Synergy of oxygen defects and structural modulation on titanium niobium oxide with a constructed conductive network for high-rate lithium-ion half/full batteries†
Abstract
Titanium niobium oxide as an electrode material for lithium-ion batteries (LIBs) has relatively high working potential and theoretical capacity, which is expected to replace a graphite anode. However, it possesses low electronic conductivity, leading to the internal electrochemical polarization of the battery during high current charging, which is mainly reflected in the large difference between the actual electrode capacity and the theoretical capacity, as well as the unsatisfactory rate performance. In this work, a strategy of oxygen defect creation and structural modulation of Ti2Nb10O29 (TNO) was applied to synthesize oxygen-deficient N-doped carbon and graphene-covered TNO (Od-TNO@NC-G). The electronic conductivity of TNO is significantly increased by this precise Od-TNO@NC-G structure, which is advantageous for increasing the electrochemical kinetics and modulating stress release during Li+ (de)insertion. As applied in LIBs, Od-TNO@NC-G delivers a high capacity of 235 mA h g−1 after 200 cycles at 1 C, which is comparable with pure TNO (112 mA h g−1 after 200 cycles at 1 C). Impressively, an ultra-stable cycle life assessment over 20 000 cycles of Od-TNO@NC-G can be achieved at 10 C. For the purpose of verifying the functionality of oxygen defects in Od-TNO@NC-G for LIBs, thorough first-principles calculations were done. The Od-TNO@NC-G//LiFePO4 pouch cell was constructed, also exhibiting a magnificent capacity of 116 mA h g−1 after 2000 cycles at 5 C (capacity retention: 93.8%). This excellent LIB performance is due to the synergistic effect of oxygen vacancy and double carbon coating structure of Od-TNO@NC-G. We provide a thorough comprehension of Od-TNO@NC-G for superior LIB performance from both practical and theoretical viewpoints, opening the door for the development of next-generation advanced energy storage systems.
- This article is part of the themed collection: 2023 Inorganic Chemistry Frontiers HOT articles
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