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.
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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. | ||||||||||||||||||
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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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