Li Han, Yan Guilong, Zhao Haoyue, Howlett Patrick C, Wang Xungai, Fang Jian
The Hong Kong Polytechnic University, JC STEM lab of Sustainable Fibers and Textiles, School of Fashion and Textiles, Hung Hom, Kowloon, Hong Kong, 999077, China.
School of New Energy and Materials, Southwest Petroleum University, Chengdu, 610500, China.
Adv Mater. 2024 Jun;36(26):e2311272. doi: 10.1002/adma.202311272. Epub 2024 Mar 25.
The rational construction of highly active and durable oxygen-reactive electrocatalysts for oxygen reduction/evolution reaction (ORR/OER) plays a critical role in rechargeable metal-air batteries. It is pivotal to achieve optimal utilization of electrocatalytically active sites and valid control of the high specific internal surface area. Inspiration for designing electrocatalysts can come from nature, as it is full of precisely manipulated and highly efficient structures. Herein, inspired by earthworms fertilizing soil, a 3D carbon nanofibrous electrocatalyst with multiple interconnected nanoconfined channels, cobalt-based heterojunction active particles and enriched N, S heteroatoms (Co/CoO/CoF@NSC with confined channels) is rationally designed, showing superior bifunctional electrocatalytic activity in alkaline electrolyte, even outperforming that of benchmark Pt/C-RuO catalyst. This work demonstrates a new method for porous structural regulation, in which the internal confined channels within the nanofibers are controllably formed by the spontaneous migration of cobalt-based nanoparticles under a CO atmosphere. Theoretical analysis reveals that constructing Co/CoO/CoF@NSC electrocatalyst with confined channels can greatly adjust the electron distribution, effectively lower the reaction barrier of inter-mediate and reduce the OER/ORR overpotential. This work introduces a novel and nature-inspired strategy for designing efficient bifunctional electrocatalysts with well-designed architectures.
用于氧还原/析氧反应(ORR/OER)的高活性和耐用性氧反应电催化剂的合理构建在可充电金属空气电池中起着关键作用。实现电催化活性位点的最佳利用和有效控制高比内表面积至关重要。设计电催化剂的灵感可以来自自然界,因为自然界充满了精确调控且高效的结构。在此,受蚯蚓给土壤施肥的启发,合理设计了一种具有多个相互连接的纳米受限通道、钴基异质结活性颗粒和富集的N、S杂原子的三维碳纳米纤维电催化剂(具有受限通道的Co/CoO/CoF@NSC),其在碱性电解质中表现出优异的双功能电催化活性,甚至优于基准Pt/C-RuO催化剂。这项工作展示了一种多孔结构调控的新方法,其中纳米纤维内的内部受限通道是通过钴基纳米颗粒在CO气氛下的自发迁移可控形成的。理论分析表明,构建具有受限通道的Co/CoO/CoF@NSC电催化剂可以极大地调整电子分布,有效降低中间体的反应势垒并降低OER/ORR过电位。这项工作引入了一种新颖的、受自然启发的策略,用于设计具有精心设计结构的高效双功能电催化剂。