Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries

Barnes, Pete; Zuo, Yunxing; Dixon, Kiev; Hou, Dewen; Lee, Sungsik; Ma, Zhiyuan; Connell, Justin G.; Zhou, Hua; Deng, Changjian; Smith, Kassiopeia; Gabriel, Eric; Liu, Yuzi; Maryon, Olivia O.; Davis, Paul H.; Zhu, Haoyu; Du, Yingge; Qi, Ji; Zhu, Zhuoying; Chen, Chi; Zhu, Zihua; Zhou, Yadong; Simmonds, Paul J.; Briggs, Ariel E.; Schwartz, Darin; Ong, Shyue Ping; Xiong, Hui

doi:10.1038/s41563-022-01242-0

Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries

Journal Article · Mon May 02 00:00:00 EDT 2022 · Nature Materials

DOI:https://doi.org/10.1038/s41563-022-01242-0· OSTI ID:1901706

^[1]; Zuo, Yunxing ^[2]; Dixon, Kiev ^[3]; Hou, Dewen ^[4]; Lee, Sungsik ^[5]; Ma, Zhiyuan ^[5]; ^[5]; ^[5]; Deng, Changjian ^[3]; Smith, Kassiopeia ^[3]; Gabriel, Eric ^[3]; ^[6]; Maryon, Olivia O. ^[3]; ^[3]; Zhu, Haoyu ^[3]; ^[7]; Qi, Ji ^[2]; Zhu, Zhuoying ^[2]; ^[2]; ^[8] more »

Boise State Univ., ID (United States); Idaho National Lab. (INL), Idaho Falls, ID (United States)
Univ. of California, San Diego, La Jolla, CA (United States)
Boise State Univ., ID (United States)
Boise State Univ., ID (United States); Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
Argonne National Lab. (ANL), Lemont, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Boise State Univ., ID (United States); Center for Advanced Energy Studies, Idaho Falls, ID (United States)

Intercalation-type metal oxides are promising negative electrode materials for safe rechargeable lithium-ion batteries due to the reduced risk of Li plating at low voltages. Nevertheless, their lower energy and power density along with cycling instability remain bottlenecks for their implementation, especially for fast-charging applications. Here, we report a nanostructured rock-salt Nb₂O₅ electrode formed through an amorphous-to-crystalline transformation during repeated electrochemical cycling with Li⁺. This electrode can reversibly cycle three lithiums per Nb₂O₅, corresponding to a capacity of 269 mAh g^–1 at 20 mA g^–1, and retains a capacity of 191 mAh g^–1 at a high rate of 1 A g^–1. Further, it exhibits superb cycling stability with a capacity of 225 mAh g^–1 at 200 mA g^–1 for 400 cycles, and a Coulombic efficiency of 99.93%. We attribute the enhanced performance to the cubic rock-salt framework, which promotes low-energy migration paths. Our work suggests that inducing crystallization of amorphous nanomaterials through electrochemical cycling is a promising avenue for creating unconventional high-performance metal oxide electrode materials.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1901706

Alternate ID(s):: OSTI ID: 1970230

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 7 Vol. 21; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (56)

