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Title: Scalable Synthesis of Defect Abundant Si Nanorods for High-Performance Li-Ion Battery Anodes

Abstract

Microsized nanostructured silicon–carbon composite is a promising anode material for high energy Li-ion batteries. However, large-scale synthesis of high-performance nano-Si materials at a low cost still remains a significant challenge. Here we report a scalable low cost method to synthesize Al/Na-doped and defect-abundant Si nanorods that have excellent electrochemical performance with high first-cycle Coulombic efficiency (90%). The unique Si nanorods are synthesized by acid etching the refined and rapidly solidified eutectic Al–Si ingot. To maintain the high electronic conductivity, a thin layer of carbon is then coated on the Si nanorods by carbonization of self-polymerized polydopamine (PDA) at 800 °C. The carbon coated Si nanorods (Si@C) electrode at 0.9 mg cm–2 loading (corresponding to area-specific-capacity of ~2.0 mAh cm–2) exhibits a reversible capacity of ~2200 mAh g–1 at 100 mA g–1 current, and maintains ~700 mAh g–1 over 1000 cycles at 1000 mA g–1 with a capacity decay rate of 0.02% per cycle. High Coulombic efficiencies of 87% in the first cycle and ~99.7% after 5 cycles are achieved due to the formation of an artificial Al2O3 solid electrolyte interphase (SEI) on the Si surface, and the low surface area (31 m2 g–1), which has never been reported before formore » nano-Si anodes. The excellent electrochemical performance results from the massive defects (twins, stacking faults, dislocations) and Al/Na doping in Si nanorods induced by rapid solidification and Na salt modifications; this greatly enhances the robustness of Si from the volume changes and alleviates the mechanical stress/strain of the Si nanorods during the lithium insertion/extraction process. Introducing massive defects and Al/Na doping in eutectic Si nanorods for Li-ion battery anodes is unexplored territory. We venture this uncharted territory to commercialize this nanostructured Si anode for the next generation of Li-ion batteries.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [2]
  1. Jiamusi Univ. (China). School of Materials Science and Engineering
  2. Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1386081
Grant/Contract Number:  
SC0001160; 31100687
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 9; Journal Issue: 6; Related Information: NEES partners with University of Maryland (lead); University of California, Irvine; University of Florida; Los Alamos National Laboratory; Sandia National Laboratories; Yale University; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium-ion battery; silicon anode; eutectic Al−Si ingot; PDA self-polymerization; Bio-inspired; Energy storage (including batteries and capacitors); Defects; Charge transport; Synthesis (novel materials); Synthesis (self-assembly); Synthesis (scalable processing)

Citation Formats

Wang, Jing, Meng, Xiangcai, Fan, Xiulin, Zhang, Wenbo, Zhang, Hongyong, and Wang, Chunsheng. Scalable Synthesis of Defect Abundant Si Nanorods for High-Performance Li-Ion Battery Anodes. United States: N. p., 2015. Web. doi:10.1021/acsnano.5b02565.
Wang, Jing, Meng, Xiangcai, Fan, Xiulin, Zhang, Wenbo, Zhang, Hongyong, & Wang, Chunsheng. Scalable Synthesis of Defect Abundant Si Nanorods for High-Performance Li-Ion Battery Anodes. United States. https://doi.org/10.1021/acsnano.5b02565
Wang, Jing, Meng, Xiangcai, Fan, Xiulin, Zhang, Wenbo, Zhang, Hongyong, and Wang, Chunsheng. Tue . "Scalable Synthesis of Defect Abundant Si Nanorods for High-Performance Li-Ion Battery Anodes". United States. https://doi.org/10.1021/acsnano.5b02565. https://www.osti.gov/servlets/purl/1386081.
@article{osti_1386081,
title = {Scalable Synthesis of Defect Abundant Si Nanorods for High-Performance Li-Ion Battery Anodes},
author = {Wang, Jing and Meng, Xiangcai and Fan, Xiulin and Zhang, Wenbo and Zhang, Hongyong and Wang, Chunsheng},
abstractNote = {Microsized nanostructured silicon–carbon composite is a promising anode material for high energy Li-ion batteries. However, large-scale synthesis of high-performance nano-Si materials at a low cost still remains a significant challenge. Here we report a scalable low cost method to synthesize Al/Na-doped and defect-abundant Si nanorods that have excellent electrochemical performance with high first-cycle Coulombic efficiency (90%). The unique Si nanorods are synthesized by acid etching the refined and rapidly solidified eutectic Al–Si ingot. To maintain the high electronic conductivity, a thin layer of carbon is then coated on the Si nanorods by carbonization of self-polymerized polydopamine (PDA) at 800 °C. The carbon coated Si nanorods (Si@C) electrode at 0.9 mg cm–2 loading (corresponding to area-specific-capacity of ~2.0 mAh cm–2) exhibits a reversible capacity of ~2200 mAh g–1 at 100 mA g–1 current, and maintains ~700 mAh g–1 over 1000 cycles at 1000 mA g–1 with a capacity decay rate of 0.02% per cycle. High Coulombic efficiencies of 87% in the first cycle and ~99.7% after 5 cycles are achieved due to the formation of an artificial Al2O3 solid electrolyte interphase (SEI) on the Si surface, and the low surface area (31 m2 g–1), which has never been reported before for nano-Si anodes. The excellent electrochemical performance results from the massive defects (twins, stacking faults, dislocations) and Al/Na doping in Si nanorods induced by rapid solidification and Na salt modifications; this greatly enhances the robustness of Si from the volume changes and alleviates the mechanical stress/strain of the Si nanorods during the lithium insertion/extraction process. Introducing massive defects and Al/Na doping in eutectic Si nanorods for Li-ion battery anodes is unexplored territory. We venture this uncharted territory to commercialize this nanostructured Si anode for the next generation of Li-ion batteries.},
doi = {10.1021/acsnano.5b02565},
journal = {ACS Nano},
number = 6,
volume = 9,
place = {United States},
year = {2015},
month = {5}
}

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