Chen Tien-Hung, Ni Chung-Sheng, Lai Chi-Yu, Gull Sanna, Chu Yun-Chen, Jao Wen-Yang, Hu Chi-Chang, Liu Shih-Fu, Chi Chong-Chi, Chen Tsung-Yi, Lee Jyh-Fu, Pao Chih-Wen, Chen Jeng-Lung, Chen Han-Yi, Huang Jin-Hua
Department of Material Science and Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan.
Department of Chemical Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan.
J Colloid Interface Sci. 2025 Feb;679(Pt A):119-131. doi: 10.1016/j.jcis.2024.09.187. Epub 2024 Sep 24.
Rechargeable zinc-air batteries (ZABs) are viewed as a promising solution for electric vehicles due to their potential to provide a clean, cost-effective, and sustainable energy storage system for the next generation. Nevertheless, sluggish kinetics of the oxygen evolution reaction (OER), the oxygen reduction reaction (ORR) at the air electrode, and low power density are significant challenges that hinder the practical application of ZABs. The key to resolving the development of ZABs is developing an affordable, efficient, and stable catalyst with bifunctional catalytic. In this study, we present a series of bifunctional catalysts composed of Co/Zn nanoparticles uniformly embedded in nitrogen-doped carbon (NC) and multi-walled carbon nanotubes (MWCNTs) denoted as Co/Zn@NC@MWCNTs. The incorporation of MWCNTs using a facile and non-toxic method significantly decreased the overpotential of the OER from 570 to 430 mV at 10 mA cm and the peak power density from 226 to 263 mW cm. Besides, the electrochemical surface area measurements and electrochemical impedance spectroscopy indicate that the three-dimensional (3D) network structure of MWCNTs facilitates mass transport for ORR and reduces electron transfer resistance during OER, leading to a small potential gap of 0.86 V between OER and ORR, high electron transfer number (3.92-3.98) of the ORR, and lowest Tafel slope (47.8 mV dec) of the OER in aqueous ZABs. In addition, in-situ Raman spectroscopy revealed a notable decrease in the I/I ratio for the optimally configured Co/Zn@NC@MWCNTs (75:25), indicating a reduction in defect density and improved structural ordering during the electrochemical process, which directly contributes to enhanced ORR activity. Hence, this study provides an excellent strategy for constructing a bifunctional catalyst material with a 3D MWCNTs conductive network for the development of advanced ZAB systems for sustainable energy applications.
可充电锌空气电池(ZABs)被视为电动汽车的一种有前景的解决方案,因为它们有潜力为下一代提供清洁、经济高效且可持续的储能系统。然而,空气电极处析氧反应(OER)、氧还原反应(ORR)的动力学缓慢以及功率密度低是阻碍ZABs实际应用的重大挑战。解决ZABs发展问题的关键在于开发一种价格合理、高效且稳定的双功能催化剂。在本研究中,我们展示了一系列由均匀嵌入氮掺杂碳(NC)和多壁碳纳米管(MWCNTs)中的Co/Zn纳米颗粒组成的双功能催化剂,记为Co/Zn@NC@MWCNTs。使用简便且无毒的方法引入MWCNTs,在10 mA cm时将OER的过电位从570 mV显著降低至430 mV,并将峰值功率密度从226 mW cm提高到263 mW cm。此外,电化学表面积测量和电化学阻抗谱表明,MWCNTs的三维(3D)网络结构有助于ORR的质量传输,并降低OER期间的电子转移电阻,导致在水性ZABs中OER和ORR之间的电位差小至0.86 V,ORR的高电子转移数(3.92 - 3.98)以及OER的最低塔菲尔斜率(47.8 mV dec)。此外,原位拉曼光谱显示,最佳配置的Co/Zn@NC@MWCNTs(75:25)的I/I比显著降低,表明在电化学过程中缺陷密度降低且结构有序性提高,这直接有助于增强ORR活性。因此,本研究为构建具有3D MWCNTs导电网络的双功能催化剂材料提供了一种出色的策略,以用于开发可持续能源应用的先进ZAB系统。