Realizing high thermoelectric performance via selective resonant doping in oxyselenide BiCuSeO

Tuning the charge carrier concentration is imperative to optimize the thermoelectric(TE)performance of a material.For BiCuSeO based oxyselenides,doping efforts have been limited to optimizing the carrier concentration.In the present work,dual-doping of In and Pb at Bi site is introduced for p-type BiCuSeO to realize the electric transport channels with intricate band characteristics to improve the power factor(PF).Herein,the impurity resonant state is realized via doping of resonant dopant In over Pb,where Pb comes forward to optimize the Fermi energy in the dual-doped BiCuSeO system to divulge the significance of complex electronic structure.The manifold roles of dual-doping are used to adjust the elevation of the PF due to the significant enhancement in electrical properties.Thus,the combined experimental and theoretical study shows that the In/Pb dual doping at Bi sites gently reduces bandgap,introduces resonant doping states with shifting down the Fermi level into valence band(VB)with a larger density of state,and thus causes to increase the carrier concentration and effective mass(m*),which are favorable to enhance the electronic transport significantly.As a result,both improved ZTmax=0.87(at 873 K)and high ZTave=0.5(at 300–873 K)are realized for InyBi(1−x)−yPbxCuSeO(where x=0.06 and y=0.04)system.The obtained results successfully demonstrate the effectiveness of the selective dual doping with resonant dopant inducing band manipulation and carrier engineering that can unlock new prospects to develop high TE materials.

In-situ growth of high-performance(Ag,Sn)co-doped CoSb_(3)thermoelectric thin films

Owing to the unique features,such as mechanically robust,low-toxic,high stability,and high thermoelectric performance,CoSb_(3)-based skutterudite materials are among art-of-the state thermoelectric candidates.In this work,we develop a facile in-situ method for the growth of well-crystallinity(Ag,Sn)co-doped CoSb_(3)thin films.This preparation method can efficiently control the dopant concentration and distribution in the thin films.Both the density functional theory calculation and the experimental results suggest that Sn and Ag dopants trend to enter the lattice and preferentially fill interstitial sites.Additionally,band structure calculation results suggest that the Fermi level moves into the conduction bands due to co-doping and eventually induces the increased electrical conductivity,which agrees with the optimization of carrier concentration.Moreover,an increase in the density of state after co-doping is responsible for the increased Seebeck coefficient.As a result,the power factors of(Ag,Sn)co-doped CoSb_(3)thin films are greatly enhanced,and the maximum power factor achieves over 0.3 m W m^(-1)K^(-2)at 623 K,which is almost two times than that of the un-doped CoSb_(3)film.Multiple microstructures,including Sb vacancies and Ag/Sn interstitial atoms as point defects,and a high density of lattice distortions coupled with nano-sized Ag-rich grains,lead to all scale phonon scatterings.As a result,a reduced thermal conductivity of~0.28 W m^(-1)K^(-1)and a maximum ZT of~0.52 at 623 K are obtained from(Ag,Sn)co-doped CoSb_(3)thin films.This study indicates our facile in-situ growth can be used to develop high-performance dual doped CoSb_(3)thins.