High-Performance Supercapacitors Based on Nanocomposites of Nb2O5 Nanocrystals and Carbon Nanotubes Wang, Xiaolei; Li, Ge; Chen, Zheng Advanced Energy Materials, Vol. 1, Issue 6 https://doi.org/10.1002/aenm.201100332	journal	October 2011
The Effect of Crystallinity on the Rapid Pseudocapacitive Response of Nb2O5 Kim, Jong Woung; Augustyn, Veronica; Dunn, Bruce Advanced Energy Materials, Vol. 2, Issue 1 https://doi.org/10.1002/aenm.201100494	journal	December 2011
Impact of the Specific Surface Area on the Memory Effect in Li-Ion Batteries: The Case of Anatase TiO ₂ Madej, Edyta; La Mantia, Fabio; Schuhmann, Wolfgang Advanced Energy Materials, Vol. 4, Issue 17 https://doi.org/10.1002/aenm.201400829	journal	July 2014
The Modifications of Niobium Pentoxide Schäfer, Harald; Gruehn, R.; Schulte, F. Angewandte Chemie International Edition in English, Vol. 5, Issue 1 https://doi.org/10.1002/anie.196600401	journal	January 1966
Formation of Highly Ordered Nanochannel Nb Oxide by Self-Organizing Anodization Lee, Kiyoung; Yang, Yang; Yang, Min Chemistry - A European Journal, Vol. 18, Issue 31 https://doi.org/10.1002/chem.201201426	journal	June 2012
Structure and morphology of niobium suboxides Monfort, Y.; Maisseu, A.; Allais, G. Physica Status Solidi (a), Vol. 15, Issue 1 https://doi.org/10.1002/pssa.2210150115	journal	January 1973
Die Oxyde des Niobs Brauer, Georg Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 248, Issue 1 https://doi.org/10.1002/zaac.19412480101	journal	September 1941
ESCA studies of some niobium compounds Bahl, M. K. Journal of Physics and Chemistry of Solids, Vol. 36, Issue 6 https://doi.org/10.1016/0022-3697(75)90132-8	journal	June 1975
X-ray photoelectron spectroscopy study of phosphorus incorporation in anodic oxide films on niobium Jouve, J.; Belkacem, Y.; Severac, C. Thin Solid Films, Vol. 139, Issue 1 https://doi.org/10.1016/0040-6090(86)90049-0	journal	May 1986
XPS study of tellurium—niobium and tellurium—tantalum oxide systems Garbassi, F.; Bart, J. C. J.; Petrini, G. Journal of Electron Spectroscopy and Related Phenomena, Vol. 22, Issue 2 https://doi.org/10.1016/0368-2048(81)80019-9	journal	January 1981
Electrochemistry of L-niobium pentoxide a lithium/non-aqueous cell Ohzuku, Tsutomu; Sawai, Keijiro; Hirai, Taketsugu Journal of Power Sources, Vol. 19, Issue 4 https://doi.org/10.1016/0378-7753(87)87005-2	journal	April 1987
Optical and electrochemical characteristics of niobium oxide films prepared by sol-gel process and magnetron sputtering A comparison Özer, Nilgün; Rubin, Michael D.; Lampert, Carl M. Solar Energy Materials and Solar Cells, Vol. 40, Issue 4 https://doi.org/10.1016/0927-0248(95)00147-6	journal	August 1996
The role and utilization of pseudocapacitance for energy storage by supercapacitors Conway, B. E.; Birss, V.; Wojtowicz, J. Journal of Power Sources, Vol. 66, Issue 1-2 https://doi.org/10.1016/S0378-7753(96)02474-3	journal	May 1997
Sol–gel niobium pentoxide: A promising material for electrochromic coatings, batteries, nanocrystalline solar cells and catalysis Aegerter, Michel A. Solar Energy Materials and Solar Cells, Vol. 68, Issue 3-4 https://doi.org/10.1016/S0927-0248(00)00372-X	journal	June 2001
Synthesis of single-crystal niobium pentoxide nanobelts Wei, Mingdeng; Qi, Zhi-mei; Ichihara, Masaki Acta Materialia, Vol. 56, Issue 11 https://doi.org/10.1016/j.actamat.2008.01.049	journal	June 2008
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav Computational Materials Science, Vol. 68 https://doi.org/10.1016/j.commatsci.2012.10.028	journal	February 2013
A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries Verma, Pallavi; Maire, Pascal; Novák, Petr Electrochimica Acta, Vol. 55, Issue 22, p. 6332-6341 https://doi.org/10.1016/j.electacta.2010.05.072	journal	September 2010
Understanding electrochemical potentials of cathode materials in rechargeable batteries Liu, Chaofeng; Neale, Zachary G.; Cao, Guozhong Materials Today, Vol. 19, Issue 2 https://doi.org/10.1016/j.mattod.2015.10.009	journal	March 2016
Nanostructured electrodes for high-power lithium ion batteries Mukherjee, Rahul; Krishnan, Rahul; Lu, Toh-Ming Nano Energy, Vol. 1, Issue 4 https://doi.org/10.1016/j.nanoen.2012.04.001	journal	July 2012
