EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO<SUB>2</SUB>-Water Interaface

LI Xian-Liang; PAN Gang; QIN Yan-Wen; HU Tian-Dou; WU Zi-Yu; XIE Ya-Ning; CHEN Hao; DU Yong-Hua

Chinese Physics C> 2003, Vol. 27> Issue(S1) : 23-27

EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface

state Key Laboratory of Environmental Aquatic Chemistry,Research center for Eco-Environmental Sciences,CAS,Beijing 100085,China2 Qingdao University of Science and Technology,Qingdao 266042,China3 Institute of High Energy Physics,CAS,Beijing 100039,China

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Microscopic structures of Zn(Ⅱ) surface complexes adsorbed at the manganite-water interface and δ-MnO₂ water interface (in a 0.1M NaNO₃ solution at 25°C )were studied using extended X-ray absorption fine structure (EXAFS) spectroscopy.Quantitative analysis of the EXAFS spectra showed that Zn(Ⅱ) was adsorbed onto the solid surface by sharing the oxygen atom in the hydrous Zn²⁺ ions and in the structural unit MnO₆ on the manganite surface at pH7.5. Most of the adsorbed Zn(Ⅱ) was in the form of octahedral Zn(H₂O)₆²⁺,but part of Zn(Ⅱ) was adsorbed as tetrahedral Zn(OH)₂ or Zn(OH)₄^2－.The average Zn-O bond length was 2.00±0.01A.EXAFS analysis of the second sphere indicated that Zn(Ⅱ) adsorbed on the manganite resulted in two Zn-Mn atomic distances of 3.08±0.02A and 3.54±0.02A,corresponding to the edge-linkage(stronger adsorption site) and corner-linkage(weaker adsorption site),respectively.The ZnO polyhedron was linked to the octahedron MnO6 of the manganite in these two modes by sharing two O atoms on the edges of the polyhedral and/or one O atom on the corners of the polyhedral.At pH 5.50,Zn(Ⅱ) was adsorbed onto δ-MnO₂ surface in the form of octahedral hydrous Zn²⁺ ions.The octahedral Zn²⁺ was linked to the structural unit of octahedral MnO6 of the δ-MnO₂ surface by sharing the O atoms.The average bond length of R_Zn-O was 2.07±0.01A and the Zn-Mn atomic distance was 3.53±0.01A,which corresponded to a corner-sharing linkage adsorption mode(weaker adsorption).Macroscopic adsorption-desorption isotherm experiments showed that,in contrast to that of Zn manganite,adsorption of Zn(Ⅱ) on δ-MnO₂ was highly reversible and no apparent adsorption hysteresis was observed.EXAFS results indicated that the adsorption reversibility was corresponded to the corner sharing linkage mode or edge sgaring linkage mode between the adsorbate and adsorbent polyhedra.

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LI Xian-Liang, PAN Gang, QIN Yan-Wen, HU Tian-Dou, WU Zi-Yu, XIE Ya-Ning, CHEN Hao and DU Yong-Hua. EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface[J]. Chinese Physics C, 2003, 27(S1): 23-27.

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Received: 2003-11-21
Revised: 1900-01-01

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface

Corresponding author: LI Xian-Liang,

state Key Laboratory of Environmental Aquatic Chemistry,Research center for Eco-Environmental Sciences,CAS,Beijing 100085,China2 Qingdao University of Science and Technology,Qingdao 266042,China3 Institute of High Energy Physics,CAS,Beijing 100039,China

Received Date: 2003-11-21

Accepted Date: 1900-01-01

Available Online: 2003-01-02

Abstract: Microscopic structures of Zn(Ⅱ) surface complexes adsorbed at the manganite-water interface and δ-MnO₂ water interface (in a 0.1M NaNO₃ solution at 25°C )were studied using extended X-ray absorption fine structure (EXAFS) spectroscopy.Quantitative analysis of the EXAFS spectra showed that Zn(Ⅱ) was adsorbed onto the solid surface by sharing the oxygen atom in the hydrous Zn²⁺ ions and in the structural unit MnO₆ on the manganite surface at pH7.5. Most of the adsorbed Zn(Ⅱ) was in the form of octahedral Zn(H₂O)₆²⁺,but part of Zn(Ⅱ) was adsorbed as tetrahedral Zn(OH)₂ or Zn(OH)₄^2－.The average Zn-O bond length was 2.00±0.01A.EXAFS analysis of the second sphere indicated that Zn(Ⅱ) adsorbed on the manganite resulted in two Zn-Mn atomic distances of 3.08±0.02A and 3.54±0.02A,corresponding to the edge-linkage(stronger adsorption site) and corner-linkage(weaker adsorption site),respectively.The ZnO polyhedron was linked to the octahedron MnO6 of the manganite in these two modes by sharing two O atoms on the edges of the polyhedral and/or one O atom on the corners of the polyhedral.At pH 5.50,Zn(Ⅱ) was adsorbed onto δ-MnO₂ surface in the form of octahedral hydrous Zn²⁺ ions.The octahedral Zn²⁺ was linked to the structural unit of octahedral MnO6 of the δ-MnO₂ surface by sharing the O atoms.The average bond length of R_Zn-O was 2.07±0.01A and the Zn-Mn atomic distance was 3.53±0.01A,which corresponded to a corner-sharing linkage adsorption mode(weaker adsorption).Macroscopic adsorption-desorption isotherm experiments showed that,in contrast to that of Zn manganite,adsorption of Zn(Ⅱ) on δ-MnO₂ was highly reversible and no apparent adsorption hysteresis was observed.EXAFS results indicated that the adsorption reversibility was corresponded to the corner sharing linkage mode or edge sgaring linkage mode between the adsorbate and adsorbent polyhedra.

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EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface

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EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface

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EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface

EXAFS Studies on Adsorption Microscopic Structures of Zn at Manganite-Water Interaface and δ-MnO₂-Water Interaface