Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 9, Issue 6, Pages 2090-2098Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ee00322b
Keywords
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Funding
- U.S. Department of Energy [DE-EE005432]
- GM
- National Science Foundation [1235535]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
- Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy
- Natural Science Foundation of China [11234012, 51572167]
- Program of Shanghai Subject Chief Scientist [16XD1401100]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- National Basic Research Program of China [2013CB632505]
- National Natural Science Foundation of China [51302205]
- China Postdoctoral Science Foundation [2013M531752]
- DOE's Office of Biological and Environmental Research at PNNL
- Scientific User Facilities Division
- Office of Basic Energy Sciences
- U.S. Department of Energy
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Introducing guests into a host framework to form a so called inclusion compound can be used to design materials with new and fascinating functionalities. The vast majority of inclusion compounds have electropositive guests with neutral or negatively charged frameworks. Here, we show a series of electronegative guest filled skutterudites with inverse polarity. The strong covalent guest-host interactions observed for the electronegative group VIA guests, i.e., S and Se, feature a unique localized cluster vibration'' which significantly influences the lattice dynamics, together with the point-defect scattering caused by element substitutions, resulting in very low lattice thermal conductivity values. The findings of electronegative guests provide a new perspective for guest-filling in skutterudites, and the covalent filler/lattice interactions lead to an unusual lattice dynamics phenomenon which can be used for designing high-efficiency thermoelectric materials and novel functional inclusion compounds with open structures.
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