Lithium intercalation into transition metal oxides: A route to generate new ordered rock salt type structure Pralong, V. Progress in Solid State Chemistry, Vol. 37, Issue 4 https://doi.org/10.1016/j.progsolidstchem.2010.08.002	journal	December 2009
Electropolishing valve metals with a sulfuric acid-methanol electrolyte at low temperature Barnes, Pete; Savva, Andreas; Dixon, Kiev Surface and Coatings Technology, Vol. 347 https://doi.org/10.1016/j.surfcoat.2018.04.082	journal	August 2018
Annealing induced structural and phase transitions in anodic aluminum oxide prepared in oxalic acid electrolyte Roslyakov, I. V.; Kolesnik, I. V.; Levin, E. E. Surface and Coatings Technology, Vol. 381 https://doi.org/10.1016/j.surfcoat.2019.125159	journal	January 2020
Multielectron Redox and Insulator-to-Metal Transition upon Lithium Insertion in the Fast-Charging, Wadsley-Roth Phase PNb ₉ O ₂₅ Preefer, Molleigh B.; Saber, Muna; Wei, Qiulong Chemistry of Materials, Vol. 32, Issue 11 https://doi.org/10.1021/acs.chemmater.0c00560	journal	May 2020
Remarkable Enhancement of Photocatalytic Water Oxidation in N ₂ /Ar Plasma Treated, Mesoporous TiO ₂ Films Islam, Syed Z.; Reed, Allen; Wanninayake, Namal The Journal of Physical Chemistry C, Vol. 120, Issue 26 https://doi.org/10.1021/acs.jpcc.6b02622	journal	June 2016
Design and Preparation of Materials for Advanced Electrochemical Storage Melot, Brent C.; Tarascon, J. -M. Accounts of Chemical Research, Vol. 46, Issue 5 https://doi.org/10.1021/ar300088q	journal	June 2012
Niobium Compounds: Preparation, Characterization, and Application in Heterogeneous Catalysis Nowak, Izabela; Ziolek, Maria Chemical Reviews, Vol. 99, Issue 12 https://doi.org/10.1021/cr9800208	journal	December 1999
Pseudocapacitive Contributions to Charge Storage in Highly Ordered Mesoporous Group V Transition Metal Oxides with Iso-Oriented Layered Nanocrystalline Domains Brezesinski, Kirstin; Wang, John; Haetge, Jan Journal of the American Chemical Society, Vol. 132, Issue 20, p. 6982-6990 https://doi.org/10.1021/ja9106385	journal	May 2010
Dynamics of Lithium Insertion in Electrochromic Titanium Dioxide Nanocrystal Ensembles Dahlman, Clayton J.; Heo, Sungyeon; Zhang, Youtian Journal of the American Chemical Society, Vol. 143, Issue 22 https://doi.org/10.1021/jacs.0c10628	journal	May 2021
High-Rate Intercalation without Nanostructuring in Metastable Nb ₂ O ₅ Bronze Phases Griffith, Kent J.; Forse, Alexander C.; Griffin, John M. Journal of the American Chemical Society, Vol. 138, Issue 28 https://doi.org/10.1021/jacs.6b04345	journal	July 2016
Redox Cycling Driven Transformation of Layered Manganese Oxides to Tunnel Structures Jung, Haesung; Taillefert, Martial; Sun, Jingying Journal of the American Chemical Society, Vol. 142, Issue 5 https://doi.org/10.1021/jacs.9b12266	journal	January 2020
Pseudocapacitive Contributions to Electrochemical Energy Storage in TiO₂ (Anatase) Nanoparticles Wang, John; Polleux, Julien; Lim, James The Journal of Physical Chemistry C, Vol. 111, Issue 40, p. 14925-14931 https://doi.org/10.1021/jp074464w	journal	October 2007
Self-Improving Anode for Lithium-Ion Batteries Based on Amorphous to Cubic Phase Transition in TiO ₂ Nanotubes Xiong, Hui; Yildirim, Handan; Shevchenko, Elena V. The Journal of Physical Chemistry C, Vol. 116, Issue 4 https://doi.org/10.1021/jp210793u	journal	January 2012
Concentration-Dependent Ordering of Lithiated Amorphous TiO ₂ Yildirim, Handan; Greeley, Jeffrey P.; Sankaranarayanan, Subramanian K. R. S. The Journal of Physical Chemistry C, Vol. 117, Issue 8 https://doi.org/10.1021/jp312079r	journal	February 2013
Theoretical Study of Li Migration in Lithium–Graphite Intercalation Compounds with Dispersion-Corrected DFT Methods Thinius, Sascha; Islam, Mazharul M.; Heitjans, Paul The Journal of Physical Chemistry C, Vol. 118, Issue 5 https://doi.org/10.1021/jp408945j	journal	January 2014
Nanostructured Nb ₂ O ₅ Polymorphs by Electrospinning for Rechargeable Lithium Batteries Viet, A. Le; Reddy, M. V.; Jose, R. The Journal of Physical Chemistry C, Vol. 114, Issue 1 https://doi.org/10.1021/jp9088589	journal	November 2009
Electrochemical Impedance Spectroscopy of Porous TiO ₂ for Photocatalytic Applications Baram, Nir; Ein-Eli, Yair The Journal of Physical Chemistry C, Vol. 114, Issue 21 https://doi.org/10.1021/jp911687w	journal	May 2010
High-rate electrochemical energy storage through Li+ intercalation pseudocapacitance Augustyn, Veronica; Come, Jérémy; Lowe, Michael A. Nature Materials, Vol. 12, Issue 6 https://doi.org/10.1038/nmat3601	journal	April 2013
