Regulating the Interfacial Charge Density by Constructing a Novel Zn Anode‐Electrolyte Interface for Highly Reversible Zn Anode

Abstract

Aqueous zinc‐ion batteries (AZIBs) have attracted considerable attention. However, due to the uneven distribution of charge density at Zn anode|electrolyte interface, severe dendrites and corrosion are generated during cycling. In this work, a facile and scalable strategy to address the above‐mentioned issues has been proposed through regulating the charge density at Zn anode|electrolyte interface. As a proof of concept, amidinothiourea (ATU) with abundant lone‐pair electrons is employed as an interfacial charge modifier for Zn anode|electrolyte interface. The uniform and increased interfacial charge distribution on Zn anode|electrolyte interface has been obtained. Moreover, the unique Zn‐bond constructed between N atoms and Zn2+ as well as the hydrogen bonds are formed among ATU and Ac‐ anion/active H2O, which promote the migration and desolvation behavior of Zn2+ at anode|electrolyte interface. Accordingly, at a trace concentration of 0.01 mg mL‐1 ATU, these features endow Zn anode with a long cycling life (more than 800 h), and a high average Columbic efficiency (99.52%) for Zn||Cu batteries. When pairing with I2 cathode, the improved cycling ability (5000 cycles) with capacity retention of 77.9% is achieved. The fundamental understanding on the regulation of charge density at anode|electrolyte interface can facilitate the development of AZIBs.

Aqueous MnO2/Mn2+ electrochemistry in batteries: progress, challenges, and perspectives

“…20,24 In contrast, Zn anode exhibits low redox potential (−0.76 V vs. SHE), high specific capacity (820 mA h g −1 ), excellent reversibility and compatibility in aqueous electrolyte; thus, MnO 2 -based batteries with Zn as anode have been extensively developed and studied. 25,26 During the in-depth investigation of the reaction mechanism, the emerging MnO 2 dissolution/deposition chemistry was proposed and confirmed.…”

Rescuing zinc anode–electrolyte interface: mechanisms, theoretical simulations and in situ characterizations

“…55,149 Calculating and comparing the adsorption energy of zinc atoms on different crystal plane of ZMA helps identify the dominant zincophilic sites and provide reasons why additives can inhibit the growth of Zn dendrites. 44,50,150–153 Moreover, the charge density distribution and surface electrostatic potential intuitively reflect the strong interaction of Zn 2+ and precise active site for Zn 2+ nucleation, 49,154,155 respectively. As shown in Fig.…”

Artificial Hydrophilic Organic and Dendrite-Suppressed Inorganic Hybrid Solid Electrolyte Interface Layer for Highly Stable Zinc Anodes

“…Lithium-ion batteries (LIBs) are prevalent in green energy storage devices, such as portable devices and electric vehicles, due to their high energy density and good rechargeability. , However, lithium ore resources are scarce, and the inherent price is high. − Lithium-ion batteries use toxic and flammable organic electrolytes, which have potential safety hazards and are easy to cause environmental pollution, which seriously hinders their further application in the field of energy storage. − It is urgent to develop new batteries to replace lithium-ion batteries. − Aqueous zinc -ion batteries (AZIBs) are considered to be a reliable alternative to LIBs. It shows a high safety characteristic due to their use of aqueous electrolytes. − However, aqueous zinc-ion batteries have poor energy density and cycle life due to side reactions, such as dendrite growth, hydrogen evolution reaction (HER), and corrosion, as well as low zinc utilization (often referred to as depth of discharge, DOD) and undesired Coulombic efficiency (Scheme a). − Addressing these issues, particularly improving the reversibility of zinc metal, is crucial for enhancing the performance of aqueous zinc metal batteries. − …”