Liu Wenjun, Zhao Junze, Dai Liming, Qi Yanli, Liang Kang, Bao Jian, Ren Yurong
School of Material Science & Engineering, Changzhou University, Changzhou 213164, P. R. China.
Institute for Energy Research, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, P. R. China.
Inorg Chem. 2024 Apr 1;63(13):6016-6025. doi: 10.1021/acs.inorgchem.4c00303. Epub 2024 Mar 18.
Exploring advanced electrocatalysts for overall seawater splitting is of great significance for large-scale green hydrogen production in which interface engineering has been considered as an effective strategy to enhance the intrinsic activities of the electrocatalysts. In this work, CeO-modified NiCoO nanoneedle arrays are designed and constructed in situ grown on Ni foam (NF) through a facile two-step synthesis method. Density functional theory calculations reveal that the strong interaction between CeO and NiCoO can regulate the electronic states of metal surfaces and optimize the electronic structures of the materials, essentially improving the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) properties. Specifically, in alkaline electrolytes, CeO@NiCoO/NF exhibits superior electrocatalytic activities and stabilities, requiring overpotentials of 238 mV for the OER and 144 mV for the HER to achieve a current density of 10 mA cm. When applied to a simulated seawater splitting device, the CeO@NiCoO/NF also maintains a battery voltage of 1.66 V to reach 10 mA cm and exhibits good stability for over 60 h, with high faradic efficiencies (FEs) close to 100% for both the OER and HER.
探索用于全海水分解的先进电催化剂对于大规模绿色制氢具有重要意义，其中界面工程被认为是提高电催化剂本征活性的有效策略。在这项工作中，通过简便的两步合成方法设计并构建了CeO修饰的NiCoO纳米针阵列，并使其原位生长在泡沫镍（NF）上。密度泛函理论计算表明，CeO与NiCoO之间的强相互作用可以调节金属表面的电子态并优化材料的电子结构，从本质上改善析氧反应（OER）和析氢反应（HER）性能。具体而言，在碱性电解质中，CeO@NiCoO/NF表现出优异的电催化活性和稳定性，在电流密度达到10 mA cm时，OER的过电位为238 mV，HER的过电位为144 mV。当应用于模拟海水分解装置时，CeO@NiCoO/NF在电流密度达到10 mA cm时也能保持1.66 V的电池电压，并在超过60小时的时间内表现出良好的稳定性，OER和HER的法拉第效率（FE）均接近100%。
