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Title: The thermal stability and consolidation of perovskite variant Cs2SnCl6 using spark plasma sintering

Abstract

We present that defect perovskites, a category of air and moisture stable perovskite molecular salts, have gained attention for photovoltaics in the search of alternatives to the organic lead-based photovoltaics which show exceptional photovoltaic performance but suffer significant environmental instability and toxicity of Pb. Defect perovskites also have exceptional structural flexibility and diverse crystal chemistry,and thus, display potentials as host phases for incorporating high amounts of halides such as iodine and chorine. In this study, pure Cs2SnCl6, a lead-free defect perovskite variant, was synthesized through a solution-based route that produced particles ranging from 200 to 500 nm. The thermal stability of the assynthesized Cs2SnCl6 powders was investigated using thermogravimetric analysis (TGA), demonstrating stability up to 615°C, above which a phase decomposition occurs leading to the loss of constituent component of SnCl4. Consolidation of Cs2SnCl6 into dense pellets (=94% theoretical density) was achieved via spark plasma sintering (SPS) at a low sintering temperature of 350°C. X-ray diffraction confirms no phase decomposition in the SPS-densified perovskite pellets as a result of rapid consolidation of the SPS sintering at a short duration and lower temperature, and the TGA analysis suggest a comparable thermal stability up to 627°C for the densified pellet, slightly bettermore » than the as-synthesized powders. The thermal diffusivity of Cs2SnCl6 at room temperature was determined as 0.388 mm2∙s-1 by laser flash measurement. Finally, this work further discussed the potential applications of the SPS-densified Cs2SnCl6 beyond perovskite photovoltaics, introducing potential nuclear separations and waste forms for chlorine.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [3];  [1]
  1. Rensselaer Polytechnic Inst., Troy, NY (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1494558
Alternate Identifier(s):
OSTI ID: 1413829
Report Number(s):
PNNL-SA-136300
Journal ID: ISSN 0002-7820
Grant/Contract Number:  
AC05-76RL01830; SC0016584
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 101; Journal Issue: 5; Journal ID: ISSN 0002-7820
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; nuclear waste; perovskites; spark plasma sintering

Citation Formats

Scott, Spencer M., Zhu, Weiguang, Yao, Tiankai, Vienna, John D., Ewing, Rodney C., and Lian, Jie. The thermal stability and consolidation of perovskite variant Cs2SnCl6 using spark plasma sintering. United States: N. p., 2017. Web. doi:10.1111/jace.15372.
Scott, Spencer M., Zhu, Weiguang, Yao, Tiankai, Vienna, John D., Ewing, Rodney C., & Lian, Jie. The thermal stability and consolidation of perovskite variant Cs2SnCl6 using spark plasma sintering. United States. doi:10.1111/jace.15372.
Scott, Spencer M., Zhu, Weiguang, Yao, Tiankai, Vienna, John D., Ewing, Rodney C., and Lian, Jie. Fri . "The thermal stability and consolidation of perovskite variant Cs2SnCl6 using spark plasma sintering". United States. doi:10.1111/jace.15372. https://www.osti.gov/servlets/purl/1494558.
@article{osti_1494558,
title = {The thermal stability and consolidation of perovskite variant Cs2SnCl6 using spark plasma sintering},
author = {Scott, Spencer M. and Zhu, Weiguang and Yao, Tiankai and Vienna, John D. and Ewing, Rodney C. and Lian, Jie},
abstractNote = {We present that defect perovskites, a category of air and moisture stable perovskite molecular salts, have gained attention for photovoltaics in the search of alternatives to the organic lead-based photovoltaics which show exceptional photovoltaic performance but suffer significant environmental instability and toxicity of Pb. Defect perovskites also have exceptional structural flexibility and diverse crystal chemistry,and thus, display potentials as host phases for incorporating high amounts of halides such as iodine and chorine. In this study, pure Cs2SnCl6, a lead-free defect perovskite variant, was synthesized through a solution-based route that produced particles ranging from 200 to 500 nm. The thermal stability of the assynthesized Cs2SnCl6 powders was investigated using thermogravimetric analysis (TGA), demonstrating stability up to 615°C, above which a phase decomposition occurs leading to the loss of constituent component of SnCl4. Consolidation of Cs2SnCl6 into dense pellets (=94% theoretical density) was achieved via spark plasma sintering (SPS) at a low sintering temperature of 350°C. X-ray diffraction confirms no phase decomposition in the SPS-densified perovskite pellets as a result of rapid consolidation of the SPS sintering at a short duration and lower temperature, and the TGA analysis suggest a comparable thermal stability up to 627°C for the densified pellet, slightly better than the as-synthesized powders. The thermal diffusivity of Cs2SnCl6 at room temperature was determined as 0.388 mm2∙s-1 by laser flash measurement. Finally, this work further discussed the potential applications of the SPS-densified Cs2SnCl6 beyond perovskite photovoltaics, introducing potential nuclear separations and waste forms for chlorine.},
doi = {10.1111/jace.15372},
journal = {Journal of the American Ceramic Society},
number = 5,
volume = 101,
place = {United States},
year = {2017},
month = {12}
}

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