Chu Jing, Huang Jian, Liu Ruiheng, Liao Jincheng, Xia Xugui, Zhang Qihao, Wang Chao, Gu Ming, Bai Shengqiang, Shi Xun, Chen Lidong
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Nat Commun. 2020 Jun 1;11(1):2723. doi: 10.1038/s41467-020-16508-x.
Although the CoSb-based skutterudite thermoelectric devices have been highly expected for wide uses such as waste heat recovery and space power supply, the limited long-term service stability majorly determined by the degradation of electrode interface obstructs its applications. Here, we built up an effective criterion for screening barrier layer based on the combination of negative interfacial reaction energy and high activation energy barrier of Sb migration through the formed interfacial reaction layer. Accordingly, we predicted niobium as a promising barrier layer. The experimental results show the skutterudite/Nb joint has the slowest interfacial reaction layer growth rate and smallest interfacial electrical resistivity. The fabricated 8-pair skutterudite module using Nb as barrier layer achieves a recorded conversion efficiency of 10.2% at hot-side temperature of 872 K and shows excellent stability during long-time aging. This simple criterion provides an effective guidance on screening barrier layer with bonding-blocking-conducting synergetic functions for thermoelectric device integration.
尽管基于CoSb的方钴矿热电装置在废热回收和空间供电等广泛应用方面备受期待，但由电极界面退化主要决定的有限长期服役稳定性阻碍了其应用。在此，我们基于负界面反应能与Sb通过形成的界面反应层迁移的高活化能垒的组合，建立了一种筛选阻挡层的有效准则。据此，我们预测铌是一种有前景的阻挡层。实验结果表明，方钴矿/铌接头具有最慢的界面反应层生长速率和最小的界面电阻率。使用铌作为阻挡层制造的8对方钴矿模块在872 K的热侧温度下实现了创纪录的10.2%的转换效率，并且在长时间老化过程中表现出优异的稳定性。这一简单准则为筛选具有键合-阻挡-传导协同功能的阻挡层以用于热电装置集成提供了有效指导。
