O)_9]^3+(aq), and the apparent hydration number of light REE^3+(aq) is changing across the series. Here is discussed nephelauxetic effects of the two REE^3+(aq) series from ΔH^0_γ data for the hydration change reaction and the tetrad effect variations of their hydration enthalpies (ΔH_hyd.) and REE-OH_2 distances. The ΔH^0_γ data combined with those data for solution of REE(ES)_3・9(H_2O) with ES = C_2H_5SO_4^- reported previously, suggest that Racah (E^1 and E^3) parameters for light REE^3+ like Nd^3+ decrease in the following order:[REE(H_2O)_9]^3+(aq)>REE(ES)_3・9(H_2O)> [REE(H_2O)_8]^3+(aq). The average REE^3+-OH_2 distance also decreases in this order. Hence this is a nephelauxetic series that Racah parameters are reduced with decreasing REE^3+-OH_2 distance. The Racah parameters for [REE(H_2O)_9]^3+(aq) series are fairly large and comparable with those of gaseous free REE^3+. No significant tetrad effect is expected in its series variation of (-ΔH_hyd.). By contrast, [REE(H_2O)8]^3+(aq) series has significantly smaller Racah parameters than gaseous free REE^3+, and a convex tetrad effect is expected in the series variation of (-ΔH_hyd.). Since (-ΔH_hyd.). of [REE(H_2O_8)]^3+(aq) in heavy REE series is fitted to a linear function of the reciprocal of observed REE-OH_2 disrance in REECl_3 solution, this relation has been extended to light REE series, and a similar relation for [REE(H_2O)_9]^3+(aq) in light REE series has also been determined from our thermodynamic mixture model and observed REE-OH_2 distances in REECL_3 (REE=La, Pr and Nd) solutions. The reciprocal of REE-OH_2 distance in [REE(H_2O)_8]^3+(aq), when plotted against the atomic number of REE, indicates a small convex tetrad effect whereas such an effect is absent in [REE(H_2O)_9]^3+(aq) , in accordance with their nephelauxetic effects. Interestingly, (-ΔH_hyd.) of [REE(H_2O)_9]^3+(aq) satisfies a linear function of 1/(REE-OH_2), and at the same time, the series variations of both (-ΔH_hyd.) and 1/(REE-OH_2) exhibit small convex tetrad effects when plotted against the atomic number of REE. This is analogous to the relationship between the lattice enthalpy of REEO_1.5(cubic) and REE-O distance. The property of (-ΔH_hyd.) and the lattice enthalpy of REEO_1.5 can be understood from the viewpoints: i) the existence of REE(III) cluster with the equilibrium configuration having the minimum energy by itself, and ii) the classical limit in quantum-chemical energetics where Planck’s constant (h) equals zero. It is emphatically noted that the observed tetrad effects and RSPET can complement the classical ion model with a tactic by which internal structures of the real REE^3+ ions are legitimately introduced into our thermodynamic discussion.
言語 en
内容記述
内容記述タイプ Other
内容記述 国立情報学研究所で電子化したコンテンツを使用している。
言語 ja
出版者
出版者 Dept. of Earth and Planetary Sciences, Nagoya University
言語 en
言語
言語 eng
資源タイプ
資源 http://purl.org/coar/resource_type/c_6501
タイプ departmental bulletin paper
出版タイプ
出版タイプ VoR
出版タイプResource http://purl.org/coar/version/c_970fb48d4fbd8a85
ID登録
ID登録 10.18999/joueps.53.51
ID登録タイプ JaLC
ISSN(print)
収録物識別子タイプ PISSN
収録物識別子 0919-875X
書誌情報 en : The Journal of Earth and Planetary Sciences, Nagoya University

巻 53, p. 51-71, 発行日 2006
フォーマット
値 application/pdf
著者版フラグ
値 publisher
URI
識別子 http://hdl.handle.net/2237/9423
識別子タイプ HDL
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