Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials
Abstract
Computational prediction of good thermoelectric (TE) performance in several n-type doped Zintl phases, combined with successful experimental realization, has sparked interest in discovering new n-type dopable members of this family of materials. However, most known Zintls are typically only p-type dopable; prior successes in finding n-type Zintl phases have been largely serendipitous. Here in this paper, we go beyond previously synthesized Zintl phases and perform chemical substitutions in known n-type dopable ABX Zintl phases to discover new ones. We use first-principles calculations to predict their stability, potential for TE performance as well as their n-type dopability. Using this approach, we find 17 new ABX Zintl phases in the KSnSb structure type that are predicted to be stable. Several of these newly predicted phases (KSnBi, RbSnBi, NaGeP) are found to exhibit promising n-type TE performance and are n-type dopable. We propose these compounds for further experimental studies, especially KSnBi and RbSnBi, which are both predicted to be good TE materials with high electron concentrations due to self-doping by native defects, when grown under alkali-rich conditions.
- Authors:
-
- Colorado School of Mines, Golden, CO (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1637303
- Alternate Identifier(s):
- OSTI ID: 1617079
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Materials Horizons
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 7; Journal ID: ISSN 2051-6347
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Gorai, Prashun, Ganose, Alex, Faghaninia, Alireza, Jain, Anubhav, and Stevanović, Vladan. Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials. United States: N. p., 2020.
Web. doi:10.1039/d0mh00197j.
Gorai, Prashun, Ganose, Alex, Faghaninia, Alireza, Jain, Anubhav, & Stevanović, Vladan. Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials. United States. https://doi.org/10.1039/d0mh00197j
Gorai, Prashun, Ganose, Alex, Faghaninia, Alireza, Jain, Anubhav, and Stevanović, Vladan. Mon .
"Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials". United States. https://doi.org/10.1039/d0mh00197j. https://www.osti.gov/servlets/purl/1637303.
@article{osti_1637303,
title = {Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials},
author = {Gorai, Prashun and Ganose, Alex and Faghaninia, Alireza and Jain, Anubhav and Stevanović, Vladan},
abstractNote = {Computational prediction of good thermoelectric (TE) performance in several n-type doped Zintl phases, combined with successful experimental realization, has sparked interest in discovering new n-type dopable members of this family of materials. However, most known Zintls are typically only p-type dopable; prior successes in finding n-type Zintl phases have been largely serendipitous. Here in this paper, we go beyond previously synthesized Zintl phases and perform chemical substitutions in known n-type dopable ABX Zintl phases to discover new ones. We use first-principles calculations to predict their stability, potential for TE performance as well as their n-type dopability. Using this approach, we find 17 new ABX Zintl phases in the KSnSb structure type that are predicted to be stable. Several of these newly predicted phases (KSnBi, RbSnBi, NaGeP) are found to exhibit promising n-type TE performance and are n-type dopable. We propose these compounds for further experimental studies, especially KSnBi and RbSnBi, which are both predicted to be good TE materials with high electron concentrations due to self-doping by native defects, when grown under alkali-rich conditions.},
doi = {10.1039/d0mh00197j},
journal = {Materials Horizons},
number = 7,
volume = 7,
place = {United States},
year = {Mon Apr 27 00:00:00 EDT 2020},
month = {Mon Apr 27 00:00:00 EDT 2020}
}
Web of Science
Works referenced in this record:
: Charge Balance in Zintl Compounds as a Route to Intermediate Yb Valence
journal, July 2000
- Fisher, I. R.; Bud'ko, S. L.; Song, C.
- Physical Review Letters, Vol. 85, Issue 5
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Optical properties and Raman-active phonon modes of two-dimensional honeycomb Zintl phases
journal, January 2017
- Arguilla, M. Q.; Cultrara, N. D.; Scudder, M. R.
