The argyrodite compounds(2 A(12)/B X6 m n n^(m+)+--(Am+=Li^(+),Cu^(+),and Ag^(+);Bn^(+)=Ga^(3+),Si^(4+),Ge^(4+),Sn^(4+),P^(5+),and As^(5+);and X^(2−)=S^(2−),Se^(2−),or Te^(2−)))have attracted great attention as excell...The argyrodite compounds(2 A(12)/B X6 m n n^(m+)+--(Am+=Li^(+),Cu^(+),and Ag^(+);Bn^(+)=Ga^(3+),Si^(4+),Ge^(4+),Sn^(4+),P^(5+),and As^(5+);and X^(2−)=S^(2−),Se^(2−),or Te^(2−)))have attracted great attention as excellent thermoelectric(TE)materials due to their extremely low lattice thermal conductivity(κl).Among them,Ag_(8)SnSe_(6)-based TE materials have high potential for TE applications.However,the pristine Ag_(8)SnSe_(6)materials have low carrier concentration(<1017 cm^(−3)),resulting in low power factors.In this study,a hydrothermal method was used to synthesize Ag_(8)SnSe_(6)with high purity,and the introduction of SnBr_(2)into the pristine Ag_(8)SnSe_(6)powders has been used to simultaneously increase the power factor and decrease the thermal conductivity(κ).On the one hand,a portion of the Br−ions acted as electrons to increase the carrier concentration,increasing the power factor to a value of~698 mW·m^(−1)·K^(−2)at 736 K.On the other hand,some of the dislocations and nanoprecipitates(SnBr_(2))were generated,resulting in a decrease ofκl(~0.13 W·m^(−1)·K^(−1))at 578 K.As a result,the zT value reaches~1.42 at 735 K for the sample Ag8Sn1.03Se5.94Br0.06,nearly 30%enhancement in contrast with that of the pristine sample(~1.09).The strategy of synergistic manipulation of carrier concentration and microstructure by introducing halogen compounds could be applied to the argyrodite compounds to improve the TE properties.展开更多
基金This work was supported by the Guangxi Natural Science Foundation of China(Grant Nos.2020GXNSFAA159111,AD20159006,2020GXNSFAA159107,AD19245160,AD21220056,and AD19110020)the National Key R&D Program of China(Grant No.2017YFE0198000)the National Natural Science Foundation of China(Grant Nos.52061009,U21A2054,and 51961011).
文摘The argyrodite compounds(2 A(12)/B X6 m n n^(m+)+--(Am+=Li^(+),Cu^(+),and Ag^(+);Bn^(+)=Ga^(3+),Si^(4+),Ge^(4+),Sn^(4+),P^(5+),and As^(5+);and X^(2−)=S^(2−),Se^(2−),or Te^(2−)))have attracted great attention as excellent thermoelectric(TE)materials due to their extremely low lattice thermal conductivity(κl).Among them,Ag_(8)SnSe_(6)-based TE materials have high potential for TE applications.However,the pristine Ag_(8)SnSe_(6)materials have low carrier concentration(<1017 cm^(−3)),resulting in low power factors.In this study,a hydrothermal method was used to synthesize Ag_(8)SnSe_(6)with high purity,and the introduction of SnBr_(2)into the pristine Ag_(8)SnSe_(6)powders has been used to simultaneously increase the power factor and decrease the thermal conductivity(κ).On the one hand,a portion of the Br−ions acted as electrons to increase the carrier concentration,increasing the power factor to a value of~698 mW·m^(−1)·K^(−2)at 736 K.On the other hand,some of the dislocations and nanoprecipitates(SnBr_(2))were generated,resulting in a decrease ofκl(~0.13 W·m^(−1)·K^(−1))at 578 K.As a result,the zT value reaches~1.42 at 735 K for the sample Ag8Sn1.03Se5.94Br0.06,nearly 30%enhancement in contrast with that of the pristine sample(~1.09).The strategy of synergistic manipulation of carrier concentration and microstructure by introducing halogen compounds could be applied to the argyrodite compounds to improve the TE properties.