Yang Jun, Shen Yong, Xian Jiahui, Xiang Runan, Li Guangqin
MOE Laboratory of Bioinorganic and Synthetic Chemistry, GBRCE for Functional Molecular Engineering, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University Guangzhou 510006 China
School of Chemical Engineering, Guangdong University of Petrochemical Technology Maoming 525000 China.
Chem Sci. 2024 Nov 22;16(2):685-692. doi: 10.1039/d4sc06574c. eCollection 2025 Jan 2.
Based on the target of carbon neutrality, it is very important to explore highly active and durable electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, a series of NiFe-based metal-organic frameworks (MOFs) with the doping of various rare-earth elements (Ce, Y, and La) were grown on nickel foam by a facile solvothermal process. The representative CeNiFe-MOF showed amazing OER performance with ultralow overpotentials of 224 and 277 mV at 500 mA cm in 1.0 M KOH and 1.0 M KOH + seawater, respectively. Moreover, it also exhibited favorable activity and durability for both alkaline freshwater and seawater splitting. Theoretical calculations unveiled that Ce doping effectively optimized the adsorption energy of H* and reduced the energy barrier from *OH to *O, thus leading to significant promotion of HER and OER performance. This work provided new inspiration for the electron modulation and activity optimization of MOF-based electrocatalysts.
基于碳中和目标，探索用于析氢反应（HER）和析氧反应（OER）的高活性和耐用性电催化剂非常重要。在此，通过简便的溶剂热法在泡沫镍上生长了一系列掺杂各种稀土元素（Ce、Y和La）的镍铁基金属有机框架（MOF）。具有代表性的CeNiFe-MOF在1.0 M KOH和1.0 M KOH + 海水中，在500 mA cm时分别具有224和277 mV的超低过电位，展现出惊人的OER性能。此外，它在碱性淡水和海水分解方面也表现出良好的活性和耐久性。理论计算表明，Ce掺杂有效地优化了H的吸附能，降低了从OH到*O的能垒，从而显著促进了HER和OER性能。这项工作为基于MOF的电催化剂的电子调制和活性优化提供了新的灵感。
