Stabilizing Interface pH by N-Modified Graphdiyne for Dendrite-Free and High-Rate Aqueous Zn-Ion Batteries

Qi YANG, Liang LI, Tanveer HUSSAIN, Donghong WANG, Lan HUI, Ying GUO, Guojin LIANG, Xinliang LI, Ze CHEN, Zhaodong HUANG, Yongjun LI, Yurui XUE, Zicheng ZUO, Jieshan QIU*, Yuliang LI*, Chunyi ZHI*

*Corresponding author for this work

Research output: Journal PublicationsJournal Article (refereed)peer-review

158 Citations (Scopus)

Abstract

Zn dendrite issue was intensively studied via tuning zinc ion flux. pH change seriously influences dendrite formation, while its importance has not been revealed. Here, we construct a N-modification graphdiyne interface (NGI) to stabilize pH by mediating hydrated zinc ion desolvation. Operando pH detection reveals pH stabilization by NGI. This works with pores in NGI to achieve dendrite-free Zn deposition and an increased symmetric cell lifespan by 116 times. Experimental and theoretical results owe pH stabilization to desolvation with a reduced activation energy achieved by electron transfer from solvation sheath to N atom. The efficient desolvation ensures that electron directly transfers from substrate to Zn2+ (rather than the coordinated H2O), avoiding O−H bond splitting. Hence, Zn-V6O13 battery achieves a long lifespan at 20.65 mA cm−2 and 1.07 mAh cm−2. This work reveals the significance of interface pH and provides a new approach to address Zn dendrite issue.

Original languageEnglish
Article numbere202112304
Number of pages9
JournalAngewandte Chemie - International Edition
Volume61
Issue number6
Early online date19 Nov 2021
DOIs
Publication statusPublished - Feb 2022
Externally publishedYes

Bibliographical note

This research was supported by GRF Scheme under Project CityU 11305218.

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