Hu Cun, Ding Fengyun, Liu Aojie, Zhou Linsen, Zeng Ning, Lv Chao, Zhang Xin, Yong Wenwen, Cai Jinguang, Tang Tao
Institute of Materials, China Academy of Engineering Physics, Jiangyou, 621908, Sichuan, China.
Institute of Materials, China Academy of Engineering Physics, Jiangyou, 621908, Sichuan, China.
J Colloid Interface Sci. 2024 Jul 15;666:331-345. doi: 10.1016/j.jcis.2024.04.027. Epub 2024 Apr 4.
Constructing heterostructured electrocatalysts has proven effective in enhancing intrinsic catalytic activity. Herein, under guidance of theoretical calculations, hierarchical porous quasi-hexagonal CoP nanosheets/Co heterostructures supported on carbon cloth (CoP/Co/CC) with a high surface area were rationally designed and elaborately constructed through electroless Co plating, electrochemical oxidation, and phosphidation process, which showed significant electrocatalytic performance toward water electrolysis. Specifically, theoretical calculations revealed that the CoP/Co heterostructure adjusted the electronic structure of CoP and Co, reducing the energy barrier for target reactions and thereby boosting electrocatalytic activities for the hydrogen evolution reaction (HER). Notably, the typical CoP/Co/CC catalyst demonstrated impressive HER performance, with low overpotentials of only 52 and 48 mV to achieve a current density of 10 mA/cm in 0.5 M HSO and 1.0 M KOH solutions, respectively. The remarkable electrocatalytic performance of the catalyst can be attributed to the improved intrinsic activity resulting from the CoP/Co heterostructures and the highly exposed active sites provided by the hierarchical porous structures. Furthermore, the CoP/Co/CC catalyst exhibited excellent oxygen evolution reaction (OER) performance in alkaline electrolyte, requiring a low overpotential of only 306 mV to achieve a current density of 100 mA/cm. Additionally, a two-electrode electrolyzer assembled with the CoP/Co/CC electrodes achieved a current density of 10 mA/cm at a low cell voltage of 1.54 V and demonstrated excellent long-term stability. This work presents a novel and feasible strategy for constructing hierarchical heterostructured electrocatalysts that enable efficient water electrolysis. By combining rational design and theoretical guidance, our approach offers promising prospects for advancing the field of electrocatalysis and facilitating sustainable energy conversion.
构建异质结构电催化剂已被证明在提高本征催化活性方面是有效的。在此，在理论计算的指导下，通过化学镀钴、电化学氧化和磷化过程，合理设计并精心构建了一种负载在碳布上的具有高表面积的分级多孔准六边形CoP纳米片/Co异质结构（CoP/Co/CC），该结构对水电解表现出显著的电催化性能。具体而言，理论计算表明，CoP/Co异质结构调整了CoP和Co的电子结构，降低了目标反应的能垒，从而提高了析氢反应（HER）的电催化活性。值得注意的是，典型的CoP/Co/CC催化剂表现出令人印象深刻的HER性能，在0.5 M H₂SO₄和1.0 M KOH溶液中，分别仅需52和48 mV的低过电位就能达到10 mA/cm²的电流密度。该催化剂卓越的电催化性能可归因于CoP/Co异质结构导致的本征活性提高以及分级多孔结构提供的高度暴露的活性位点。此外，CoP/Co/CC催化剂在碱性电解质中表现出优异的析氧反应（OER）性能，仅需306 mV的低过电位就能达到100 mA/cm²的电流密度。此外，用CoP/Co/CC电极组装的双电极电解槽在1.54 V的低电池电压下实现了10 mA/cm²的电流密度，并表现出优异的长期稳定性。这项工作提出了一种构建分级异质结构电催化剂以实现高效水电解的新颖可行策略。通过结合合理设计和理论指导，我们的方法为推进电催化领域和促进可持续能源转换提供了广阔前景。
