Supercooled liquid sulfur maintained in three-dimensional current collector for high-performance Li-S batteries

Zhou, Guangmin; Yang, Ankun; Gao, Guoping; Yu, Xiaoyun; Xu, Jinwei; Liu, Chenwei; Ye, Yusheng; Pei, Allen; Wu, Yecun; Peng, Yucan; Li, Yanxi; Liang, Zheng; Liu, Kai; Wang, Lin-Wang; Cui, Yi

doi:10.1126/sciadv.aay5098

Title: Supercooled liquid sulfur maintained in three-dimensional current collector for high-performance Li-S batteries

Journal Article · Fri May 22 00:00:00 EDT 2020 · Science Advances

DOI:https://doi.org/10.1126/sciadv.aay5098· OSTI ID:1638191

^[1];

^[2];

^[3]; Yu, Xiaoyun ^[2]; Xu, Jinwei ^[2];

^[2];

^[2]; Li, Yanxi ^[2];

^[2]; Liu, Kai ^[2];

^[3];

^[4]

Stanford Univ., CA (United States); Tsinghua Univ., Shenzhen (China). Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Inst.
Stanford Univ., CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

In lithium-sulfur (Li-S) chemistry, the electrically/ionically insulating nature of sulfur and Li2S leads to sluggish electron/ion transfer kinetics for sulfur species conversion. Sulfur and Li2S are recognized as solid at room temperature, and solid-liquid phase transitions are the limiting steps in Li-S batteries. Here, we visualize the distinct sulfur growth behaviors on Al, carbon, Ni current collectors and demonstrate that (i) liquid sulfur generated on Ni provides higher reversible capacity, faster kinetics, and better cycling life compared to solid sulfur; and (ii) Ni facilitates the phase transition (e.g., Li2S decomposition). Accordingly, light-weight, 3D Ni-based current collector is designed to control the deposition and catalytic conversion of sulfur species toward high-performance Li-S batteries. This work provides insights on the critical role of the current collector in determining the physical state of sulfur and elucidates the correlation between sulfur state and battery performance, which will advance electrode designs in high-energy Li-S batteries.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Battery500 Consortium; Natural Key R&D Development Program of China; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515; 2019YFA0705700; AC02-05CH11231

OSTI ID:: 1638191

Alternate ID(s):: OSTI ID: 1695726

Journal Information:: Science Advances, Vol. 6, Issue 21; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 76 works

Citation information provided by
Web of Science

References (49)

