Zhanpeng Huang,Weiwei Zhang,Hong Zhang,Lin Fu,Bin Song,Wenli Zhang,Qianwang Chen,Ke Lu
Rough interfacial Zn electrodeposition and severe parasitic side reactions in aqueous electrolyte , resulting in increased internal resistance and limited reversibility, have significantly hindered the commercial deployment of Zn metal anode. Interfacial engineering offers a versatile platform for manipulating the zinc-ion flux and suppressing side reactions, via pre-formation of an artificial interlayer. Herein, we demonstrate a zincophile interphase based on metal-organic framework cation reservoir. The zinc hexacyanoferrate nanocubes with interconnected open cation transfer channels uniformize the interfacial electric field and render the protected electrode with faster zinc redox kinetic and higher exchange current density . The cations within the reservoir served as an ion-transfer mediator could regulate interfacial Zn 2+ even distribution and lower zinc-ion nucleation energy barrier, consequently promoting the homogeneous Zn electrodeposition. Additionally, the in situ pre-formed film also enhances the thermodynamic stability of metal anode and avoids the water-induced side interfacial reaction. The protected anode exhibits an extremely low voltage hysteresis and achieves a high average Coulombic efficiency (∼99.6%) for 400 h with dendrite-free behaviors. When coupled with an iodine cathode, the favorable electrochemical performance of full Zn–I 2 cells is realized, representing an advanced practical step toward stable Zn metal anode for real applications.
Fengwei Bai,Yan Li,Ziyu Chen,Yongchao Zhou,Chengzong Li,Tao Li
High-voltage lithium (Li)-metal batteries with cell-level energy density over 350 Wh kg −1 are promising energy storage systems . However, the aggressive interphase chemistries associated with highly reactive Li-metal anode and high-voltage cathodes impede their practical applications. Herein, we demonstrate the targeted stabilization of solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in high-voltage Li-metal batteries by asymmetrically sustained-releasing different additives. An asymmetric sustained-release film loaded with lithium bis-(oxalate)borate (LiBOB) and LiNO 3 on each side is investigated as a proof-of-concept. The sustained-releasing of LiBOB and LiNO 3 can maintain a localized concentration at the high-voltage cathode and Li-metal anode fronts respectively, thus forming a stable B-containing CEI and N-containing SEI. As such, issues like dendrites growth, parasitic side reactions and transition metals dissolution under high-voltage are addressed simultaneously. Based on this strategy, the 30 μm Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 (4.1 mAh cm −2 ) batteries deliver a capacity retention of 80% after 173 cycles under a cut-off voltage of 4.5 V.
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