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

doi:10.1002/anie.202112304

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 Publications › Journal Article (refereed) › peer-review

191 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 language	English
Article number	e202112304
Number of pages	9
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	6
Early online date	19 Nov 2021
DOIs	https://doi.org/10.1002/anie.202112304
Publication status	Published - 1 Feb 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Funding

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

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YANG, Q., LI, L., HUSSAIN, T., WANG, D., HUI, L., GUO, Y., LIANG, G., LI, X., CHEN, Z., HUANG, Z., LI, Y., XUE, Y., ZUO, Z., QIU, J., LI, Y., & ZHI, C. (2022). Stabilizing Interface pH by N-Modified Graphdiyne for Dendrite-Free and High-Rate Aqueous Zn-Ion Batteries. Angewandte Chemie - International Edition, 61(6), Article e202112304. https://doi.org/10.1002/anie.202112304

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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. ",

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

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AU - YANG, Qi

AU - LI, Liang

AU - HUSSAIN, Tanveer

AU - WANG, Donghong

AU - HUI, Lan

AU - GUO, Ying

AU - LIANG, Guojin

AU - LI, Xinliang

AU - CHEN, Ze

AU - HUANG, Zhaodong

AU - LI, Yongjun

AU - XUE, Yurui

AU - ZUO, Zicheng

AU - QIU, Jieshan

AU - LI, Yuliang

AU - ZHI, Chunyi

PY - 2022/2/1

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N2 - 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.

AB - 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.

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M3 - Journal Article (refereed)

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JO - Angewandte Chemie - International Edition

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

Abstract

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