Ultrahigh‐Speed Aqueous Copper Electrodes Stabilized by Phosphorylated Interphase

作者：Yuanhe Sun, Zeying Yao, Qi Lei, Yuanxin Zhao, Zhiguo Ren, Wei Zhang, Jingying Si, Lei Zhang, Wen Wen, Daming Zhu, Xiaolong Li, Renzhong Tai · 发表于：Advanced Materials · 年份：2023 · DOI：10.1002/adma.202305087 · 被引用次数：21 · 研究领域：Advanced battery technologies research、Advanced Battery Materials and Technologies、Supercapacitor Materials and Fabrication

Abstract High‐energy metal anodes for large‐scale reversible batteries with inexpensive and nonflammable aqueous electrolytes promise the capability of supporting higher current density, satisfactory lifetime, nontoxicity, and low‐cost commercial manufacturing, yet remain out of reach due to the lack of reliable electrode–electrolyte interphase engineering. Herein, in situ formed robust interphase on copper metal electrodes (CMEs) induced by a trace amount of potassium dihydrogen phosphate (0.05 m in 1 m CuSO 4 –H 2 O electrolyte) to fulfill all aforementioned requirements is demonstrated. Impressively, an unprecedented ultrahigh‐speed copper plating/stripping capability is achieved at 100 mA cm −2 for over 12 000 cycles, corresponding to an accumulative areal capacity up to tens of times higher than previously reported CMEs. The use of solid‐electrolyte interface‐protection strategy brings at least an order of magnitude improvement in cycling stability for symmetric cells (Cu||Cu, 2800 h) and full batteries with CMEs using either sulfur cathodes (S||Cu, 1000 cycles without capacity decay) or zinc anodes (Cu||Zn with all‐metal electrodes, discharge voltage ≈1.02 V). The comprehensive analysis reveals that the hydrophilic phosphate‐rich interphase nanostructures homogenize copper‐ion deposition and suppress nucleation overpotential, enabling dendrite‐free CMEs with sustainability and ability to tolerate unusual‐high power densities. The findings represent an elegant forerunner...