TY - JOUR
T1 - Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance
AU - Alsufyani, Maryam
AU - Stoeckel, Marc-Antoine
AU - Chen, Xingxing
AU - Thorely, Karl
AU - Hallani, Rawad K
AU - Puttisong, Yuttapoom
AU - Ji, Xudong
AU - Meli, Dilara
AU - Paulsen, Bryan D
AU - Strzalka, Joseph
AU - Regeta, Khrystyna
AU - Combe, Craig
AU - Chen, Hu
AU - Tian, Junfu
AU - Rivnay, Jonathan
AU - Fabiano, Simone
AU - McCulloch, Iain
N1 - KAUST Repository Item: Exported on 2021-11-24
Acknowledged KAUST grant number(s): OSR-2018-CRG/CCF-3079, OSR-2018-CRG7-3749, OSR-2019-CRG8-4086
Acknowledgements: We acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards no. OSR-2018-CRG/CCF-3079, OSR-2019-CRG8-4086 and OSR-2018-CRG7-3749. We acknowledge funding from ERC Synergy Grant SC2 (610115), the european union horizon 2020 research and innovation programme under grant agreement n°952911, project BOOSTER and grant agreement n°862474, project RoLA-FLEX, as well as EPSRC Project EP/T026219/1B.D.P. and J.R. gratefully acknowledge support from the National Science Foundation grant no. NSF DMR-1751308. This research used resources of the Advanced Photon Source (beamline 8-ID-E), a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The work at Linköping University was financially supported by the Knut and Alice Wallenberg foundation, the Swedish Research Council (2020 03243), Olle Engkvists Stiftelse (204-0256), the EC for the ITN projects HORATES (GA-955837), and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971).
PY - 2021/11/19
Y1 - 2021/11/19
N2 - 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.
AB - 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.
UR - http://hdl.handle.net/10754/673728
UR - https://onlinelibrary.wiley.com/doi/10.1002/anie.202113078
U2 - 10.1002/anie.202113078
DO - 10.1002/anie.202113078
M3 - Article
C2 - 34797584
SN - 1433-7851
JO - Angewandte Chemie International Edition
JF - Angewandte Chemie International Edition
ER -