In thermoelectricity,the inherent coupling between electrical conductivity and Seebeck coefficient represents a fundamental challenge in thermoelectric materials development.Herein,we present a unique pressure-tuning ...In thermoelectricity,the inherent coupling between electrical conductivity and Seebeck coefficient represents a fundamental challenge in thermoelectric materials development.Herein,we present a unique pressure-tuning strategy using compressible layered 2H-MoTe2,achieving an effective decoupling between the electrical conductivity and Seebeck coefficient.The applied pressure simultaneously induces two complementary effects:(1)bandgap reduction that moderately enhances carrier concentration to improve the electrical conductivity,and(2)band convergence that dramatically increases density-of-states effective mass to boost the Seebeck coefficient.This dual mechanism yields an extraordinary 18.5-fold enhancement in the average power factor.First-principles calculations and Boltzmann transport modeling precisely reproduce the experimental observations,validating this pressure-induced decoupling mechanism.The pressure-tuning mechanism provides a feasible and effective strategy for breaking through the optimization limits of the power factor,facilitating the design of high-performance thermoelectric materials.展开更多
基金supported by the Science and Technology Development Project of Jilin Province(Grant No.SKL202402004)the Program for the Development of Science and Technology of Jilin Province(Grant No.YDZJ202201ZYTS308)+1 种基金the Open Research Fund of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,Jilin University(Grant Nos.202216 and 2022-23)the National Natural Science Foundation of China(Grant No.12350410372)。
文摘In thermoelectricity,the inherent coupling between electrical conductivity and Seebeck coefficient represents a fundamental challenge in thermoelectric materials development.Herein,we present a unique pressure-tuning strategy using compressible layered 2H-MoTe2,achieving an effective decoupling between the electrical conductivity and Seebeck coefficient.The applied pressure simultaneously induces two complementary effects:(1)bandgap reduction that moderately enhances carrier concentration to improve the electrical conductivity,and(2)band convergence that dramatically increases density-of-states effective mass to boost the Seebeck coefficient.This dual mechanism yields an extraordinary 18.5-fold enhancement in the average power factor.First-principles calculations and Boltzmann transport modeling precisely reproduce the experimental observations,validating this pressure-induced decoupling mechanism.The pressure-tuning mechanism provides a feasible and effective strategy for breaking through the optimization limits of the power factor,facilitating the design of high-performance thermoelectric materials.