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Single-Phase Ternary Compounds with a disordered lattice and Liquid Metal Phase for High-Performance Li-Ion Battery Anodes

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Nano-Micro Letters 2023年第5期15卷 36-50页

作者： Yanhong Li Lei Zhang Hung-Yu Yen Yucun Zhou Gun Jang Songliu Yuan Jeng-Han Wang Peixun Xiong Meilin Liu Ho Seok Park Wenwu Li School of Chemical Engineering Sungkyunkwan University2066Seobu-roJangan-guSuwon-SiGyeonggi-Do 440-746Korea School of Physics Huazhong University of Science and TechnologyWuhan 430074People’s Republic of China School of Materials Science and Engineering Georgia Institute of TechnologyAtlantaGA 30332USA Department of Chemistry National Taiwan Normal UniversityTaipei 11677TaiwanPeople’s Republic of China Samsung Advanced Institute for Health Sciences and Technology(SAIHST) Sungkyunkwan University2066 SeoburoJangan-guSuwon 440-746Korea SKKU Advanced Institute of Nano Technology(SAINT) Sungkyunkwan University2066 SeoburoJangan-guSuwon 440-746Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan University2066 SeoburoJangan-guSuwon 440-746Korea

Si is considered as the promising anode materials for lithium-ion batteries(LIBs)owing to their high capacities of 4200 mAh g-1and natural ***,severe electrode pulverization and poor electronic and Li-ionic conductivities hinder their practical *** resolve the afore-mentioned problems,we first demonstrate a cation-mixed disordered lattice and unique Li storage mechanism of single-phase ternary GaSiP_(2)compound,where the liquid metallic Ga and highly reactive P are incorporated into Si through a ball milling *** confirmed by experimental and theoretical analyses,the introduced Ga and P enables to achieve the stronger resistance against volume variation and metallic conductivity,respectively,while the cation-mixed lattice provides the faster Li-ionic diffusion capability than those of the parent GaP and Si *** resulting GaSiP_(2)electrodes delivered the high specific capacity of 1615 mAh g-1and high initial Coulombic efficiency of 91%,while the graphite-modified GaSiP_(2)(GaSiP_(2)@C)achieved 83%of capacity retention after 900 cycles and high-rate capacity of 800 at 10,000 mA ***,the LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)//Ga SiP_(2)@C full cells achieved the high specific capacity of 1049 mAh g-1after 100 cycles,paving a way for the rational design of high-performance LIB anode materials.

关键词： Multinary compounds Liquid metal GaSiP_(2) disordered lattice Li-ion batteries

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A class of Ga-Al-P-based compounds with disordered lattice as advanced anode materials for Li-ion batteries

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Journal of Energy Chemistry 2023年第4期79卷 12-21页

作者： Yanhong Li Peixun Xiong Lei Zhang Songliu Yuan Wenwu Li School of Physics Huazhong University of Science and TechnologyWuhan 430074HubeiChina School of Chemical Engineering Sungkyunkwan University2066Seobu-roJangan-guSuwon 440-746Republic of Korea School of Materials Science&Engineering Georgia Institute of TechnologyAtlantaGA 30332USA

Phosphides possess large reversible capacity, small voltage hysteresis, and high energy efficiency, thus promising to be new anode candidates to replace commercial graphite for Li-ion batteries(LIBs).Through a facile mechanochemistry method, we prepare a novel ternary phosphide of Ga0.5Al0.5P whose crystalline structure is determined to be a cation-disordered cubic zinc sulfide structure according to XRD refinement. As an anode for LIBs, the Ga0.5Al0.5P delivers a reversible capacity of 1,352 mA h g^(-1)at100 mA g^(-1)with an initial Coulombic efficiency(ICE) up to 90.0% based on a reversible Li-storage mechanism integrating intercalation and subsequent conversion processes as confirmed by various characterizations techniques including in-situ XRD, ex-situ Raman, and XPS and electrochemical ***-modified Ga0.5Al0.5P exhibits a long-lasting cycling stability of retaining 1,182 mA h g^(-1)after300 cycles at 100 m A g^(-1), and 625 mA h g^(-1)after 800 cycles at 2,000 mA g^(-1), and a high-rate performance of remaining 342 m A h g^(-1)at 20,000 mA g^(-1). The outstanding electrochemical performances can be attributed to enhanced reaction kinetics enabled by the capacitive behaviors and the faster Liion diffusion enabled by the cation-mixing. Importantly, by tuning the cationic ratio, we develop a novel series of cation-mixed compounds of Ga_(1/3)Al_(2/3)P, Ga_(1/4)Al_(3/4)P, Ga_(1/5)Al_(4/5)P, Ga_(2/3)Al_(1/3)P, Ga_(3/4)Al_(1/4)P, and Ga_(4/5)Al_(1/5)P, which demonstrate large capacity, high ICE, and suitable anode potentials. Broadly, these compounds with disordered lattices probably present novel physicochemical properties, and high electrochemical performances, thus providing a new perspective for new materials design.

关键词： Multinary phosphides disordered lattice Anode Li-ion batteries

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