Memory effect in a lithium-ion battery Sasaki, Tsuyoshi; Ukyo, Yoshio; Novák, Petr Nature Materials, Vol. 12, Issue 6 https://doi.org/10.1038/nmat3623	journal	April 2013
Niobium tungsten oxides for high-rate lithium-ion energy storage Griffith, Kent J.; Wiaderek, Kamila M.; Cibin, Giannantonio Nature, Vol. 559, Issue 7715 https://doi.org/10.1038/s41586-018-0347-0	journal	July 2018
A disordered rock salt anode for fast-charging lithium-ion batteries Liu, Haodong; Zhu, Zhuoying; Yan, Qizhang Nature, Vol. 585, Issue 7823 https://doi.org/10.1038/s41586-020-2637-6	journal	September 2020
Effects of cycling on lithium-ion battery hysteresis and overvoltage Ovejas, V. J.; Cuadras, A. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-51474-5	journal	October 2019
Thin films and nanostructures of niobium pentoxide: fundamental properties, synthesis methods and applications Rani, Rozina Abdul; Zoolfakar, Ahmad Sabirin; O'Mullane, Anthony P. J. Mater. Chem. A, Vol. 2, Issue 38 https://doi.org/10.1039/C4TA02561J	journal	January 2014
Understanding memory effects in Li-ion batteries: evidence of a kinetic origin in TiO ₂ upon hydrogen annealing Ventosa, E.; Löffler, T.; La Mantia, F. Chemical Communications, Vol. 52, Issue 77 https://doi.org/10.1039/C6CC06070F	journal	January 2016
Recent advances in nanostructured Nb-based oxides for electrochemical energy storage Yan, Litao; Rui, Xianhong; Chen, Gen Nanoscale, Vol. 8, Issue 16 https://doi.org/10.1039/C6NR01340F	journal	January 2016
Defect generation in TiO ₂ nanotube anodes via heat treatment in various atmospheres for lithium-ion batteries Savva, Andreas I.; Smith, Kassiopeia A.; Lawson, Matthew Physical Chemistry Chemical Physics, Vol. 20, Issue 35 https://doi.org/10.1039/C8CP04368J	journal	January 2018
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
High-capacity electrode materials for rechargeable lithium batteries: Li ₃ NbO ₄ -based system with cation-disordered rocksalt structure Yabuuchi, Naoaki; Takeuchi, Mitsue; Nakayama, Masanobu Proceedings of the National Academy of Sciences, Vol. 112, Issue 25 https://doi.org/10.1073/pnas.1504901112	journal	June 2015
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
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
Ab initio study of lithium intercalation in metal oxides and metal dichalcogenides Aydinol, M. K.; Kohan, A. F.; Ceder, G. Physical Review B, Vol. 56, Issue 3 https://doi.org/10.1103/PhysRevB.56.1354	journal	July 1997
First-principles theory of ionic diffusion with nondilute carriers Van der Ven, A.; Ceder, G.; Asta, M. Physical Review B, Vol. 64, Issue 18 https://doi.org/10.1103/PhysRevB.64.184307	journal	October 2001
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
Algorithm for generating derivative structures Hart, Gus L. W.; Forcade, Rodney W. Physical Review B, Vol. 77, Issue 22 https://doi.org/10.1103/Physrevb.77.224115	journal	June 2008
Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries Lee, J.; Urban, A.; Li, X. Science, Vol. 343, Issue 6170 https://doi.org/10.1126/science.1246432	journal	January 2014
The Application of Nb2 O 5 as a Cathode in Nonaqueous Lithium Cells Reichman, Benjamin; Bard, Allen J. Journal of The Electrochemical Society, Vol. 128, Issue 2 https://doi.org/10.1149/1.2127416	journal	February 1981
EIS Characterization of the Barrier Layer Formed over Ti during its Potentiostatic Anodization in 0.1 M HClO₄/x mM HF (1 mM ≤x≤ 500 mM) Acevedo-Peña, Próspero; González, Ignacio Journal of The Electrochemical Society, Vol. 159, Issue 3 https://doi.org/10.1149/2.035203jes	journal	January 2012

Similar Records

Nanostructured lithium nickel manganese oxides for lithium-ion batteries.

Journal Article · Wed Feb 24 23:00:00 EST 2010 · J. Electrochem. Soc. · OSTI ID:992400

Construction of reduced graphene oxide supported molybdenum carbides composite electrode as high-performance anode materials for lithium ion batteries

Journal Article · Thu Jan 14 23:00:00 EST 2016 · Materials Research Bulletin · OSTI ID:22584281

Related Subjects

25 ENERGY STORAGE
Atomistic models
Batteries
Synthesis and processing

Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries

Citation Formats

References (56)

Similar Records

Related Subjects