Liu Xin, Bai Li, Guo Xinrong, Li Haoyu, Liu Xiaoyan, Cao Jian, Yang Lili, Wei Maobin, Chen Yanli, Liu Huilian, Tao Qiang
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, China.
National Demonstration Center for Experimental Physics Education, Jilin Normal University, Siping 136000, China.
Molecules. 2025 Mar 25;30(7):1461. doi: 10.3390/molecules30071461.
The construction of high-performance catalysts for overall water splitting (OWS) is crucial. Nickel-iron-layered double hydroxide (NiFe LDH) is a promising catalyst for OWS. However, the slow kinetics of the HER under alkaline conditions seriously hinder the application of NiFe LDH in OWS. This work presents a strategy to optimize OWS performance by adjusting the entropy of multi-metallic LDH. Quaternary NiFeCrCo LDH was constructed, which exhibited remarkable OWS activity. The OER and HER of NiFeCrCo LDH were stable for 100 h and 80 h, respectively. The OWS activity of NiFeCrCo LDH//NiFeCrCo LDH only required 1.42 V to reach 10 mA cm, and 100 mA cm required 1.54 V. Under simulated seawater conditions, NiFeCrCo LDH//NiFeCrCo LDH required 1.57 V to reach 10 mA cm and 1.71 V to reach 100 mA cm. The introduction of Co into the structure induced Cr to provide more electrons to Fe, which regulated the electronic state of NiFeCrCo LDH. The appropriate electronic state of the structure is essential for the remarkable performance of OWS. This work proposes a new strategy to achieve excellent OWS performance through entropy-increase engineering.
构建用于全水解（OWS）的高性能催化剂至关重要。镍铁层状双氢氧化物（NiFe LDH）是一种很有前景的OWS催化剂。然而，碱性条件下析氢反应（HER）的缓慢动力学严重阻碍了NiFe LDH在OWS中的应用。这项工作提出了一种通过调节多金属LDH的熵来优化OWS性能的策略。构建了四元NiFeCrCo LDH，其表现出显著的OWS活性。NiFeCrCo LDH的析氧反应（OER）和HER分别稳定100小时和80小时。NiFeCrCo LDH//NiFeCrCo LDH的OWS活性仅需1.42 V即可达到10 mA cm，达到100 mA cm则需要1.54 V。在模拟海水条件下，NiFeCrCo LDH//NiFeCrCo LDH达到10 mA cm需要1.57 V，达到100 mA cm需要1.71 V。Co引入结构中促使Cr向Fe提供更多电子，从而调节了NiFeCrCo LDH的电子态。结构的适当电子态对于OWS的卓越性能至关重要。这项工作提出了一种通过熵增工程实现优异OWS性能的新策略。
