期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 121, 期 2, 页码 1000-1012出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b09113
关键词
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资金
- Russian Foundation for Basic Research [15-03-01114]
- Ural Branch of the Russian Academy of Sciences [15-9-2-9]
- Collaborative Research Center on Energy Materials, Tohoku University
- JSPS KAKENHI [25220911, 2682031]
- CRDF Global [FSCX-15-61826-0]
- US DOE Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office [DE-AC36-08GO28308]
- US DOE's National Nuclear Security Administration [DE-AC04-94AL85000]
- National Science Foundation [DMR-0944772, DMR-1508249]
- Russian Federal Agency of Scientific Organizations [01201463330]
The disordered phases of the 1-carba-closo-decaborates LiCB9H10 and NaCB(9)Hi(10) exhibit the best solid-state ionic conductivities to date among all known polycrystalline competitors, likely facilitated in part by the highly orientationally mobile CB9H10- anions. We have undertaken both NMR and quasielastic neutron scattering (QENS) measurements to help characterize the monovalent anion reorientational mobilities and mechanisms associated with these two compounds and to compare their anion reorientational behaviors with those for the divalent B10H102- anions in the related Li(2)B(10)Hio and Na2B10H10 compounds. NMR data show that the transition from the low-T ordered to the high-T disordered phase for both LiCB9H10 and NaCB9Hio is accompanied by a nearly two-orders-of-magnitude increase in the reorientational jump rate of CB9H10 anions. QENS measurements of the various disordered compounds indicate anion jump correlation frequencies on the order of 10(10)-10(11) s(-1) and confirm that NaCB9H10 displays jump frequencies about 60% to 120% higher than those for LiCB9H10 and Na2B10H10 at comparable temperatures. The Qdependent quasielastic scattering suggests similar small-angular-jump reorientational mechanisms for the different disordered anions, changing from more uniaxial in character at lower temperatures to more multidimensional at higher temperatures, although still falling short of full three-dimensional rotational diffusion below 500 K within the nanosecond neutron window.
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