Chen Ze, Wang Shengnan, Wei Zhiquan, Wang Yiqiao, Wu Zhuoxi, Hou Yue, Zhu Jiaxiong, Wang Yanbo, Liang Guojin, Huang Zhaodong, Chen Ao, Wang Donghong, Zhi Chunyi
Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong 999077, China.
Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE), Shatin, Hong Kong 999077, China.
J Am Chem Soc. 2023 Sep 20;145(37):20521-20529. doi: 10.1021/jacs.3c06488. Epub 2023 Sep 6.
Chalcogens, especially tellurium (Te), as conversion-type cathodes possess promising prospects for zinc batteries (ZBs) with potential rich valence supply and high energy density. However, the conversion reaction of Te is normally restricted to the Te/Te redox with a low voltage plateau at ∼0.59 V (vs Zn/Zn) rather than the expected positive valence conversion of Te to Te, inhibiting the development of Te-based batteries toward high output voltage and energy density. Herein, the desired reversible Te/Te/Te/Te redox behavior with up to six-electron transfer was successfully activated by employing a highly concentrated Cl-containing electrolyte (Cl as strong nucleophile) for the first time. Three flat discharge plateaus located at 1.24, 0.77, and 0.51 V, respectively, are attained with a total capacity of 802.7 mAh g. Furthermore, to improve the stability of Te products and enhance the cycling stability, a modified ionic liquid (IL)-based electrolyte was fabricated, leading to a high-performance Zn∥Te battery with high areal capacity (7.13 mAh cm), high energy density (542 Wh kg or 227 Wh L), excellent cycling performance, and a low self-discharge rate based on 400 mAh-level pouch cell. The results enhance the understanding of tellurium chemistry in batteries, substantially promising a remarkable route for advanced ZBs.
硫族元素,尤其是碲(Te),作为转换型阴极,对于具有丰富价态供应潜力和高能量密度的锌电池(ZB)具有广阔的前景。然而,Te的转换反应通常局限于Te/Te氧化还原,在约0.59 V(相对于Zn/Zn)处有一个低电压平台,而不是预期的Te从正价态转换为Te,这抑制了基于Te的电池向高输出电压和能量密度方向的发展。在此,首次通过使用高浓度含Cl电解质(Cl作为强亲核试剂)成功激活了所需的具有多达六电子转移的可逆Te/Te/Te/Te氧化还原行为。分别在1.24、0.77和0.51 V处获得了三个平坦的放电平台,总容量为802.7 mAh g。此外,为了提高Te产物的稳定性并增强循环稳定性,制备了一种改性的基于离子液体(IL)的电解质,从而得到了一种高性能的Zn∥Te电池,该电池具有高面积容量(7.13 mAh cm)、高能量密度(542 Wh kg或227 Wh L)、优异的循环性能以及基于400 mAh级软包电池的低自放电率。这些结果加深了对电池中碲化学的理解,为先进的锌电池开辟了一条极具前景的路线。