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

Barnes, Pete; Zuo, Yang; Dixon, Kiev; Hou, Dewen; Lee, Sungwon; 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, D. M.; Ong, Shyue Ping; Xiong, Hui

doi:10.1038/s41563-022-01242-0

Cited by 80 publications

(81 citation statements)

References 57 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The electronic interaction between the two can further be boosted via fast Nb 2 O 5 surface redox (Nb 4+ /Nb 5+ ), accompanied with O v creation and refilling. Specially, as a pseudocapacitive oxide, Nb 2 O 5 has been widely used in both supercapacitors and Li-ion batteries, with the Nb 4+ /Nb 5+ redox participating in the charging/discharging process. , However, the effect of the Nb redox on electrocatalysis in fuel cells has been left unexplored. Given that the Nb redox process comprises fast electron delivery and surface oxygen species refilling, we postulate that it might act as a reservoir for both electron and oxygen species, which might be helpful in addressing the stability issue of Pt during ORR.…”

Section: Resultsmentioning

confidence: 99%

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

et al. 2022

View full text Add to dashboard Cite

The limited durability of Pt-based catalysts has largely plagued the road of proton conductive membrane fuel cell-based vehicles to the mass market for years. Herein, we overcome the degradation issue by employing intelligent catalyst design to concomitantly suppress the oxidation and dissolution of Pt via introducing reducible niobium oxide (Nb2O5) support as a reservoir for electron and oxygen species. Benefiting from the corrosion resistance of Nb2O5 and strong metal–support interactions, the Pt–Nb2O5 catalyst exhibits negligible activity decay after 70k potential cycling between 0.6 and 1.0 V and maintains compelling stability even at higher voltages. In situ X-ray absorption fine structure and theoretical calculations have revealed that the reversible dynamic change of Nb4+/Nb5+ can inhibit the strongly bonded oxygenated species formation to attenuate Pt oxidation. Meanwhile, the Pt dissolution can be gratifyingly suppressed via the spillover of oxygenated intermediates from Pt to Nb2O5, accompanied with electron flowing from Nb2O5 to Pt. This work paves a way to develop intelligent catalysts to alleviate the degradation issue of Pt-based catalysts in a wide potential window.

show abstract

Section: Resultsmentioning

confidence: 99%

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

et al. 2022

View full text Add to dashboard Cite

show abstract

“…These observations are consistent with the fact that the DRX is synthesized under the application of an external driving force, such as high temperatures, ball milling, or electrochemical lithiation. 5,6,40 Lithium Intercalation Mechanism and Predicted Voltage Profile. The mechanism of intercalation of Li + into DRX structures is strongly affected by the distribution of the tetrahedral sites with different local environments and connectivity.…”

Section: Validation Of the Cluster Expansion Modelmentioning

confidence: 99%

Intercalation Chemistry of the Disordered Rocksalt Li₃V₂O₅ Anode from Cluster Expansions and Machine Learning Interatomic Potentials

2023

Self Cite

View full text Add to dashboard Cite

Disordered rocksalt (DRX) Li 3 V 2 O 5 is a promising anode candidate for rechargeable lithium-ion batteries because of its low voltage, high rate capability, and good cycling stability. Herein, we present a comprehensive study of the intercalation chemistry of the DRX-Li 3 V 2 O 5 anode using density functional theory (DFT) calculations combined with machine learning cluster expansions and interatomic potentials. The predicted voltage profile of the DRX Li 3 V 2 O 5 anode at room temperature based on Monte Carlo simulations with a fitted cluster expansion model is in good agreement with experiments. In contrast to previous DFT results, we find that Li ions predominately intercalate into tetrahedral sites during charging, while a majority of Li and V ions at octahedral sites remain stable. In addition, molecular dynamics simulations with a fitted moment tensor potential attribute the fast-charging capability of DRX-Li 3 V 2 O 5 to the facile diffusivity of Li + via a tetrahedral−octahedral−tetrahedral pathway. We further suggest tuning the Li:V ratio as a means of trading off increased lithiation capacity and decreased anode voltage in this system. This work provides in-depth insights into the high-performance DRX-Li 3 V 2 O 5 anode and paves the way for the discovery of other disordered anode materials.

show abstract

“…They are usually subjected to structure collapse and lithium dendrites when being charged at a high current density, resulting in sharp capacity decay and battery short circuit. Transition metal oxides have been proven to be potential fast-charging electrode materials for LIBs. − Among them, titania (TiO 2 ) is one of the most promising candidates because of its remarkable advantages. − First, TiO 2 is an environmentally benign, low-cost, and highly abundant material that is easy to prepare. Second, TiO 2 materials have a higher operating voltage than graphite, avoiding the formation of lithium dendrites.…”

Section: Introductionmentioning

confidence: 99%

In Situ Conformal Carbon Coating for Constructing Hierarchical Mesoporous Titania/Carbon Spheres as High-Rate Lithium-Ion Battery Anodes

Zhu

Feng

Xue

et al. 2022

ACS Sustainable Chem. Eng.

View full text Add to dashboard Cite

It is of vital importance to improve the transport of electrons and lithium ions at the same time for optimizing the rate capability of lithium-ion battery anode materials. In this work, hierarchical mesoporous titania/carbon (TiO 2 /C) spheres are fabricated via a soft method and followed by the in situ carbonation of the residual nhexadecylamine structure-directing agent. This green synthetic method ingeniously makes the waste organic species turn into coaxially conductive carbon layers but does not compromise the high porosity of TiO 2 . The hierarchical mesoporous TiO 2 /C spheres not only effectively improve the electrical conductivity of TiO 2 electrodes but also accelerate the entry and diffusion of lithium ions. They deliver much superior rate capability compared to mesoporous TiO 2 , nonporous TiO 2 /C, and nonporous TiO 2 spheres. Furthermore, synthetic conditions of solvothermal time and calcination temperature are systematically investigated. The results demonstrate that the conductive layer, porosity, and nanocrystal size all determine the rate capability of the TiO 2 electrode. This work not only represents a green and lowcost method for the synthesis of advanced TiO 2 anode materials but also constructs an advanced electrode with high electronic conductivity, high porosity, and small nanocrystals, affording an important and meaningful reference for material synthesis and electrode design.

show abstract

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

Cited by 80 publications

References 57 publications

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

Intercalation Chemistry of the Disordered Rocksalt Li₃V₂O₅ Anode from Cluster Expansions and Machine Learning Interatomic Potentials

In Situ Conformal Carbon Coating for Constructing Hierarchical Mesoporous Titania/Carbon Spheres as High-Rate Lithium-Ion Battery Anodes

Contact Info

Product

Resources

About

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

Cited by 80 publications

References 57 publications

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

Stabilizing Pt Electrocatalysts via Introducing Reducible Oxide Support as Reservoir of Electrons and Oxygen Species

Intercalation Chemistry of the Disordered Rocksalt Li3V2O5 Anode from Cluster Expansions and Machine Learning Interatomic Potentials

In Situ Conformal Carbon Coating for Constructing Hierarchical Mesoporous Titania/Carbon Spheres as High-Rate Lithium-Ion Battery Anodes

Contact Info

Product

Resources

About

Intercalation Chemistry of the Disordered Rocksalt Li₃V₂O₅ Anode from Cluster Expansions and Machine Learning Interatomic Potentials