TY - JOUR
T1 - Bonding Hierarchy Gives Rise to High Thermoelectric Performance in Layered Zintl Compound BaAu2P4
AU - Pal, Koushik
AU - He, Jiangang
AU - Wolverton, C.
N1 - Funding Information:
K.P. (DFT, thermoelectric calculations, and analysis of the results) and C.W. (overall leadership of project) acknowledge support from the U.S. Department of Energy under Contract No. DE-SC0015106. J.H. (data analysis and interpretation of results) acknowledges support from the U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences, under Award No. DE-SC0014520. The authors acknowledge computing resources provided by (a) the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231 and (b) the Quest high performance computing facility at Northwestern University which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology.
Funding Information:
K.P. (DFT,thermoelectric calculations, and analysis of the results) and C.W. (overall leadership of project) acknowledge support from the U.S. Department of Energy under Contract No. DE-SC0015106. J.H. (data analysis and interpretation of results) acknowledges support from the U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences, under Award No. DE-SC0014520. The authors acknowledge computing resources provided by (a) the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231 and (b) the Quest high performance computing facility at Northwestern University which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/11/13
Y1 - 2018/11/13
N2 - The search for new thermoelectric materials has gained rapid progress in recent years as thermoelectric technology offers the potential for environmentally friendly and sustainable energy conversion methods from waste heat to electricity. In this work, we use first-principles calculations based on density functional theory to predict high thermoelectric performance in BaAu2P4, a layered Zintl compound with a small band gap. BaAu2P4 exhibits crystallographic heterogeneity in which rigid [Au2P4]2- units are separated by layers of Ba2+ cations, which are bonded relatively weakly to the lattice through electrostatic interactions. The phosphorus atoms are covalently bonded to each other and form infinite chains within the crystal. While the phosphorus chains facilitate large electrical conductivity, the presence of multiple bands near the Fermi level gives rise to an enhanced Seebeck coefficient. On the other hand, the loosely bound Ba along with Au strongly scatter the heat carrying acoustic phonons, significantly reducing the lattice thermal conduction along the stacking direction. As a consequence of this bonding hierarchy (i.e., coexisting rigid and fluctuating sublattices), BaAu2P4 exhibits a large power factor and low lattice thermal conductivity, which results in a high thermoelectric figure of merit (zT). Thus, our findings should encourage the exploration of new thermoelectric materials in the family of layered compounds with small band gaps and crystallographic heterogeneity.
AB - The search for new thermoelectric materials has gained rapid progress in recent years as thermoelectric technology offers the potential for environmentally friendly and sustainable energy conversion methods from waste heat to electricity. In this work, we use first-principles calculations based on density functional theory to predict high thermoelectric performance in BaAu2P4, a layered Zintl compound with a small band gap. BaAu2P4 exhibits crystallographic heterogeneity in which rigid [Au2P4]2- units are separated by layers of Ba2+ cations, which are bonded relatively weakly to the lattice through electrostatic interactions. The phosphorus atoms are covalently bonded to each other and form infinite chains within the crystal. While the phosphorus chains facilitate large electrical conductivity, the presence of multiple bands near the Fermi level gives rise to an enhanced Seebeck coefficient. On the other hand, the loosely bound Ba along with Au strongly scatter the heat carrying acoustic phonons, significantly reducing the lattice thermal conduction along the stacking direction. As a consequence of this bonding hierarchy (i.e., coexisting rigid and fluctuating sublattices), BaAu2P4 exhibits a large power factor and low lattice thermal conductivity, which results in a high thermoelectric figure of merit (zT). Thus, our findings should encourage the exploration of new thermoelectric materials in the family of layered compounds with small band gaps and crystallographic heterogeneity.
UR - http://www.scopus.com/inward/record.url?scp=85055690991&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85055690991&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.8b03130
DO - 10.1021/acs.chemmater.8b03130
M3 - Article
AN - SCOPUS:85055690991
SN - 0897-4756
VL - 30
SP - 7760
EP - 7768
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 21
ER -