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      Modulation of the morphotropic phase boundary for high-performance ductile thermoelectric materials

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          Abstract

          The flexible thermoelectric technique, which can convert heat from the human body to electricity via the Seebeck effect, is expected to provide a peerless solution for the power supply of wearables. The recent discovery of ductile semiconductors has opened a new avenue for flexible thermoelectric technology, but their power factor and figure-of-merit values are still much lower than those of classic thermoelectric materials. Herein, we demonstrate the presence of morphotropic phase boundary in Ag 2Se-Ag 2S pseudobinary compounds. The morphotropic phase boundary can be freely tuned by adjusting the material thermal treatment processes. High-performance ductile thermoelectric materials with excellent power factor (22 μWcm −1 K −2) and figure-of-merit (0.61) values are realized near the morphotropic phase boundary at 300 K. These materials perform better than all existing ductile inorganic semiconductors and organic materials. Furthermore, the in-plane flexible thermoelectric device based on these high-performance thermoelectric materials demonstrates a normalized maximum power density reaching 0.26 Wm −1 under a temperature gradient of 20 K, which is at least two orders of magnitude higher than those of flexible organic thermoelectric devices. This work can greatly accelerate the development of flexible thermoelectric technology.

          Abstract

          Power factor and figure-of-merit values are normally low in flexible thermoelectric materials. Here, the authors fabricate high-performance ductile thermoelectric materials with high power factor and figure-of-merit values near the morphotropic phase boundary in Ag 2Se-Ag 2S pseudobinary compound.

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          Most cited references59

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          From ultrasoft pseudopotentials to the projector augmented-wave method

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              A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu.

              The method of dispersion correction as an add-on to standard Kohn-Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%-40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C(6) coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.
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                Author and article information

                Contributors
                qiupf@mail.sic.ac.cn
                zkp.1989@sjtu.edu.cn
                xshi@mail.sic.ac.cn
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                19 December 2023
                19 December 2023
                2023
                : 14
                : 8442
                Affiliations
                [1 ]GRID grid.9227.e, ISNI 0000000119573309, State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, , Chinese Academy of Sciences, ; Shanghai, China
                [2 ]Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, ( https://ror.org/05qbk4x57) Beijing, China
                [3 ]School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, ( https://ror.org/05qbk4x57) Hangzhou, China
                [4 ]State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, ( https://ror.org/0220qvk04) Shanghai, China
                Author information
                http://orcid.org/0000-0001-6011-1210
                http://orcid.org/0000-0003-1994-117X
                http://orcid.org/0000-0002-9977-3139
                http://orcid.org/0000-0002-9683-037X
                http://orcid.org/0000-0002-8086-6407
                Article
                44318
                10.1038/s41467-023-44318-4
                10730612
                38114552
                8f39c6f1-aa14-4251-b90c-5feceb06e1c0
                © The Author(s) 2023

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 31 May 2023
                : 7 December 2023
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100001809, National Natural Science Foundation of China (National Science Foundation of China);
                Award ID: 52232010
                Award ID: 91963208
                Award Recipient :
                Categories
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                © Springer Nature Limited 2023

                Uncategorized
                thermoelectrics,thermoelectric devices and materials
                Uncategorized
                thermoelectrics, thermoelectric devices and materials

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