Self-healing SEI enables full-cell cycling of a silicon-majority anode with a coulombic efficiency exceeding 99.9%

Jin, Yang; Li, Sa; Kushima, Akihiro; Zheng, Xiaoquan; Sun, Yongming; Xie, Jin; Sun, Jie; Xue, Weijiang; Zhou, Guangmin; Wu, Jiang; Shi, Feifei; Zhang, Rufan; Zhu, Zhi; So, Kangpyo; Cui, Yi; Li, Ju

doi:10.1039/c6ee02685k

Title: Self-healing SEI enables full-cell cycling of a silicon-majority anode with a coulombic efficiency exceeding 99.9%

Journal Article · 06 January 2017 · Energy & Environmental Science

DOI: https://doi.org/10.1039/c6ee02685k · OSTI ID:1353104

Jin, Yang ^[1]; Li, Sa ^[2]; Kushima, Akihiro ^[3]; Zheng, Xiaoquan ^[4]; Sun, Yongming ^[5]; Xie, Jin ^[5]; Sun, Jie ^[5]; Xue, Weijiang ^[3]; Zhou, Guangmin ^[5]; Wu, Jiang ^[4]; Shi, Feifei ^[5]; Zhang, Rufan ^[5]; Zhu, Zhi ^[3]; So, Kangpyo ^[3]; Cui, Yi ^[6];

^[7]

Xi'an Jiaotong Univ., Xi'an (China). State Key Lab. of Electrical Insulation and Power Equipment, School of Electrical Engineering; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering and Dept. of Materials Science and Engineering; Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
Tongji Univ., Shanghai (China). School of Materials Science and Engineering
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering and Dept. of Materials Science and Engineering
Xi'an Jiaotong Univ., Xi'an (China). State Key Lab. of Electrical Insulation and Power Equipment, School of Electrical Engineering
Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering and Dept. of Materials Science and Engineering; Tongji Univ., Shanghai (China). School of Materials Science and Engineering

Despite active developments, full-cell cycling of Li-battery anodes with >50 wt% Si (a Si-majority anode, SiMA) is rare. The main challenge lies in the solid electrolyte interphase (SEI), which when formed naturally (nSEI), is fragile and cannot tolerate the large volume changes of Si during lithiation/delithiation. An artificial SEI (aSEI) with a specific set of mechanical characteristics is henceforth designed; we enclose Si within a TiO₂ shell thinner than 15 nm, which may or may not be completely hermetic at the beginning. In situ TEM experiments show that the TiO₂ shell exhibits 5× greater strength than an amorphous carbon shell. Void-padded compartmentalization of Si can survive the huge volume changes and electrolyte ingression, with a self-healing aSEI + nSEI. The half-cell capacity exceeds 990 mA h g^-1 after 1500 cycles. To improve the volumetric capacity, we further compress SiMA 3-fold from its tap density (0.4 g cm^-3) to 1.4 g cm^-3, and then run the full-cell battery tests against a 3 mA h cm^-2 LiCoO₂ cathode. Despite some TiO₂ enclosures being inevitably broken, 2× the volumetric capacity (1100 mA h cm^-3) and 2× the gravimetric capacity (762 mA h g^-1) of commercial graphite anode is achieved in stable full-cell battery cycling, with a stabilized areal capacity of 1.6 mA h cm^-2 at the 100th cycle. The initial lithium loss, characterized by the coulombic inefficiency (CI), is carefully tallied on a logarithmic scale and compared with the actual full-cell capacity loss. In conclusion, it is shown that a strong, non-adherent aSEI, even if partially cracked, facilitates an adaptive self-repair mechanism that enables full-cell cycling of a SiMA, leading to a stabilized coulombic efficiency exceeding 99.9%.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1353104

Journal Information:: Energy & Environmental Science, Vol. 10, Issue 2; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 390 works

