• 文献标题:   Controlling the Thermoelectric Behavior of La-Doped SrTiO3 through Processing and Addition of Graphene Oxide
  • 文献类型:   Article
  • 作  者:   EKREN D, CAO JY, AZOUGH F, KEPAPTSOGLOU D, RAMASSE Q, KINLOCH IA, FREER R
  • 作者关键词:   srtio3, thermoelectric, grain boundary, graphene oxide, composite
  • 出版物名称:   ACS APPLIED MATERIALS INTERFACES
  • ISSN:   1944-8244 EI 1944-8252
  • 通讯作者地址:  
  • 被引频次:   2
  • DOI:   10.1021/acsami.2c14408 EA NOV 2022
  • 出版年:   2022

▎ 摘  要

The addition of graphene has been reported as a potential route to enhance the thermoelectric performance of SrTiO3. However, the interplay between processing parameters and graphene addition complicates understanding this enhancement. Herein, we examine the effects of processing parameters and graphene addition on the thermoelectric performance of La-doped SrTiO3 (LSTO). Briefly, two types of graphene oxide (GO) at different oxidation degrees were used, while the LSTO pellets were densified under two conditions with different reducing strengths (with/without using oxygen-scavenging carbon powder bed muffling). Raman imaging of the LSTO green body and sintered pellets suggests that the added GO sacrificially reacts with the lattice oxygen, which creates more oxygen vacancies and improves electrical conductivity regardless of the processing conditions. The addition of mildly oxidized electrochemical GO (EGO) yields better performance than the conventional heavily oxidized chemical GO (CGO). Moreover, we found that muffling the green body with an oxygen-scavenging carbon powder bed during sintering is vital to achieving a single-crystal-like temperature dependence of electrical conductivity, implying that a highly reducing environment is critical for eliminating the grain boundary barriers. Combining 1.0 wt % EGO addition with a highly reducing environment leads to the highest electrical conductivity of 2395 S cm-1 and power factor of 2525 mu W m-1 K-2 at 300 K, with an improved average zT value across the operating temperature range of 300-867 K. STEM-EELS maps of the optimized sample show a pronounced depletion of Sr and evident deficiency of O and La at the grain boundary region. Theoretical modeling using a twophase model implies that the addition of GO can effectively improve carrier mobility in the grain boundary phase. This work provides guidance for the development of high-performance thermoelectric ceramic oxides.