Aqueous Ni-Zn microbatteries are safe,reliable and inexpensive but notoriously suffer from inadequate energy and power densities.Herein,we present a novel mechanism of superoxide-activated Ni substrate that realizes t...Aqueous Ni-Zn microbatteries are safe,reliable and inexpensive but notoriously suffer from inadequate energy and power densities.Herein,we present a novel mechanism of superoxide-activated Ni substrate that realizes the redox reaction featuring three-electron transfers(Ni↔Ni3+).The superoxide activates the direct redox reaction between Ni substrate and KNiO_(2)by lowering the reaction Gibbs free energy,supported by in-situ Raman and density functional theory simulations.The prepared chronopotentiostatic superoxidation-activated Ni(CPS-Ni)electrodes exhibit an ultrahigh capacity of 3.21 mAh cm^(-2)at the current density of 5 mA cm^(-2),nearly 8 times that of traditional one-electron processes electrodes.Even under the ultrahigh 200 mA cm^(-2)current density,the CPS-Ni electrodes show 86.4%capacity retention with a Columbic efficiency of 99.2%after 10,000 cycles.The CPS-Ni||Zn microbattery achieves an exceptional energy density of 6.88 mWh cm^(-2)and power density of 339.56 mW cm^(-2).Device demonstration shows that the power source can continuously operate for more than 7 days in powering the sensing and computation intensive practical application of photoplethysmographic waveform monitoring.This work paves the way to the development of multi-electron transfer mechanisms for advanced aqueous Ni-Zn batteries with high capacity and long lifetime.展开更多
Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish...Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.展开更多
基金supported by InnoHK Project at Hong Kong Centre for Cerebro-cardiovascular Health Engineering (COCHE)City University of Hong Kong (7006108)。
文摘Aqueous Ni-Zn microbatteries are safe,reliable and inexpensive but notoriously suffer from inadequate energy and power densities.Herein,we present a novel mechanism of superoxide-activated Ni substrate that realizes the redox reaction featuring three-electron transfers(Ni↔Ni3+).The superoxide activates the direct redox reaction between Ni substrate and KNiO_(2)by lowering the reaction Gibbs free energy,supported by in-situ Raman and density functional theory simulations.The prepared chronopotentiostatic superoxidation-activated Ni(CPS-Ni)electrodes exhibit an ultrahigh capacity of 3.21 mAh cm^(-2)at the current density of 5 mA cm^(-2),nearly 8 times that of traditional one-electron processes electrodes.Even under the ultrahigh 200 mA cm^(-2)current density,the CPS-Ni electrodes show 86.4%capacity retention with a Columbic efficiency of 99.2%after 10,000 cycles.The CPS-Ni||Zn microbattery achieves an exceptional energy density of 6.88 mWh cm^(-2)and power density of 339.56 mW cm^(-2).Device demonstration shows that the power source can continuously operate for more than 7 days in powering the sensing and computation intensive practical application of photoplethysmographic waveform monitoring.This work paves the way to the development of multi-electron transfer mechanisms for advanced aqueous Ni-Zn batteries with high capacity and long lifetime.
基金financially supported by National Natural Science Foundation of China (22209133, 22272131, 21972111, 22211540712)Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX1411)+1 种基金Chongqing Engineering Research Center for Micro-Nano Biomedical Materials and DevicesChongqing Key Laboratory for Advanced Materials and Technologies。
文摘Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.
