Hao Junnan, Yuan Libei, Zhu Yilong, Jaroniec Mietek, Qiao Shi-Zhang
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, South Australia, 5005, Australia.
Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, New South Wales, 2522, Australia.
Adv Mater. 2022 Nov;34(44):e2206963. doi: 10.1002/adma.202206963. Epub 2022 Oct 3.
The poor Zn reversibility has been criticized for limiting applications of aqueous Zn-ion batteries (ZIBs); however, its behavior in aqueous media is not fully uncovered yet. Here, this knowledge gap is addressed, indicating that Zn electrodes face a O -involving corrosion, besides H evolution and dendrite growth. Differing from aqueous Li/Na batteries, removing O cannot enhance ZIB performance because of the aggravated competing H evolution. To address Zn issues, a one-off electrolyte strategy is reported by introducing the triple-function C H Na O P, which can take effects during the shelf time of battery. It regulates H concentration and reduces free-water activity, inhibiting H evolution. A self-healing solid/electrolyte interphase (SEI) can be triggered before battery operation, which suppresses O adsorption corrosion and dendritic deposition. Consequently, a high Zn reversibility of 99.6% is achieved under a high discharge depth of 85%. The pouch full-cell with a lean electrolyte displays a record lifespan with capacity retention of 95.5% after 500 cycles. This study not only looks deeply into Zn behavior in aqueous media but also underscores rules for the design of active metal anodes, including Zn and Li metals, during shelf time toward real applications.
锌的可逆性较差，这一问题一直被认为限制了水系锌离子电池（ZIBs）的应用；然而，其在水性介质中的行为尚未完全被揭示。在此，我们填补了这一知识空白，表明锌电极除了析氢和枝晶生长外，还面临涉及氧的腐蚀。与水系锂/钠电池不同，去除氧并不能提高ZIB的性能，因为析氢竞争加剧。为了解决锌的问题，我们报道了一种一次性电解质策略，通过引入具有三重功能的C H Na O P，它可以在电池的储存期内发挥作用。它调节氢离子浓度并降低自由水活性，抑制析氢。在电池运行前可以触发一种自愈的固体/电解质界面（SEI），从而抑制氧吸附腐蚀和枝晶沉积。因此，在85%的高放电深度下实现了99.6%的高锌可逆性。具有贫电解质的软包全电池显示出创纪录的寿命，在500次循环后容量保持率为95.5%。这项研究不仅深入研究了锌在水性介质中的行为，还强调了在面向实际应用的储存期内设计包括锌和锂金属在内的活性金属负极的规则。
