89Y magic-angle spinning NMR of Y2Ti2-xSnxO7 pyrochlores

被引:41
作者
Ashbrook, Sharon E. [1 ]
Whittle, Karl R.
Lumpkin, Gregory R.
Farnan, Ian
机构
[1] Univ St Andrews, Sch Chem, St Andrews KY16 9ST, Fife, Scotland
[2] Univ St Andrews, EaStCHEM, St Andrews KY16 9ST, Fife, Scotland
[3] Univ Cambridge, Dept Earth Sci, Cambridge CB2 3EQ, England
关键词
D O I
10.1021/jp060844q
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The yttrium local environment in the series of pyrochlores Y2Ti2-xSnxO7 was studied using Y-89 NMR. Oxides with the pyrochlore structure exhibit a range of interesting physical and chemical properties, resulting in many technological applications, including the encapsulation of lanthanide- and actinide-bearing radioactive waste. The use of the nonradioactive Y3+ cation provides a sensitive probe for any changes in the local structure and ordering with solid solution composition, through Y-89 ( I = 1/2) NMR. We confirm that a single pyrochlore phase is formed over the entire compositional range, with Y found only on the eight-coordinated A site. A significant ( similar to 15 ppm) chemical shift is observed for each Sn substituted into the Y second neighbor coordination environment. The spectral signal intensities of the possible combinations of Sn/Ti neighbors match those predicted statistically assuming a random distribution of Sn4+/Ti4+ on the six-coordinated pyrochlore B site.
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页码:10358 / 10364
页数:7
相关论文
共 22 条
[1]   Revisiting Y2Si2O7 and Y2SiO5 polymorphic structures by 89Y MAS-NMR spectroscopy [J].
Becerro, AI ;
Escudero, A ;
Florian, P ;
Massiot, D ;
Alba, MD .
JOURNAL OF SOLID STATE CHEMISTRY, 2004, 177 (08) :2783-2789
[2]   NUCLEAR SPIN-LATTICE RELAXATION CAUSED BY PARAMAGNETIC IMPURITIES [J].
BLUMBERG, WE .
PHYSICAL REVIEW, 1960, 119 (01) :79-84
[3]   SYSTEMATICS OF THE PYROCHLORE STRUCTURE TYPE, IDEAL A2B2X6Y [J].
CHAKOUMAKOS, BC .
JOURNAL OF SOLID STATE CHEMISTRY, 1984, 53 (01) :120-129
[4]   STRUCTURAL INFLUENCES ON HIGH-RESOLUTION Y-89 NMR-SPECTRA OF SOLIDS [J].
DUPREE, R ;
SMITH, ME .
CHEMICAL PHYSICS LETTERS, 1988, 148 (01) :41-44
[5]   Nuclear waste disposal-pyrochlore (A2B2O7):: Nuclear waste form for the immobilization of plutonium and "minor" actinides [J].
Ewing, RC ;
Weber, WJ ;
Lian, J .
JOURNAL OF APPLIED PHYSICS, 2004, 95 (11) :5949-5971
[6]   Y-89 MAS NMR-STUDY OF RARE-EARTH PYROCHLORES - PARAMAGNETIC SHIFTS IN THE SOLID-STATE [J].
GREY, CP ;
SMITH, ME ;
CHEETHAM, AK ;
DOBSON, CM ;
DUPREE, R .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1990, 112 (12) :4670-4675
[7]  
GREY CP, 1990, THESIS U OXFORD
[8]  
HAILE SM, 1990, MATER RES SOC SYMP P, V166, P81
[9]   Chemical shift, chemical shift anisotropy, and spin-lattice relaxation time in Y-89-MAS and -static NMR of yttrium compounds [J].
Harazono, T ;
Watanabe, T .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1997, 70 (10) :2383-2388
[10]   FAST-ION CONDUCTING Y-2(ZRYTI1-Y)(2)O-7 PYROCHLORES - NEUTRON RIETVELD ANALYSIS OF DISORDER-INDUCED BY ZR SUBSTITUTION [J].
HEREMANS, C ;
WUENSCH, BJ ;
STALICK, JK ;
PRINCE, E .
JOURNAL OF SOLID STATE CHEMISTRY, 1995, 117 (01) :108-121