Bai Jirong, Chen Changfan, Lian Yuebin, Deng Yaoyao, Xiang Mei, Zhou Quanfa, Tang Yawen, Su Yaqiong
Research Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China; Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China.
Research Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China.
J Colloid Interface Sci. 2024 Jun;663:280-286. doi: 10.1016/j.jcis.2024.02.093. Epub 2024 Feb 15.
Amorphous engineering and atomistic doping provide an effective way to improve the catalytic activity in the oxygen evolution reaction (OER) of transition metal layered double hydroxides. Herein, Cerium (Ce) was introduced into NiFe-based oxyhydroxide using a modified aqueous sol-gel procedure. Ce as an electron acceptor promoted the coupling oxidation of Ni/ in NiFe oxyhydroxide, and the activated oxyhydroxide showed excellent catalytic activity in OER. The amorphous NiFeCe oxyhydroxide electrocatalyst demonstrated great modified OER catalytic activity under alkaline conditions and excellent cyclic stability, with an overpotential of only 284 mV at 50 mA cm, which was significantly better than amorphous NiFe oxyhydroxide and crystalline NiFeCe oxyhydroxide. Theoretical investigations further indicated that the overpotential of the rate-determining step (*OOH deprotonation) decreased from 0.66 to 0.41 V after Ce doping and strong electron interaction, effectively reducing the dependence of proton activity in the solution of OER, and optimizing the adsorption/desorption process of related oxygen-containing species in the reaction. This work also provides a good reference for optimizing OER activity by using rare-earth-metal induced electronic regulation strategies.
非晶态工程和原子掺杂为提高过渡金属层状双氢氧化物析氧反应(OER)的催化活性提供了一种有效方法。在此,采用改进的水溶胶-凝胶法将铈(Ce)引入到镍铁基羟基氧化物中。Ce作为电子受体促进了镍铁羟基氧化物中Ni/的耦合氧化,活化后的羟基氧化物在OER中表现出优异的催化活性。非晶态NiFeCe羟基氧化物电催化剂在碱性条件下表现出极大的改性OER催化活性和优异的循环稳定性,在50 mA cm时过电位仅为284 mV,明显优于非晶态NiFe羟基氧化物和晶态NiFeCe羟基氧化物。理论研究进一步表明,Ce掺杂和强电子相互作用后,速率决定步骤(*OOH去质子化)的过电位从0.66降至0.41 V,有效降低了OER溶液中质子活性的依赖性,并优化了反应中相关含氧化合物的吸附/解吸过程。这项工作也为采用稀土金属诱导电子调控策略优化OER活性提供了很好的参考。