Probing the local structure of FLiBe melts and solidified salts by in situ high-temperature NMR
Physical chemistry chemical physics : PCCP(2023)
摘要
The 2LiF-BeF2 (FLiBe) salt melt is considered the primary choice for a coolant and fuel carrier for the generation IV molten salt reactor (MSR). However, the basics of ionic coordination and short-range ordered structures have been rarely reported due to the toxicity and volatility of beryllium fluorides, as well as the lack of suitable high-temperature in situ probe methods. In this work, the local structure of FLiBe melts was investigated in detail using the newly designed HT-NMR method. It was found that the local structure was comprised of a series of tetrahedral coordinated ionic clusters (e.g., BeF42-, Be2F73-, Be3F104-, and polymeric intermediate-range units). Li+ ions were coordinated by BeF42- ions and the polymeric Be-F network through the analysis of the NMR chemical shifts. Using solid-state NMR, the structure of solid FLiBe solidified mixed salts was confirmed to form a 3D network structure, significantly similar to those of silicates. The above results provide new insights into the local structure of FLiBe salts, which verifies the strong covalent interactions of Be-F coordination and the specific structural transformation to the polymeric ions above 25% BeF2 concentration.
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关键词
flibe melts,solidified salt,in-situ,high-temperature
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