Insights into Li-S Battery Cathode Capacity Fading Mechanisms: Irreversible Oxidation of Active Mass during Cycling Diao, Yan; Xie, Kai; Xiong, Shizhao Journal of The Electrochemical Society, Vol. 159, Issue 11 https://doi.org/10.1149/2.020211jes	journal	January 2012
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
A Lithium-Sulfur Battery using a 2D Current Collector Architecture with a Large-Sized Sulfur Host Operated under High Areal Loading and Low E/S Ratio Li, Matthew; Zhang, Yining; Bai, Zhengyu Advanced Materials, Vol. 30, Issue 46 https://doi.org/10.1002/adma.201804271	journal	October 2018
A graphene foam electrode with high sulfur loading for flexible and high energy Li-S batteries Zhou, Guangmin; Li, Lu; Ma, Chaoqun Nano Energy, Vol. 11 https://doi.org/10.1016/j.nanoen.2014.11.025	journal	January 2015
Interpretation of Raman spectra of disordered and amorphous carbon Ferrari, A. C.; Robertson, J. Physical Review B, Vol. 61, Issue 20, p. 14095-14107 https://doi.org/10.1103/PhysRevB.61.14095	journal	May 2000
Powering Lithium–Sulfur Battery Performance by Propelling Polysulfide Redox at Sulfiphilic Hosts Yuan, Zhe; Peng, Hong-Jie; Hou, Ting-Zheng Nano Letters, Vol. 16, Issue 1 https://doi.org/10.1021/acs.nanolett.5b04166	journal	December 2015
3D Carbonaceous Current Collectors: The Origin of Enhanced Cycling Stability for High-Sulfur-Loading Lithium-Sulfur Batteries Peng, Hong-Jie; Xu, Wen-Tao; Zhu, Lin Advanced Functional Materials, Vol. 26, Issue 35 https://doi.org/10.1002/adfm.201602071	journal	June 2016
Review of nanostructured current collectors in lithium–sulfur batteries Kong, Long; Peng, Hong-Jie; Huang, Jia-Qi Nano Research, Vol. 10, Issue 12 https://doi.org/10.1007/s12274-017-1652-x	journal	July 2017
Twinborn TiO ₂ –TiN heterostructures enabling smooth trapping–diffusion–conversion of polysulfides towards ultralong life lithium–sulfur batteries Zhou, Tianhong; Lv, Wei; Li, Jia Energy & Environmental Science, Vol. 10, Issue 7 https://doi.org/10.1039/C7EE01430A	journal	January 2017
Direct electrochemical generation of supercooled sulfur microdroplets well below their melting temperature Liu, Nian; Zhou, Guangmin; Yang, Ankun Proceedings of the National Academy of Sciences, Vol. 116, Issue 3 https://doi.org/10.1073/pnas.1817286116	journal	January 2019
Porous Hollow Carbon@Sulfur Composites for High-Power Lithium-Sulfur Batteries Jayaprakash, N.; Shen, J.; Moganty, Surya S. Angewandte Chemie International Edition, Vol. 50, Issue 26, p. 5904-5908 https://doi.org/10.1002/anie.201100637	journal	May 2011
Rechargeable Lithium–Sulfur Batteries Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng Chemical Reviews, Vol. 114, Issue 23 https://doi.org/10.1021/cr500062v	journal	July 2014
Electrochemical generation of liquid and solid sulfur on two-dimensional layered materials with distinct areal capacities Yang, Ankun; Zhou, Guangmin; Kong, Xian Nature Nanotechnology, Vol. 15, Issue 3 https://doi.org/10.1038/s41565-019-0624-6	journal	January 2020
Smaller Sulfur Molecules Promise Better Lithium–Sulfur Batteries Xin, Sen; Gu, Lin; Zhao, Na-Hong Journal of the American Chemical Society, Vol. 134, Issue 45 https://doi.org/10.1021/ja308170k	journal	October 2012
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
High-quality graphene via microwave reduction of solution-exfoliated graphene oxide Voiry, D.; Yang, J.; Kupferberg, J. Science, Vol. 353, Issue 6306 https://doi.org/10.1126/science.aah3398	journal	September 2016
Strongly Coupled Interfaces between a Heterogeneous Carbon Host and a Sulfur-Containing Guest for Highly Stable Lithium-Sulfur Batteries: Mechanistic Insight into Capacity Degradation Peng, Hong-Jie; Hou, Ting-Zheng; Zhang, Qiang Advanced Materials Interfaces, Vol. 1, Issue 7 https://doi.org/10.1002/admi.201400227	journal	July 2014
Design of Complex Nanomaterials for Energy Storage: Past Success and Future Opportunity Liu, Yayuan; Zhou, Guangmin; Liu, Kai Accounts of Chemical Research, Vol. 50, Issue 12 https://doi.org/10.1021/acs.accounts.7b00450	journal	December 2017
Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes Pang, Quan; Liang, Xiao; Kwok, Chun Yuen Nature Energy, Vol. 1, Issue 9 https://doi.org/10.1038/nenergy.2016.132	journal	September 2016
Two-dimensional layered transition metal disulphides for effective encapsulation of high-capacity lithium sulphide cathodes Seh, Zhi Wei; Yu, Jung Ho; Li, Weiyang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6017	journal	September 2014
Design Hierarchical Electrodes with Highly Conductive NiCo ₂ S ₄ Nanotube Arrays Grown on Carbon Fiber Paper for High-Performance Pseudocapacitors Xiao, Junwu; Wan, Lian; Yang, Shihe Nano Letters, Vol. 14, Issue 2 https://doi.org/10.1021/nl404199v	journal	January 2014
Amphiphilic Surface Modification of Hollow Carbon Nanofibers for Improved Cycle Life of Lithium Sulfur Batteries Zheng, Guangyuan; Zhang, Qianfan; Cha, Judy J. Nano Letters, Vol. 13, Issue 3, p. 1265-1270 https://doi.org/10.1021/nl304795g	journal	February 2013
Single Atom (Pd/Pt) Supported on Graphitic Carbon Nitride as an Efficient Photocatalyst for Visible-Light Reduction of Carbon Dioxide Gao, Guoping; Jiao, Yan; Waclawik, Eric R. Journal of the American Chemical Society, Vol. 138, Issue 19 https://doi.org/10.1021/jacs.6b02692	journal	May 2016