- Journal of Materials Chemistry C, Vol. 5, Issue 43
Thermoelectric properties of Sr3GaSb3 – a chain-forming Zintl compound
journal, January 2012
- Zevalkink, Alex; Zeier, Wolfgang G.; Pomrehn, Gregory
- Energy & Environmental Science, Vol. 5, Issue 10
Elasticity and constitution of the Earth's interior
journal, June 1952
- Birch, Francis
- Journal of Geophysical Research, Vol. 57, Issue 2
Influence of the optical-acoustic phonon hybridization on phonon scattering and thermal conductivity
journal, May 2016
- Li, Wu; Carrete, Jesús; Madsen, Georg K. H.
- Physical Review B, Vol. 93, Issue 20
Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb 4
journal, May 2017
- Ortiz, Brenden R.; Gorai, Prashun; Stevanović, Vladan
- Chemistry of Materials, Vol. 29, Issue 10
Lattice instabilities in metallic elements
journal, June 2012
- Grimvall, Göran; Magyari-Köpe, Blanka; Ozoliņš, Vidvuds
- Reviews of Modern Physics, Vol. 84, Issue 2
Computational predictions of energy materials using density functional theory
journal, January 2016
- Jain, Anubhav; Shin, Yongwoo; Persson, Kristin A.
- Nature Reviews Materials, Vol. 1, Issue 1
Atomate: A high-level interface to generate, execute, and analyze computational materials science workflows
journal, November 2017
- Mathew, Kiran; Montoya, Joseph H.; Faghaninia, Alireza
- Computational Materials Science, Vol. 139
On the Problem of Polar Intermetallic Compounds: The Stimulation of E. Zintl's Work for the Modern Chemistry of Intermetallics
journal, August 1985
- Schäfer, Herbert
- Annual Review of Materials Science, Vol. 15, Issue 1
FireWorks: a dynamic workflow system designed for high-throughput applications: FireWorks: A Dynamic Workflow System Designed for High-Throughput Applications
journal, May 2015
- Jain, Anubhav; Ong, Shyue Ping; Chen, Wei
- Concurrency and Computation: Practice and Experience, Vol. 27, Issue 17
Traversing the Metal-Insulator Transition in a Zintl Phase: Rational Enhancement of Thermoelectric Efficiency in Yb 14 Mn 1− x Al x Sb 11
journal, September 2008
- Toberer, Eric S.; Cox, Catherine A.; Brown, Shawna R.
- Advanced Functional Materials, Vol. 18, Issue 18
Computational Screening of Homovalent Lead Substitution in Organic–Inorganic Halide Perovskites
journal, December 2015
- Filip, Marina R.; Giustino, Feliciano
- The Journal of Physical Chemistry C, Vol. 120, Issue 1
Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds
journal, March 2015
- Gautier, Romain; Zhang, Xiuwen; Hu, Linhua
- Nature Chemistry, Vol. 7, Issue 4
The high-throughput highway to computational materials design
journal, February 2013
- Curtarolo, Stefano; Hart, Gus L. W.; Nardelli, Marco Buongiorno
- Nature Materials, Vol. 12, Issue 3
Computationally guided discovery of thermoelectric materials
journal, August 2017
- Gorai, Prashun; Stevanović, Vladan; Toberer, Eric S.
- Nature Reviews Materials, Vol. 2, Issue 9
Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs
journal, December 2008
- Lany, Stephan; Zunger, Alex
- Physical Review B, Vol. 78, Issue 23, Article No. 235104
Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures
journal, February 2012
- Zhang, Xiuwen; Yu, Liping; Zakutayev, Andriy
- Advanced Functional Materials, Vol. 22, Issue 7
New developments in the Inorganic Crystal Structure Database (ICSD): accessibility in support of materials research and design
journal, May 2002
- Belsky, Alec; Hellenbrandt, Mariette; Karen, Vicky Lynn
- Acta Crystallographica Section B Structural Science, Vol. 58, Issue 3
Looking for new thermoelectric materials among TMX intermetallics using high-throughput calculations
journal, January 2019
- Barreteau, Celine; Crivello, Jean-Claude; Joubert, Jean-Marc
- Computational Materials Science, Vol. 156
Investigation of n-type doping strategies for Mg 3 Sb 2
journal, January 2018
- Gorai, Prashun; Ortiz, Brenden R.; Toberer, Eric S.
