Vacancy Control in TiNb2O7: Implications for Energy Applications

Voskanyan, Albert A.; Jayanthi, Kumar; Navrotsky, Alexandra

doi:10.1021/acs.chemmater.2c01569

Vacancy Control in TiNb₂O₇: Implications for Energy Applications

Journal Article · Thu Dec 01 23:00:00 EST 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c01569· OSTI ID:1909090

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Arizona State Univ., Tempe, AZ (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Rapid global electrification, including for transportation, has dramatically increased demand for long-lasting and faster-charging batteries. Titanium niobium oxide (TiNb₂O₇) is one of the most promising anode materials for high-power lithium-ion batteries (LIBs). However, the intrinsic low electronic conductivity of TiNb₂O₇ is a significant drawback. Herein, an almost 10 orders of magnitude increase in conductivity is achieved via reduction of TiNb₂O₇ in H₂ at 900 °C. The observed dramatic increase in electron conductivity upon reduction is unprecedented and opens new possibilities to produce niobium-based conductive materials for next-generation energy storage. Upon extended reduction, TiNb₂O₇ converts into a distorted rutile TiNb₂O₆ structure, which can be reoxidized back into the crystallographic shear phase. In addition, TiNb₂O₇ can be thermally reduced in an inert atmosphere and reoxidized by CO₂ with excellent oxygen exchange capacity. Thus, the TiNb₂O₇ Wadsley–Roth phase demonstrates outstanding potential for solar-driven thermochemical CO₂ splitting at 1400 °C. In conclusion, these findings manifest that controlling defect chemistry paves the way for developing advanced materials for LIBs and solar-driven thermochemical fuel production.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0021987

OSTI ID:: 1909090

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 23 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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