Electrocatalytic Polysulfide Traps for Controlling Redox Shuttle Process of Li–S Batteries Al Salem, Hesham; Babu, Ganguli; V. Rao, Chitturi Journal of the American Chemical Society, Vol. 137, Issue 36 https://doi.org/10.1021/jacs.5b04472	journal	September 2015
On the Surface Chemical Aspects of Very High Energy Density, Rechargeable Li–Sulfur Batteries Aurbach, Doron; Pollak, Elad; Elazari, Ran Journal of The Electrochemical Society, Vol. 156, Issue 8, p. A694-A702 https://doi.org/10.1149/1.3148721	journal	January 2009
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
An Aqueous Inorganic Polymer Binder for High Performance Lithium–Sulfur Batteries with Flame-Retardant Properties Zhou, Guangmin; Liu, Kai; Fan, Yanchen ACS Central Science, Vol. 4, Issue 2 https://doi.org/10.1021/acscentsci.7b00569	journal	February 2018
Electrochemical reaction of sulfur cathodes with Ni foam current collector in Li-S batteries Liu, Li-Jun; Chen, Yang; Zhang, Zhi-Feng Journal of Power Sources, Vol. 325 https://doi.org/10.1016/j.jpowsour.2016.06.002	journal	September 2016
Electrocatalysis of Lithium Polysulfides: Current Collectors as Electrodes in Li/S Battery Configuration Babu, Ganguli; Ababtain, Khalid; Ng, K. Y. Simon Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep08763	journal	March 2015
Balancing surface adsorption and diffusion of lithium-polysulfides on nonconductive oxides for lithium–sulfur battery design Tao, Xinyong; Wang, Jianguo; Liu, Chong Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11203	journal	April 2016
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer Su, Yu-Sheng; Manthiram, Arumugam Nature Communications, Vol. 3, Article No. 1166 https://doi.org/10.1038/ncomms2163	journal	January 2012
Enhancing lithium–sulphur battery performance by strongly binding the discharge products on amino-functionalized reduced graphene oxide Wang, Zhiyu; Dong, Yanfeng; Li, Hongjiang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6002	journal	September 2014
Three-dimensional flexible and conductive interconnected graphene networks grown by chemical vapour deposition Chen, Zongping; Ren, Wencai; Gao, Libo Nature Materials, Vol. 10, Issue 6, p. 424-428 https://doi.org/10.1038/nmat3001	journal	April 2011
Catalytic Effects in Lithium-Sulfur Batteries: Promoted Sulfur Transformation and Reduced Shuttle Effect Liu, Donghai; Zhang, Chen; Zhou, Guangmin Advanced Science, Vol. 5, Issue 1 https://doi.org/10.1002/advs.201700270	journal	September 2017
A Graphene-Pure-Sulfur Sandwich Structure for Ultrafast, Long-Life Lithium-Sulfur Batteries Zhou, Guangmin; Pei, Songfeng; Li, Lu Advanced Materials, Vol. 26, Issue 4 https://doi.org/10.1002/adma.201302877	journal	November 2013
High-Capacity Micrometer-Sized Li₂ S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries Yang, Yuan; Zheng, Guangyuan; Misra, Sumohan Journal of the American Chemical Society, Vol. 134, Issue 37, p. 15387-15394 https://doi.org/10.1021/ja3052206	journal	September 2012
Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Efficient Activation of Li ₂ S by Transition Metal Phosphides Nanoparticles for Highly Stable Lithium–Sulfur Batteries Yuan, Huadong; Chen, Xianlang; Zhou, Guangmin ACS Energy Letters, Vol. 2, Issue 7 https://doi.org/10.1021/acsenergylett.7b00465	journal	June 2017
Catalytic oxidation of Li ₂ S on the surface of metal sulfides for Li−S batteries Zhou, Guangmin; Tian, Hongzhen; Jin, Yang Proceedings of the National Academy of Sciences, Vol. 114, Issue 5 https://doi.org/10.1073/pnas.1615837114	journal	January 2017
Sulfur Nanodots Stitched in 2D “Bubble-Like” Interconnected Carbon Fabric as Reversibility-Enhanced Cathodes for Lithium–Sulfur Batteries Wu, Feng; Ye, Yu-Sheng; Huang, Jia-Qi ACS Nano, Vol. 11, Issue 5 https://doi.org/10.1021/acsnano.7b00596	journal	April 2017
Li–O₂ and Li–S batteries with high energy storage Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J. Nature Materials, Vol. 11, Issue 1, p. 19-29 https://doi.org/10.1038/nmat3191	journal	January 2012
Multi-functional separator/interlayer system for high-stable lithium-sulfur batteries: Progress and prospects Huang, Jia-Qi; Zhang, Qiang; Wei, Fei Energy Storage Materials, Vol. 1 https://doi.org/10.1016/j.ensm.2015.09.008	journal	November 2015
A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries Ji, Xiulei; Lee, Kyu Tae; Nazar, Linda F. Nature Materials, Vol. 8, Issue 6, p. 500-506 https://doi.org/10.1038/nmat2460	journal	May 2009
A Foldable Lithium–Sulfur Battery Li, Lu; Wu, Zi Ping; Sun, Hao ACS Nano, Vol. 9, Issue 11 https://doi.org/10.1021/acsnano.5b05068	journal	October 2015
Understanding the Role of Different Conductive Polymers in Improving the Nanostructured Sulfur Cathode Performance Li, Weiyang; Zhang, Qianfan; Zheng, Guangyuan Nano Letters, Vol. 13, Issue 11 https://doi.org/10.1021/nl403130h	journal	October 2013
The use of elemental sulfur as an alternative feedstock for polymeric materials Chung, Woo Jin; Griebel, Jared J.; Kim, Eui Tae Nature Chemistry, Vol. 5, Issue 6 https://doi.org/10.1038/nchem.1624	journal	April 2013
Lithium–sulfur batteries with superior cycle stability by employing porous current collectors Chung, Sheng-Heng; Manthiram, Arumugam Electrochimica Acta, Vol. 107 https://doi.org/10.1016/j.electacta.2013.06.034	journal	September 2013
A flexible nanostructured sulphur–carbon nanotube cathode with high rate performance for Li-S batteries Zhou, Guangmin; Wang, Da-Wei; Li, Feng Energy & Environmental Science, Vol. 5, Issue 10 https://doi.org/10.1039/c2ee22294a	journal	January 2012