Zhao Wei, Jin Kangpeng, Fu Liangwei, Shi Zhan, Xu Biao
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.
Nano Lett. 2022 Jun 22;22(12):4750-4757. doi: 10.1021/acs.nanolett.2c00947. Epub 2022 May 31.
Single-atom materials are widely explored in catalysis, batteries, sensors, etc. However, limited by mass production and centimeter-scale assembly, they are rarely studied in thermoelectrics. Herein, we demonstrate a solvothermal synthesis assisted by a syringe-pump method to yield BiS-supported Pt single-atom materials (BiS-Pt) at a 10 g scale. Different from Pt clusters, Pt single atoms can increase carrier concentration at a high doping efficiency and provide a unique atomic environment to enhance carrier mobility, and an enlarged effective mass leads to an enhanced Seebeck coefficient. As a result, a high power factor (348 μW m K) is achieved at 823 K. Benefiting from the scattering of phonons by Pt atomic sites, a minimum thermal conductivity of 0.37 W m K is achieved. Consequently, the BiS-0.5 wt % Pt realizes a record-high of ∼0.75 at 823 K, being among the best in the state-of-the-art n-type environmentally friendly metal sulfides. The enhancement of the carrier mobility and suppression of the thermal conduction by the unique Pt single atoms will inspire various fields, as exemplified by electronic devices and thermal management.
单原子材料在催化、电池、传感器等领域得到了广泛研究。然而,受限于大规模生产和厘米级组装,它们在热电领域的研究较少。在此,我们展示了一种由注射泵辅助的溶剂热合成方法,可大规模(10 g)制备BiS负载的Pt单原子材料(BiS-Pt)。与Pt团簇不同,Pt单原子能够以高掺杂效率增加载流子浓度,并提供独特的原子环境以提高载流子迁移率,而增大的有效质量会导致塞贝克系数增强。结果,在823 K时实现了高功率因子(348 μW m K)。受益于Pt原子位点对声子的散射,实现了最低热导率0.37 W m K。因此,BiS-0.5 wt% Pt在823 K时实现了创纪录的约0.75,在最先进的n型环境友好金属硫化物中名列前茅。独特的Pt单原子对载流子迁移率的增强和对热传导的抑制将为电子器件和热管理等各个领域带来启发。