Jian Wang, Hongfei Hu, Lujie Jia, Jing Zhang, Quan Zhuang, Linge Li, Yongzheng Zhang, Dong Wang, Qinghua Guan, Huimin Hu, Meinan Liu, Liang Zhan, Henry Adenusi, Stefano Passerini, Hongzhen Lin
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引用次数: 0
摘要
基于水性电解质的低温锌电池(LT-ZIBs)因其自然资源丰富、成本低廉而在实际应用中大有可为。然而,由于笨重的 Zn(H2O)62+ 溶胶结构的解离和自由 Zn2+ 扩散,它们的动力学缓慢,能垒升高,导致寿命和性能不尽人意。与溶壳调整或层间距增大工程不同,本文提出通过构建固有缺陷工程使电子在阴极中脱域,从而实现快速电催化解溶,获得自由 Zn2+ 以进行插入/提取。密度泛函理论计算和界面光谱特性分析表明,固有的脱局域电子分布推动了 Zn(H2O)62+ 的解离,形成了可逆的间相,促进了 Zn2+ 在电解质/阴极界面上的扩散。在分层多孔碳(ODVO@HPC)上制造的富氧缺陷 V2O5 电极在 25 至 -20°C 的温度范围内表现出高容量稳定性。在-20°C下工作时,ODVO@HPC在50 A g-1的条件下可提供191 mAh g-1的电量,在10 A g-1的条件下可持续50 000次循环,与之前的报告相比,显著提高了低温环境下的功率密度和使用寿命。即使钮扣电池和袋装电池的平均质量负载为 ~13 mg cm-2,它们仍能保持出色的稳定性和平均容量,实现了实用的高性能 LT-ZIB。
Fast interfacial electrocatalytic desolvation enabling low-temperature and long-cycle-life aqueous Zn batteries
Low-temperature zinc batteries (LT-ZIBs) based on aqueous electrolytes show great promise for practical applications owing to their natural resource abundance and low cost. However, they suffer from sluggish kinetics with elevated energy barriers due to the dissociation of bulky Zn(H2O)62+ solvation structure and free Zn2+ diffusion, resulting in unsatisfactory lifespan and performance. Herein, dissimilar to solvation shell tuning or layer spacing enlargement engineering, delocalized electrons in cathode through constructing intrinsic defect engineering is proposed to achieve a rapid electrocatalytic desolvation to obtain free Zn2+ for insertion/extraction. As revealed by density functional theory calculations and interfacial spectroscopic characterizations, the intrinsic delocalized electron distribution propels the Zn(H2O)62+ dissociation, forming a reversible interphase and facilitating Zn2+ diffusion across the electrolyte/cathode interface. The as-fabricated oxygen defect-rich V2O5 on hierarchical porous carbon (ODVO@HPC) electrode exhibits high capacity robustness from 25 to −20°C. Operating at −20°C, the ODVO@HPC delivers 191 mAh g−1 at 50 A g−1 and lasts for 50 000 cycles at 10 A g−1, significantly enhancing the power density and lifespan under low-temperature environments in comparison to previous reports. Even with areal mass loading of ~13 mg cm−2, both coin cells and pouch batteries maintain excellent stability and areal capacities, realizing practical high-performance LT-ZIBs.
期刊介绍:
InfoMat, an interdisciplinary and open-access journal, caters to the growing scientific interest in novel materials with unique electrical, optical, and magnetic properties, focusing on their applications in the rapid advancement of information technology. The journal serves as a high-quality platform for researchers across diverse scientific areas to share their findings, critical opinions, and foster collaboration between the materials science and information technology communities.