Lan Jing, Yu Yuran, Miao Fujun, Zhang Peng, Shao Guosheng
State Center for International Cooperation on Designer Low-Carbon and Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, 100 Kexue Avenue, Zhengzhou 450001, China.
Zhengzhou Materials Genome Institute (ZMGI), Zhongyuanzhigu, Xingyang, Zhengzhou 450100, China.
Nanoscale. 2024 May 30;16(21):10283-10291. doi: 10.1039/d4nr00263f.
Lithium-oxygen batteries (LOBs) with extraordinarily high energy density are some of the most captivating energy storage devices. Designing an efficient catalyst system that can minimize the energy barriers and address the oxidant intermediate and side-product issues is the major challenge regarding LOBs. Herein, we have developed a new type of integrated cathode of Cu foam-supported hierarchical nanowires decorated with highly catalytic Au nanoparticles which achieves a good combination of a gas diffusion electrode and a catalyst electrode, contributing to the synchronous multiphase transport of ions, oxygen, and electrons as well as improving the cathode reaction kinetics effectively. Benefiting from such a unique hierarchical architecture, the integrated cathode delivered superior electrochemical performance, including a high discharge capacity of up to 11.5 mA h cm and a small overpotential of 0.49 V at 0.1 mA cm, a favorable energy efficiency of 84.3% and exceptional cycling stability with nearly 1200 h at 0.1 mA cm under a fixed capacity of 0.25 mA h cm. Furthermore, density functional theory (DFT) calculations further reveal the intrinsic direct catalytic ability to form/decompose LiO during the ORR/OER process. As a consequence, this work provides an insightful investigation on the structural engineering of catalysts and holds great potential for advanced integrated cathode design for LOBs.
具有极高能量密度的锂氧电池(LOBs)是最具吸引力的储能设备之一。设计一种能够最小化能量势垒并解决氧化剂中间体和副产物问题的高效催化剂体系是锂氧电池面临的主要挑战。在此,我们开发了一种新型的集成阴极,它是由泡沫铜支撑的分层纳米线,表面装饰有高催化活性的金纳米颗粒,实现了气体扩散电极和催化剂电极的良好结合,有助于离子、氧气和电子的同步多相传输,并有效改善阴极反应动力学。受益于这种独特的分层结构,该集成阴极展现出优异的电化学性能,包括高达11.5 mA h cm的高放电容量以及在0.1 mA cm下0.49 V的小过电位、84.3%的良好能量效率和在0.1 mA cm固定容量为0.25 mA h cm下近1200 h的出色循环稳定性。此外,密度泛函理论(DFT)计算进一步揭示了在氧还原反应/析氧反应(ORR/OER)过程中形成/分解LiO的内在直接催化能力。因此,这项工作为催化剂的结构工程提供了有见地的研究,并为锂氧电池的先进集成阴极设计具有巨大潜力。