Monolithic Phosphate Interphase for Highly Reversible and Stable Zn Metal Anode

Abstract

Zinc metal battery (ZMB) is promising as the next generation of energy storage system, but challenges relating to dendrites and corrosion of the zinc anode are restricting its practical application. Here, to stabilize Zn anode, we report a controlled electrolytic method for a monolithic solid‐electrolyte interphase (SEI) via a high dipole moment solvent dimethyl methylphosphonate (DMMP). The DMMP‐based electrolytes can generate a homogeneous and robust phosphate SEI (Zn3(PO4)2 and ZnP2O6). Benefiting from the protecting impact of this in situ monolithic SEI, the zinc electrode exhibits long‐term cycling of 4700 h and a high Coulombic efficiency 99.89 % in Zn|Zn and Zn|Cu cell, respectively. The full V2O5|Zn battery with DMMP‐H2O hybrid electrolyte exhibits a high capacity retention of 82.2 % following 4000 cycles under 5 A g−1. The first success in constructing the monolithic phosphate SEI will open a new avenue in electrolyte design for highly reversible and stable Zn metal anodes.

Aqueous all-manganese batteries

“…It was reported that in typical aqueous metal-ion batteries, the difference in the redox properties of different anions will have impact on the electrochemical behaviors of electrode reactions. 6,32 Considering the ability of different anions to coordinate with metal cations, 31,50 we firstly studied the Mn anode in three most commonly used Mn-based electrolytes, i.e. , manganese sulfate (MnSO 4 ), manganese chloride (MnCl 2 ) and manganese nitrate (Mn(NO 3 ) 2 ).…”

“…S2, ESI†). 13,49–51 This provides great opportunities for the Mn/Mn 2+ reactions to occur in some engineered electrolytes. Therefore, it is theoretically feasible to construct an AAMB with a theoretical potential of 2.42 V.…”

Recent progress of dendrite‐free stable zinc anodes for advanced zinc‐based rechargeable batteries: Fundamentals, challenges, and perspectives

“…Presently, it is acknowledged that the development of zinc anode is impeded by numerous issues, originating from dendrites formation, hydrogen evolution, corrosion and passivation, and their interactive influence. 39,40…”

Highly Potent and Low‐Volume Concentration Additives for Durable Aqueous Zinc Batteries: Machine Learning‐Enabled Performance Rationalization

“…The corresponding voltage-capacity profiles for G) additive-free and H) 1% Butandiol electrolyte cells at 2 mA cm −2 and 2 mAh cm −2 with 10 μm Zn. I) The comparison of cumulative plated capacity, electrolyte to capacity (E/C) ratio, Zn utilization, separator thickness, and additive concentration with other reported low-concentration organic additives [33][34][35] and in situ SEI [22,25,36,37] constructing electrolyte additives.…”

“…Nonetheless, the remarkable long-term zinc cycling reversibility exhibited under high Zn utilization, low E/C ratio, and thin separator, achieved with the low concentration (1 vol%) of the butanediol additive, exceeds the performance of nearly all previous additive-based research works. [22,25,[33][34][35][36][37]…”