Tan Wanting, Hu Pengzhan, Feng Tianxiang, Zhao Siliang, Wang Shuai, Song Hui, Qi Zhaoyu, Li Wenjie
School of Ecology and Environment, Zhengzhou University, Zhengzhou 450001, China.
College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
Nanomaterials (Basel). 2025 Apr 11;15(8):585. doi: 10.3390/nano15080585.
Solid oxide electrolysis cells (SOECs) are considered one of the most promising technologies for carbon neutralization, as they can efficiently convert CO into CO fuel. SrFeMoO (SFM) double perovskite is a potential cathode material, but its catalytic activity for CO reduction needs further improvement. In this study, Cu ions were introduced to partially replace Mo ions in SFM to adjust the electrochemical performance of the cathode, and the role of the Cu atom was revealed. The results show Cu substitution induced lattice expansion and restrained impurity in the electrode. The particle size of the SrFeMoCuO (SFMC0.1) electrode was about 500 nm, and the crystallite size obtained from the Williamson-Hall plot was 75 nm. Moreover, Cu doping increased the concentration of oxygen vacancies, creating abundant electrochemical active sites, and led to a reduction in the oxidation states of Fe and Mo ions. Compared with other electrodes, the SFMC0.1 electrode exhibited the highest current density and the lowest polarization resistance. The current density of SFMC0.1 reached 202.20 mA cm at 800 °C and 1.8 V, which was 12.8% and 102.8% higher than the SFM electrodes with and without an isolation layer, respectively. Electrochemical impedance spectroscopy (EIS) analysis demonstrated that Cu doping not only promoted CO adsorption, dissociation and diffusion processes, but improved the charge transfer and oxygen ion migration. Theory calculations confirm that Cu doping lowered the surface and lattice oxygen vacancy formation energy of the material, thereby providing more CO active sites and facilitating oxygen ion transfer.
固体氧化物电解槽(SOECs)被认为是实现碳中和最具前景的技术之一,因为它们能够有效地将二氧化碳转化为一氧化碳燃料。锶铁钼氧化物(SFM)双钙钛矿是一种潜在的阴极材料,但其对一氧化碳还原的催化活性仍需进一步提高。在本研究中,引入铜离子部分取代SFM中的钼离子以调节阴极的电化学性能,并揭示了铜原子的作用。结果表明,铜取代导致晶格膨胀并抑制了电极中的杂质。SrFeMoCuO(SFMC0.1)电极的粒径约为500纳米,通过威廉姆森-霍尔图得到的微晶尺寸为75纳米。此外,铜掺杂增加了氧空位浓度,产生了丰富的电化学活性位点,并导致铁和钼离子的氧化态降低。与其他电极相比,SFMC0.1电极表现出最高的电流密度和最低的极化电阻。SFMC0.1在800℃和1.8V时的电流密度达到202.20 mA/cm²,分别比有和没有隔离层的SFM电极高12.8%和102.8%。电化学阻抗谱(EIS)分析表明,铜掺杂不仅促进了一氧化碳的吸附、解离和扩散过程,还改善了电荷转移和氧离子迁移。理论计算证实,铜掺杂降低了材料表面和晶格氧空位的形成能,从而提供了更多的一氧化碳活性位点并促进了氧离子转移。