Due to their uncontrollable assembly and crystallization process, the synthesis of mesoporous metal oxide single crystals remains a formidable challenge. Herein, we report the synthesis of single-crystal-like mesoporous LiTiSiO by using soft micelles as templates. The key lies in the atomic-scale self-assembly and step-crystallization processes, which ensure the formation of single-crystal-like mesoporous LiTiSiO microparticles via an oriented attachment growth mechanism under the confinement of an formed carbon matrix. The mesoporous LiTiSiO anode achieves a superior rate capability (148 mAh g at 5.0 A g) and outstanding long-term cycling stability (138 mAh g after 3000 cycles at 2.0 A g) for lithium storage as a result of the ultrafast Li diffusion caused by penetrating mesochannels and nanosized crystal frameworks (5-10 nm). In comparison, bulk LiTiSiO exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths. This method is very simple and reproducible, heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.
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