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Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics

Marlton, Frederick P. ; Nayak, Sanjib ; Venkateshwarlu, Sarangi ; Chan, Ngai Hang ; Kong, Jing ; Zhang, Yuanpeng ; Tucker, Matthew G. ; Jørgensen, Mads Ry Vogel LU orcid and Pramanick, Abhijit (2021) In Chemistry of Materials 33(22).
Abstract

Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO3-based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric... (More)

Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO3-based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry of Materials
volume
33
issue
22
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85119059541
ISSN
0897-4756
DOI
10.1021/acs.chemmater.1c03066
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2021 American Chemical Society.
id
c5ddab9a-3411-4c02-9f21-ad88bed4a123
date added to LUP
2021-12-09 08:48:13
date last changed
2022-04-27 06:33:13
@article{c5ddab9a-3411-4c02-9f21-ad88bed4a123,
  abstract     = {{<p>Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO3-based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications. </p>}},
  author       = {{Marlton, Frederick P. and Nayak, Sanjib and Venkateshwarlu, Sarangi and Chan, Ngai Hang and Kong, Jing and Zhang, Yuanpeng and Tucker, Matthew G. and Jørgensen, Mads Ry Vogel and Pramanick, Abhijit}},
  issn         = {{0897-4756}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{22}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Chemistry of Materials}},
  title        = {{Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics}},
  url          = {{http://dx.doi.org/10.1021/acs.chemmater.1c03066}},
  doi          = {{10.1021/acs.chemmater.1c03066}},
  volume       = {{33}},
  year         = {{2021}},
}