Dai Mingxuan, Tong Yongcheng, He Wentao, Jiang Shuangting, Sun Zesi, Sun Wenping, Jiao Zhenjun, Tong Xiaofeng, Zhan Zhongliang
Deep Space Exploration Laboratory, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Key Laboratory of Precision and Intelligent Chemistry, Department of Materials Science & Engineering, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
ACS Appl Mater Interfaces. 2025 Jul 2;17(26):37879-37888. doi: 10.1021/acsami.5c04996. Epub 2025 Jun 16.
Protonic ceramic cells are an emerging solid-state device for the efficient conversion between electricity and fuels. Ni cermet electrodes with a protonic ceramic matrix such as BaZrCeYO (BZCY) are highly active for hydrogen oxidation and evolution reactions. Nevertheless, performance deterioration remains problematic for their practical applications due to poor ceramic-metal wettability and the resultant interfacial debonding. Here, we show that the catalytic durability of Ni-BZCY cermets can be effectively enhanced by introducing CeGdO (GDC) into the ceramic matrix, which acts as an anchoring component to thermodynamically promote Ni/BZCY wettability and thereby increases the microstructural stability, as demonstrated by phase-field modeling. Density-functional theory (DFT) calculations reveal more charge transfer from metallic Ni and larger adsorption energy of Ni clusters on GDC, yielding stronger ceramic-metal interaction and higher Ni wettability than on BZCY. Symmetrical protonic ceramic cells with GDC-modified Ni-BZCY cermet electrodes can produce a stable H pumping flux of 7.37 mL·min·cm with an electricity consumption of 0.90 kWh·Nm at 700 °C. This work highlights the critical role of interfacial wettability in typical heterogeneous electrocatalysis and offers some insights and practices for the design of highly durable catalysts.
质子陶瓷电池是一种新兴的固态装置，可实现电与燃料之间的高效转换。具有质子陶瓷基体（如BaZrCeYO，简称BZCY）的镍基金属陶瓷电极对氢氧化反应和析氢反应具有很高的活性。然而，由于陶瓷与金属的润湿性差以及由此导致的界面脱粘，其性能劣化仍然是实际应用中的一个问题。在此，我们表明，通过将CeGdO（简称GDC）引入陶瓷基体中，可以有效提高Ni-BZCY金属陶瓷的催化耐久性，GDC作为一种锚定成分，从热力学角度促进Ni/BZCY的润湿性，从而提高微观结构稳定性，相场模拟证明了这一点。密度泛函理论（DFT）计算表明，与BZCY相比，金属Ni向GDC的电荷转移更多，Ni团簇在GDC上的吸附能更大，从而产生更强的陶瓷-金属相互作用和更高的Ni润湿性。具有GDC修饰的Ni-BZCY金属陶瓷电极的对称质子陶瓷电池在700℃下可产生7.37 mL·min·cm稳定的H泵浦通量，耗电量为0.90 kWh·Nm。这项工作突出了界面润湿性在典型的多相电催化中的关键作用，并为设计高耐久性催化剂提供了一些见解和实践方法。
