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Unlocking the potential of metal halide perovskites for high-performance thermoelectric energy conversion through stable polymorphic phase mixing and electronic heterostructure 认领 引用
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作者 Mohammad-Reza Ahmadian-Yazdi Lifu Yan +2 位作者 Shangchao Lin Ge Fu Mojtaba Abdi-Jalebi 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第6期810-823,I0019,共14页
Metal halide perovskites(MHPs)have been accelerating next generation high performance solar cells due to their high charge carrier transport and optoelectronic properties.However,their thermoelectric properties fall b... Metal halide perovskites(MHPs)have been accelerating next generation high performance solar cells due to their high charge carrier transport and optoelectronic properties.However,their thermoelectric properties fall behind their optoelectronic counterparts,although they have ultralow thermal conductivities and are highly suitable for low grade heat harvesting.A major challenge is how to efficiently dope MHPs in order to achieve high electrical conductivities.As the state-of-the-art MHP for thermoelectric energy conversion,CsSnI3 shows unusual metallic behavior due to the intrinsic Sn vacancies,but it undergoes complex polymorphic phase transitions which hinders its carrier mobility.In this work,we report,for the first time,synthesis of a novel MHP-based thermoelectric device using bulk CsSnI3.This is achieved by leveraging stable polymorphic phase mixing(of orthorhombic and tetragonal phases)and electronic heterostructure.CsSnI3 synthesized by spark-plasma sintering with carbon fiber inclusion shows highly enhanced Seebeck coefficient of~250μV/K,resulting from successful control of the degree of polymorphic phase mixing.The CsSnI3 demonstrates high electrical conductivity of~8400 S/m,attributed to its high carrier mobility.Our approach to control the phase mixing suppresses lattice thermal conductivity to~0.4 W/(m K)through the phonon-boundary scattering.First-principle calculations of the two phases and the phase-interface confirm the strong effect of hybridization and reconstruction of structure at the interface of two phases,which decouples the Seebeck coefficient from electrical conductivity here.The optimized CsSnI3 achieves a power factor of 311μW/(m K2)and ZT of 0.27±0.04,the highest among all reported bulk MHPs.The MHP-based thermoelectric device operates stably across temperature differences of 40 to 260 K,delivering a power density of 3.5 W/m2.This work unlocks the potential of emerging MHPs for thermoelectric devices for low-grade heat harvesting.This could also enable synergistic cooperation between photovoltaic and thermoelectric effects in MHPs for more efficient renewable solar and thermal energy co-harvesting. 展开更多
关键词 Metal halide perovskite Thermoelectric energy conversion Polymorphic phase mixing First-principle density functional theory Electronic heterostructure
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