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Dimethylacrylamide, a novel electrolyte additive, can improve the electrochemical performances of silicon anodes in lithium-ion batteries Zhu, Guobin; Yang, Siming; Wang, Yan RSC Advances, Vol. 9, Issue 1 https://doi.org/10.1039/c8ra07988a	journal	January 2019
A high-tap-density nanosphere-assembled microcluster to simultaneously enable high gravimetric, areal and volumetric capacities: a case study of TiO ₂ anode Chang, Baisong; Liu, Jinping; Qing, Guangyan Journal of Materials Chemistry A, Vol. 6, Issue 25 https://doi.org/10.1039/c8ta02554a	journal	January 2018
Reduced expansion and improved full-cell cycling of a SnO _x #C embedded structure for lithium-ion batteries Yang, Lie; Sun, Liu-Yang; Zhang, Rong-Rong Journal of Materials Chemistry A, Vol. 6, Issue 32 https://doi.org/10.1039/c8ta04822c	journal	January 2018
Facile synthesis of N,O-codoped hard carbon on the kilogram scale for fast capacitive sodium storage Huang, Man; Xi, Baojuan; Feng, Zhenyu Journal of Materials Chemistry A, Vol. 6, Issue 34 https://doi.org/10.1039/c8ta06160b	journal	January 2018
Chemomechanical behaviors of layered cathode materials in alkali metal ion batteries Xu, Zhengrui; Rahman, Muhammad Mominur; Mu, Linqin Journal of Materials Chemistry A, Vol. 6, Issue 44 https://doi.org/10.1039/c8ta06875e	journal	January 2018
Porous Si@C ball-in-ball hollow spheres for lithium-ion capacitors with improved energy and power densities Li, Bo; Li, Shixiong; Jin, Ying Journal of Materials Chemistry A, Vol. 6, Issue 42 https://doi.org/10.1039/c8ta07576j	journal	January 2018
A new family of cation-disordered Zn(Cu)–Si–P compounds as high-performance anodes for next-generation Li-ion batteries Li, Wenwu; Li, Xinwei; Liao, Jun Energy & Environmental Science, Vol. 12, Issue 7 https://doi.org/10.1039/c9ee00953a	journal	January 2019
High-performance sodium-ion batteries with a hard carbon anode: transition from the half-cell to full-cell perspective Chen, Xinlong; Zheng, Yuheng; Liu, Wenjian Nanoscale, Vol. 11, Issue 46 https://doi.org/10.1039/c9nr07545c	journal	January 2019
Towards high energy density lithium battery anodes: silicon and lithium Zhu, Bin; Wang, Xinyu; Yao, Pengcheng Chemical Science, Vol. 10, Issue 30 https://doi.org/10.1039/c9sc01201j	journal	January 2019
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries Suo, Liumin; Xue, Weijiang; Gobet, Mallory Proceedings of the National Academy of Sciences, Vol. 115, Issue 6 https://doi.org/10.1073/pnas.1712895115	journal	January 2018
Highlighting the Importance of Full-Cell Testing for High Performance Anode Materials Comprising Li Alloying Nanowires Geaney, Hugh; Bree, Gerard; Stokes, Killian Journal of The Electrochemical Society, Vol. 166, Issue 13 https://doi.org/10.1149/2.0291913jes	journal	January 2019
Enhanced Capacity and Rate Capability of Nitrogen/Oxygen Dual-Doped Hard Carbon in Capacitive Potassium-Ion Storage Yang, Jinlin; Ju, Zhicheng; Jiang, Yong Advanced Materials, Vol. 30, Issue 4 https://doi.org/10.1002/adma.201700104	journal	December 2017
One‐Step Construction of N,P‐Codoped Porous Carbon Sheets/CoP Hybrids with Enhanced Lithium and Potassium Storage Bai, Jing; Xi, Baojuan; Mao, Hongzhi Advanced Materials, Vol. 30, Issue 35 https://doi.org/10.1002/adma.201802310	journal	July 2018
Challenges and Recent Progress in the Development of Si Anodes for Lithium-Ion Battery Jin, Yan; Zhu, Bin; Lu, Zhenda Advanced Energy Materials, Vol. 7, Issue 23 https://doi.org/10.1002/aenm.201700715	journal	September 2017
Evolving affinity between Coulombic reversibility and hysteretic phase transformations in nano-structured silicon-based lithium-ion batteries Ogata, K.; Jeon, S.; Ko, D. -S. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-02824-w	journal	February 2018
Phase boundary-enhanced Ni ₃ N–Co ₃ N@CNT composite materials for lithium-ion batteries Zhou, Han; Li, Zhaoyang; Wang, Ke Journal of Materials Chemistry A, Vol. 7, Issue 4 https://doi.org/10.1039/c8ta10604e	journal	January 2019
Carbon-based materials for lithium-ion capacitors Wang, Xiaojun; Liu, Lili; Niu, Zhiqiang Materials Chemistry Frontiers, Vol. 3, Issue 7 https://doi.org/10.1039/c9qm00062c	journal	January 2019
Designing superior solid electrolyte interfaces on silicon anodes for high-performance lithium-ion batteries Zhang, Yaguang; Du, Ning; Yang, Deren Nanoscale, Vol. 11, Issue 41 https://doi.org/10.1039/c9nr05748j	journal	January 2019

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