- Journal of Materials Chemistry A, Vol. 6, Issue 28
A simple chemical guide for finding novel n-type dopable Zintl pnictide thermoelectric materials
journal, January 2019
- Gorai, Prashun; Goyal, Anuj; Toberer, Eric S.
- Journal of Materials Chemistry A, Vol. 7, Issue 33
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies
journal, March 2012
- Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen
- Physical Review B, Vol. 85, Issue 11
Recharging lithium battery research with first-principles methods
journal, March 2011
- Ceder, G.; Hautier, G.; Jain, A.
- MRS Bulletin, Vol. 36, Issue 3
Predicting the Thermodynamic Stability of Solids Combining Density Functional Theory and Machine Learning
journal, May 2017
- Schmidt, Jonathan; Shi, Jingming; Borlido, Pedro
- Chemistry of Materials, Vol. 29, Issue 12
From the computer to the laboratory: materials discovery and design using first-principles calculations
journal, May 2012
- Hautier, Geoffroy; Jain, Anubhav; Ong, Shyue Ping
- Journal of Materials Science, Vol. 47, Issue 21
Bonding Patterns in Intermetallic Compounds
journal, July 1991
- Nesper, Reinhard
- Angewandte Chemie International Edition in English, Vol. 30, Issue 7
Potential for high thermoelectric performance in n-type Zintl compounds: a case study of Ba doped KAlSb 4
journal, January 2017
- Ortiz, Brenden R.; Gorai, Prashun; Krishna, Lakshmi
- Journal of Materials Chemistry A, Vol. 5, Issue 8
Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability
journal, April 2012
- Hautier, Geoffroy; Ong, Shyue Ping; Jain, Anubhav
- Physical Review B, Vol. 85, Issue 15
A computational framework for automation of point defect calculations
journal, April 2017
- Goyal, Anuj; Gorai, Prashun; Peng, Haowei
- Computational Materials Science, Vol. 130
Structural, elastic, electronic and optical properties of novel antiferroelectric KNaX (X = S, Se, and Te) compounds: First principles study
journal, September 2018
- Belghit, R.; Belkhir, H.; Kadri, M. T.
- Physica B: Condensed Matter, Vol. 545
Phase Boundary Mapping to Obtain n-type Mg3Sb2-Based Thermoelectrics
journal, January 2018
- Ohno, Saneyuki; Imasato, Kazuki; Anand, Shashwat
- Joule, Vol. 2, Issue 1
Ternary lanthanoid-transition metal pnictides with ThCr2Si2-type structure
journal, April 1978
- Marchand, Roger; Jeitschko, Wolfgang
- Journal of Solid State Chemistry, Vol. 24, Issue 3-4
CsBi4Te6: A High-Performance Thermoelectric Material for Low-Temperature Applications
journal, February 2000
- Chung, D.
- Science, Vol. 287, Issue 5455
Material descriptors for predicting thermoelectric performance
journal, January 2015
- Yan, Jun; Gorai, Prashun; Ortiz, Brenden
- Energy & Environmental Science, Vol. 8, Issue 3
Discovery of earth-abundant nitride semiconductors by computational screening and high-pressure synthesis
journal, June 2016
- Hinuma, Yoyo; Hatakeyama, Taisuke; Kumagai, Yu
- Nature Communications, Vol. 7, Issue 1
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Named Entity Recognition and Normalization Applied to Large-Scale Information Extraction from the Materials Science Literature
journal, July 2019
- Weston, L.; Tshitoyan, V.; Dagdelen, J.
