Yuan Qingyuan, Liu Tingting, Ma Dui, Liao Yong, Wang Weizhi, Meng Hongtao, You Qifan, Zeng Fanyan, Xie Meilan, Huang Hongbo, Liu Cailing, Liang Xiao
School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063 PR China.
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082 PR China.
J Colloid Interface Sci. 2025 Apr 15;684(Pt 1):783-791. doi: 10.1016/j.jcis.2025.01.055. Epub 2025 Jan 9.
High-entropy phosphides (HEPs) have garnered increasing interest as innovative electrocatalysts for water splitting, highlighted by their distinctive catalytic activity, elemental synergy, and tunable electronic configuration. Herein, a novel electrode comprising CoNiCuZnFeP nanocubes with rich phosphorus vacancies was fabricated through coprecipitation and phosphorization two-step method. The synergistic interaction among metal elements and the modulation of the electronic configuration by phosphorus vacancies augmentation enhance the catalytic performance for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). The CoNiCuZnFeP catalyst demonstrates overpotentials of 318 mV for HER and 204 mV for OER at 100 mA cm, while maintaining a remarkable durability exceeding 700 h. The catalyst, as the dual-electrode for water electrolysis, requires a voltage of 1.74 V to attain 100 mA cm. Theoretical calculations reveal that the combination of high entropy and phosphorus vacancies can effectively regulate the local charge distribution and electronic characteristics of phosphides, leading to the optimization of adsorption energies and the reduction of the potential energy barrier for water decomposition. This study provides an attractive OER electrocatalyst for renewable hydrogen via efficient water splitting, and paves the way for the design of efficient and stable electrocatalysts with high-entropy materials.
高熵磷化物（HEPs）作为用于水分解的创新型电催化剂，因其独特的催化活性、元素协同作用和可调节的电子构型而受到越来越多的关注。在此，通过共沉淀和磷化两步法制备了一种包含具有丰富磷空位的CoNiCuZnFeP纳米立方体的新型电极。金属元素之间的协同相互作用以及通过增加磷空位对电子构型的调制增强了析氧反应（OER）和析氢反应（HER）的催化性能。CoNiCuZnFeP催化剂在100 mA cm时，HER的过电位为318 mV，OER的过电位为204 mV，同时保持超过700小时的显著耐久性。该催化剂作为水电解的双电极，达到100 mA cm需要1.74 V的电压。理论计算表明，高熵和磷空位的结合可以有效地调节磷化物的局部电荷分布和电子特性，从而优化吸附能并降低水分解的势能垒。本研究通过高效水分解提供了一种有吸引力的用于可再生氢的OER电催化剂，并为设计具有高熵材料的高效稳定电催化剂铺平了道路。
