Dynamically Interfacial pH-Buffering Effect Enabled by N-Methylimidazole Molecules as Spontaneous Proton Pumps toward Highly Reversible Zinc-Metal Anodes

Bibliographische Detailangaben
Veröffentlicht in:	Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 15 vom: 10. Apr., Seite e2208630
1. Verfasser:	Zhang, Minghao (VerfasserIn)
Weitere Verfasser:	Hua, Haiming, Dai, Pengpeng, He, Zheng, Han, Lianhuan, Tang, Peiwen, Yang, Jin, Lin, Pengxiang, Zhang, Yufei, Zhan, Dongping, Chen, Jianken, Qiao, Yu, Li, Cheng Chao, Zhao, Jinbao, Yang, Yang
Format:	Online-Aufsatz
Sprache:	English
Veröffentlicht:	2023
Zugriff auf das übergeordnete Werk:	Advanced materials (Deerfield Beach, Fla.)
Schlagworte:	Journal Article EQCM and pH ultra-microelectrodes N-methylimidazole dissolution/deposition processes of MnO2 interfacial pH-buffering strategy proton pumps

Beschreibung
Zusammenfassung:	© 2023 Wiley-VCH GmbH. Aqueous zinc-metal batteries have attracted extensive attention due to their outstanding merits of high safety and low cost. However, the intrinsic thermodynamic instability of zinc in aqueous electrolyte inevitably results in hydrogen evolution, and the consequent generation of OH- at the interface will dramatically exacerbate the formation of dead zinc and dendrites. Herein, a dynamically interfacial pH-buffering strategy implemented by N-methylimidazole (NMI) additive is proposed to remove the detrimental OH- at zinc/electrolyte interface in real-time, thus eliminating the accumulation of by-products fundamentally. Electrochemical quartz crystal microbalance and molecular dynamics simulation results reveal the existence of an interfacial absorption layer assembled by NMI and protonated NMI (NMIH+ ), which acts as an ion pump for replenishing the interface with protons constantly. Moreover, an in situ interfacial pH detection method with micro-sized spatial resolution based on the ultra-microelectrode technology is developed to probe the pH evolution in diffusion layer, confirming the stabilized interfacial chemical environment in NMI-containing electrolyte. Accordingly, with the existence of NMI, an excellent cumulative plating capacity of 4.2 Ah cm-2 and ultrahigh Coulombic efficiency of 99.74% are realized for zinc electrodes. Meanwhile, the NMI/NMIH+ buffer additive can accelerate the dissolution/deposition process of MnO2 /Mn2+ on the cathode, leading to enhanced cycling capacity
Beschreibung:	Date Completed 13.04.2023 Date Revised 13.04.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE
ISSN:	1521-4095
DOI:	10.1002/adma.202208630