- Journal of Chemical Information and Modeling, Vol. 59, Issue 9
Identification of Potential Photovoltaic Absorbers Based on First-Principles Spectroscopic Screening of Materials
journal, February 2012
- Yu, Liping; Zunger, Alex
- Physical Review Letters, Vol. 108, Issue 6
Ionic vs. van der Waals layered materials: identification and comparison of elastic anisotropy
journal, January 2018
- McKinney, Robert W.; Gorai, Prashun; Manna, Sukriti
- Journal of Materials Chemistry A, Vol. 6, Issue 32
Li−Fe−P−O 2 Phase Diagram from First Principles Calculations
journal, February 2008
- Ong, Shyue Ping; Wang, Lei; Kang, Byoungwoo
- Chemistry of Materials, Vol. 20, Issue 5
Formation enthalpies by mixing GGA and GGA calculations
journal, July 2011
- Jain, Anubhav; Hautier, Geoffroy; Ong, Shyue Ping
- Physical Review B, Vol. 84, Issue 4
Screening billions of candidates for solid lithium-ion conductors: A transfer learning approach for small data
journal, June 2019
- Cubuk, Ekin D.; Sendek, Austin D.; Reed, Evan J.
- The Journal of Chemical Physics, Vol. 150, Issue 21
Yb5In2Sb6: A New Rare Earth Zintl Phase with a Narrow Band Gap
journal, November 2000
- Kim, Sung-Jin; Ireland, John R.; Kannewurf, Carl R.
- Journal of Solid State Chemistry, Vol. 155, Issue 1
Electronic and optical properties of the LiCdX (X=N, P, As and Sb) filled-tetrahedral compounds with the Tran–Blaha modified Becke–Johnson density functional
journal, April 2015
- Bouhemadou, A.; Bin-Omran, S.; Allali, D.
- Materials Research Bulletin, Vol. 64
Large-scale screening of hypothetical metal–organic frameworks
journal, November 2011
- Wilmer, Christopher E.; Leaf, Michael; Lee, Chang Yeon
- Nature Chemistry, Vol. 4, Issue 2, p. 83-89
The Zintl Compound Ca5Al2Sb6 for Low-Cost Thermoelectric Power Generation
journal, September 2010
- Toberer, Eric S.; Zevalkink, Alexandra; Crisosto, Nicole
- Advanced Functional Materials, Vol. 20, Issue 24
Emergence of a few distinct structures from a single formal structure type during high-throughput screening for stable compounds: The case of RbCuS and RbCuSe
journal, October 2015
- Trimarchi, Giancarlo; Zhang, Xiuwen; DeVries Vermeer, Michael J.
- Physical Review B, Vol. 92, Issue 16
Insights into the design of thermoelectric Mg3Sb2 and its analogs by combining theory and experiment
journal, July 2019
- Zhang, Jiawei; Song, Lirong; Iversen, Bo Brummerstedt
- npj Computational Materials, Vol. 5, Issue 1
Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
journal, February 2018
- Mounet, Nicolas; Gibertini, Marco; Schwaller, Philippe
- Nature Nanotechnology, Vol. 13, Issue 3
The Zintl-Klemm Concept - A Historical Survey: The Zintl-Klemm Concept - A Historical Survey
journal, November 2014
- Nesper, Reinhard
- Zeitschrift für anorganische und allgemeine Chemie, Vol. 640, Issue 14
Combinatorial screening for new materials in unconstrained composition space with machine learning
journal, March 2014
- Meredig, B.; Agrawal, A.; Kirklin, S.
- Physical Review B, Vol. 89, Issue 9
Electronic fitness function for screening semiconductors as thermoelectric materials
journal, November 2017
- Xing, Guangzong; Sun, Jifeng; Li, Yuwei
- Physical Review Materials, Vol. 1, Issue 6
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis
journal, February 2013
- Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav
- Computational Materials Science, Vol. 68
First-Principles Study of the Thermoelectric Properties of the Zintl Compound KSnSb
journal, February 2018
- Huang, S.; Liu, H. J.; Fan, D. D.
- The Journal of Physical Chemistry C, Vol. 122, Issue 8