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Deposition of Horizontally Stacked Zn Crystals on Single Layer 1T-VSe₂ for Dendrite-Free Zn Metal Anodes

Li, Yuyin and Wong, Hoilun and Wang, Jun and Peng, Weiliang and Shen, Yidi and Xu, Mengyang and An, Qi and Kim, Jang-Kyo and Yuan, Bin and Goddard, William A., III and Luo, Zhengtang (2022) Deposition of Horizontally Stacked Zn Crystals on Single Layer 1T-VSe₂ for Dendrite-Free Zn Metal Anodes. Advanced Energy Materials, 12 (47). p. 2202983. ISSN 1614-6832. doi:10.1002/aenm.202202983. https://resolver.caltech.edu/CaltechAUTHORS:20221110-430801400.17

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Abstract

Owing to the moderate redox potential and high safety, Zn metal anodes have been garnering great attention. However, the poor reversibility and limited-service period caused by side reactions and dendrites hinder their applications. Here, a novel anode material consisting of a hexagonal 1T-Vanadium diselenide (1T-VSe₂) film on graphene is developed as a zincophilic template to epitaxially electrodeposit hexagonal closest packed Zn to replace the conventional metal substrates in Zn batteries. The 1T-VSe₂/Zn anode induces a horizontally (002)-oriented plate-like Zn crystal deposition morphology instead of randomly oriented grains that prompts the compact Zn deposition. According to density functional theory calculations, the VSe₂ substrate exhibits a higher Zn adsorption (−0.54 eV) than the graphene (−0.38 eV) or neat Zn (−0.48 eV) counterparts, leading to the enhanced zincophilicity and a lower nucleation overpotential, in agreement with the experimental results. The force field-based molecular dynamics simulations visualize Zn nucleation and morphological evolution at the atomistic level. The rapid adatom diffusion on VSe₂ leads to layer-by-layer Zn electrodeposits with higher fraction of the (002) facets to effectively prohibit dendrite formation. The symmetric cell with 1T-VSe₂/Zn delivers an ultra-stable cyclic life of 2500 h with 50 mV overpotential at 1 mA cm⁻² and 1 mAh cm⁻².


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/aenm.202202983DOIArticle
ORCID:
AuthorORCID
Li, Yuyin0000-0002-3709-7606
Wong, Hoilun0000-0002-2343-849X
Xu, Mengyang0000-0002-9289-4384
An, Qi0000-0003-4838-6232
Goddard, William A., III0000-0003-0097-5716
Luo, Zhengtang0000-0002-5134-9240
Additional Information:Y.L. and H.W. contributed equally to this work. Z.L. acknowledges support by the RGC (16304421), the Innovation and Technology Commission (ITC-CNERC14SC01), Guangdong Science and Technology Department (Project#: 2020A0505090003), Research Fund of Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology (No. 2020B1212030010), IER foundation (HT-JD-CXY-201907), and Shenzhen Special Fund for Central Guiding the Local Science and Technology Development (2021Szvup136). Technical assistance from the Materials Characterization and Preparation Facilities of HKUST is greatly appreciated. W.A.G. acknowledges financial support by the US National Science Foundation (NSF CBET-2005250) and from the Hong Kong Quantum AI Lab Ltd. in the frame of the InnoHK initiative.
Funders:
Funding AgencyGrant Number
Innovation and Technology Commission (Hong Kong)ITC-CNERC14SC01
Guangdong Science and Technology Department2020A0505090003
Research Grants Council of Hong Kong16304421
Research Fund of Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology2020B1212030010
IER FoundationHT-JD-CXY-201907
Shenzhen Special Fund for Central Guiding the Local Science and Technology Development2021Szvup136
NSFCBET-2005250
InnoHK initiativeUNSPECIFIED
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1543
Issue or Number:47
DOI:10.1002/aenm.202202983
Record Number:CaltechAUTHORS:20221110-430801400.17
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20221110-430801400.17
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117831
Collection:CaltechAUTHORS
Deposited By: Donna Wrublewski
Deposited On:08 Dec 2022 17:54
Last Modified:17 Dec 2022 01:47

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