Huang Yifan, Kong Fantao, Yu Xu, Yang Tao, Wu Ping, Shen Ruxiang, Zhuo Shangjun, Cui Xiangzhi, Shi Jianlin
State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
Adv Mater. 2025 Feb;37(7):e2419887. doi: 10.1002/adma.202419887. Epub 2024 Dec 30.
Nickel-iron layered double hydroxides (NiFe LDHs) are considered as promising substitutes for precious metals in oxygen evolution reaction (OER). However, most of the reported NiFe LDHs suffer from poor long-term stability because of the Fe loss during OER resulting in severe inactivation. Herein, a dynamically stable chelating interface through in situ transformation of asymmetric aldehyde-ligand (THB, 1,3,5-Tris(3'-hydroxy-4'-formylphenyl)-benzene) modified NiFe LDHs to anchor Fe and significantly enhance the OER stability is reported. The fabricated asymmetric aldehyde-containing ligand THB is capable of stimulating much more interfacial charge transfer from NiFe LDHs to the oxygen group of THB and accelerating the formation of highly valent active Fe species leading to the strong combination between Fe and ligand and the reduced activation energy barrier of the intermediate, respectively. The optimized aldehyde-ligand-chelated NiFe LDHs (NiFe LDH/THB) shows enhanced OER performance featuring an overpotential of 224 mV at 100 mA cm and robust stability for over 3860 h at 100 mA cm in a water splitting device maintaining a cell voltage of only 1.68 V, which paves a new avenue to improve the water electrolysis performance of non-noble metal catalysts.
镍铁层状双氢氧化物（NiFe LDHs）被认为是析氧反应（OER）中贵金属的有前途的替代品。然而，大多数已报道的NiFe LDHs由于在OER过程中的铁损失导致严重失活，长期稳定性较差。在此，报道了一种通过将不对称醛配体（THB，1,3,5-三（3'-羟基-4'-甲酰基苯基）-苯）修饰的NiFe LDHs原位转化来锚定铁并显著提高OER稳定性的动态稳定螯合界面。所制备的含不对称醛的配体THB能够刺激更多的界面电荷从NiFe LDHs转移到THB的氧基团，并加速高价活性铁物种的形成，分别导致铁与配体之间的强结合以及中间体活化能垒的降低。优化后的醛-配体螯合NiFe LDHs（NiFe LDH/THB）在析氧反应中表现出增强的性能，在100 mA cm时过电位为224 mV，在水电解装置中，在100 mA cm下保持仅1.68 V的电池电压时具有超过3860 h的稳健稳定性，这为提高非贵金属催化剂的水电解性能开辟了一条新途径。
