Pang Huimei, Qiu Yuting, Wang Dongyang, Qin Yongxin, Huang Rong, Yang Zhenzhong, Zhang Xiao, Zhao Li-Dong
School of Materials Science and Engineering, Beihang University, Beijing 100191, China.
Beihang School, Beihang University, Beijing 100191, China.
J Am Chem Soc. 2021 Jun 16;143(23):8538-8542. doi: 10.1021/jacs.1c02346. Epub 2021 Jun 2.
Due to the intrinsically plentiful Sn vacancies, developing n-type SnTe thermoelectric materials is a big challenge. Herein, n-type SnTe thermoelectric materials with remarkable performance were successfully synthesized through suppressing Sn vacancies, followed by electron-doping. Pb alloying notably depressed the Sn vacancies via populating Sn vacancies in SnTe (supported by transmission electron microscopy), and the electrical transports were shifted from p-type to n-type through introducing electrons using I doping. In the n-type SnTe, we found that the electrical conductivity could be enhanced by increased carrier mobility through sharpening conduction bands after alloying Pb, while the lattice thermal conductivity could be reduced via strong phonon scattering after introducing defects by Pb alloying and I doping. Resulting from these enhancements, the n-type SnPbTeI achieves a notably high ∼ 0.8 at 573 K and a remarkable ∼ 0.51 at 300-823 K, which can match many excellent p-type SnTe. This work indicates that n-type SnTe could be experimentally acquired and is a promising candidate for thermoelectric generation, which will stimulate further research on n-type SnTe thermoelectric materials and even devices on the basis of both n- and p-type SnTe legs.
由于本质上存在大量的锡空位,开发n型锡碲化物热电材料是一项巨大挑战。在此,通过抑制锡空位并随后进行电子掺杂,成功合成了具有卓越性能的n型锡碲化物热电材料。铅合金化通过在锡碲化物中填充锡空位显著降低了锡空位(由透射电子显微镜证实),并且通过碘掺杂引入电子使电输运从p型转变为n型。在n型锡碲化物中,我们发现通过在铅合金化后锐化导带来提高载流子迁移率可增强电导率,而通过铅合金化和碘掺杂引入缺陷后通过强声子散射可降低晶格热导率。由于这些增强作用,n型锡铅碲碘化物在573 K时实现了显著高的约0.8,在300 - 823 K时达到了显著的约0.51,这可与许多优异的p型锡碲化物相匹配。这项工作表明n型锡碲化物可以通过实验获得,并且是热电发电的有前途的候选材料,这将激发基于n型和p型锡碲化物支腿的n型锡碲化物热电材料甚至器件的进一步研究。