Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance
Abstract
We report three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0% benzene (P-0), to 50% (P-50), and 75% (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S/cm and Power factors of 13.2 μWm-1 K-2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.
- Authors:
-
[1];
[2];
[3];
[5];
[5];
[6];
[3];
[1];
[5];
[2];
[7]
- Univ. of Oxford (United Kingdom)
- Linköping Univ., Norrköping (Sweden)
- King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
- Univ. of Kentucky, Lexington, KY (United States)
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Univ. of Oxford (United Kingdom); King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); King Abdullah University of Science and Technology (KAUST); European Union - Horizon 2020 Research and Innovation Programme; National Science Foundation (NSF); Knut and Alice Wallenberg Foundation; European Research Council (ERC); Swedish Research Council (SRC)
- OSTI Identifier:
- 1869177
- Grant/Contract Number:
- AC02-06CH11357; OSR-2018-CRG/CCF-3079; OSR-2019-CRG8-4086; OSR-2018-CRG7-3749; 610115; 952911; 862474; DMR-1751308; SFO-Mat-Liu2002-00971
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie
- Additional Journal Information:
- Journal Volume: 134; Journal Issue: 7; Journal ID: ISSN 0044-8249
- Publisher:
- German Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Alsufyani, Maryam, Stoeckel, Marc‐Antoine, Chen, Xingxing, Thorley, Karl, Hallani, Rawad K., Puttisong, Yuttapoom, Ji, Xudong, Meli, Dilara, Paulsen, Bryan D., Strzalka, Joseph, Regeta, Khrystyna, Combe, Craig, Chen, Hu, Tian, Junfu, Rivnay, Jonathan, Fabiano, Simone, and McCulloch, Iain. Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance. United States: N. p., 2021.
Web. doi:10.1002/ange.202113078.
Alsufyani, Maryam, Stoeckel, Marc‐Antoine, Chen, Xingxing, Thorley, Karl, Hallani, Rawad K., Puttisong, Yuttapoom, Ji, Xudong, Meli, Dilara, Paulsen, Bryan D., Strzalka, Joseph, Regeta, Khrystyna, Combe, Craig, Chen, Hu, Tian, Junfu, Rivnay, Jonathan, Fabiano, Simone, & McCulloch, Iain. Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance. United States. https://doi.org/10.1002/ange.202113078
Alsufyani, Maryam, Stoeckel, Marc‐Antoine, Chen, Xingxing, Thorley, Karl, Hallani, Rawad K., Puttisong, Yuttapoom, Ji, Xudong, Meli, Dilara, Paulsen, Bryan D., Strzalka, Joseph, Regeta, Khrystyna, Combe, Craig, Chen, Hu, Tian, Junfu, Rivnay, Jonathan, Fabiano, Simone, and McCulloch, Iain. Fri .
"Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance". United States. https://doi.org/10.1002/ange.202113078. https://www.osti.gov/servlets/purl/1869177.
@article{osti_1869177,
title = {Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance},
author = {Alsufyani, Maryam and Stoeckel, Marc‐Antoine and Chen, Xingxing and Thorley, Karl and Hallani, Rawad K. and Puttisong, Yuttapoom and Ji, Xudong and Meli, Dilara and Paulsen, Bryan D. and Strzalka, Joseph and Regeta, Khrystyna and Combe, Craig and Chen, Hu and Tian, Junfu and Rivnay, Jonathan and Fabiano, Simone and McCulloch, Iain},
abstractNote = {We report three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0% benzene (P-0), to 50% (P-50), and 75% (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S/cm and Power factors of 13.2 μWm-1 K-2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.},
doi = {10.1002/ange.202113078},
journal = {Angewandte Chemie},
number = 7,
volume = 134,
place = {United States},
year = {Fri Nov 19 00:00:00 EST 2021},
month = {Fri Nov 19 00:00:00 EST 2021}
}
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