Affiliation: | 1. Sauvage Laboratory for Smart Materials, State Key Laboratory of Advanced Welding and Joining, Shenzhen Key Laboratory of Flexible Printed Electronics Technology, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen, 518055 China These authors contributed equally to this work.;2. Key Laboratory of Radiation Physics and Technology of Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University, Chengdu, 610064 China These authors contributed equally to this work.;3. Sauvage Laboratory for Smart Materials, State Key Laboratory of Advanced Welding and Joining, Shenzhen Key Laboratory of Flexible Printed Electronics Technology, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen, 518055 China;4. Education Center of Experiments and Innovation, Harbin Institute of Technology (Shenzhen), Shenzhen, 518055 China;5. Key Laboratory of Radiation Physics and Technology of Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University, Chengdu, 610064 China;6. College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060 China |
Abstract: | In aqueous electrolytes, the uncontrollable interfacial evolution caused by a series of factors such as pH variation and unregulated Zn2+ diffusion would usually result in the rapid failure of metallic Zn anode. Considering the high correlation among various triggers that induce the anode deterioration, a synergistic modulation strategy based on electrolyte modification is developed. Benefitting from the unique pH buffer mechanism of the electrolyte additive and its capability to in situ construct a zincophilic solid interface, this synergistic effect can comprehensively manage the thermodynamic and kinetic properties of Zn anode by inhibiting the pH variation and parasitic side reactions, accelerating de-solvation of hydrated Zn2+, and regulating the diffusion behavior of Zn2+ to realize uniform Zn deposition. Thus, the modified Zn anode can achieve an impressive lifespan at ultra-high current density and areal capacity, operating stably for 609 and 209 hours at 20 mA cm−2, 20 mAh cm−2 and 40 mA cm−2, 20 mAh cm−2, respectively. Based on this exceptional performance, high loading Zn||NH4V4O10 batteries can achieve excellent cycle stability and rate performance. Compared with those previously reported single pH buffer strategies, the synergistic modulation concept is expected to provide a new approach for highly stable Zn anode in aqueous zinc-ion batteries. |