High-temperature in situ 11B NMR study of network dynamics in boron-containing glass-forming liquids

被引:32
作者
Wu, Jingshi [1 ]
Potuzak, Marcel [2 ]
Stebbins, Jonathan F. [1 ]
机构
[1] Stanford Univ, Dept Geol & Environm Sci, Stanford, CA 94305 USA
[2] Corning Inc, Div Sci & Technol, Corning, NY 14831 USA
基金
美国国家科学基金会;
关键词
High-T in situ NMR; Chemical exchange; Temperature effect; Boron-coordination; NUCLEAR-MAGNETIC-RESONANCE; SODIUM-BORATE GLASSES; NON-BRIDGING OXYGEN; FICTIVE TEMPERATURE; HIGH-RESOLUTION; SI-29; NMR; STRUCTURAL RELAXATION; BOROALUMINATE LIQUIDS; BOROSILICATE GLASSES; COORDINATION-NUMBER;
D O I
10.1016/j.jnoncrysol.2011.08.013
中图分类号
TQ174 [陶瓷工业]; TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
In situ high-temperature nuclear magnetic resonance (NMR) spectroscopy can be very useful for probing changes in structure and dynamics in glass-forming liquids, and is a unique method for observing chemical exchange among structural species (e.g. BO3-BO4, Q(n)-Q(n+1), and NBO-BO) at the seconds to microseconds time scales. High-temperature B-11 MAS NMR line shape measurements were made at about 100 K above the glass transitions on (Na2O)(0.3)(B2O3)(0.7) and (Na2O)(0.2)(B2O3)(0.21)(Al2O3)(0.08)(SiO2)(0.51) glass-forming liquids. BO3 and BO4 groups are well resolved in B-11 MAS NMR spectra at 14.1 T with sample spinning at 5000 Hz. At higher temperatures, partial peak coalescence occurred due to exchange of BO3 and BO4. Temperature effects on borate speciation were also determined by varying the fictive temperature (Tf) of glasses, where Tf estimated from differential scanning calorimetry measurements. We combined these complementary data sets to model structural exchange in the liquid state. The time scale of BO3-BO4 exchange from NMR data, Trov, appears to be "decoupled" from that of the macroscopic shear relaxation process T-5 derived from the viscosity, however, at higher temperatures, T-s approaches T-(NmR). The "decoupling" at lower temperature may be related to intermediate-range compositional heterogeneities, and/or fast modifier cation diffusivities which trigger "unsuccessful" network exchange events. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:3944 / 3951
页数:8
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