Topotactic reduction of layered double hydroxides for atomically thick two-dimensional non-noble-metal alloy
Layered double hydroxides (LDHs) have been widely used as catalysts owing to their tunable structure and atomic dispersion of high-valence metal ions; however, limited tunability of electronic structure and valence states have hindered further improvement in their catalytic performance. Herein, we reduced ultrathin LDH precursors in situ and topotactically converted them to atomically thick (~2 nm) two-dimensional (2D) multi-metallic, single crystalline alloy nanosheets with highly tunable metallic compositions. The as-obtained alloy nanosheets not only maintained the vertically aligned ultrathin 2D structure, but also inherited the atomic dispersion of the minor metallic compositions of the LDH precursors, even though the atomic percentage was higher than 20%, which is far beyond the reported percentages for single-atom dispersions (usually less than 0.1%). Besides, surface engineering of the alloy nanosheets can finely tune the surface electronic structure for catalytic applications. Such in situ topotactic conversion strategy has introduced a novel approach for atomically dispersed alloy nanostructures and reinforced the synthetic methodology for ultrathin 2D metal-based catalysts.
Keywordsatomic thickness two-dimensional (2D) nanosheets non-noble-metal alloy atomic dispersion catalysis
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- Duan, H. H.; Yan, N.; Yu, R.; Chang, C. R.; Zhou, G.; Hu, H. S.; Rong, H. P.; Niu, Z. Q.; Mao, J. J.; Asakura, H. et al. Ultrathin rhodium nanosheets. Nat. Commun. 2014, 5, 3093.Google Scholar
- Song, F.; Hu, X. L. Exfoliation of layered double hydroxides for enhanced oxygen evolution catalysis. Nat. Commun. 2014, 5, 4477.Google Scholar
- Hogeboom, G. H.; Schneider, W. C.; Pallade, G. E. Cytochemical studies of mammalian tissues I. Isolation of intact mitochondria from rat liver; some biochemical properties of mitochondria and submicroscopic particulate material. J. Biol. Chem. 1948, 172, 619–635.Google Scholar
- Evans, D. G.; Slade, R. C. T. Structural aspects of layered double hydroxides. In Layered Double Hydroxides; Duan, X.; Evans, D. G., Eds.; Springer: Berlin Heidelberg, 2006; pp 1–87.Google Scholar
- Schneider, W. Methods for the isolation of particulate components of the cell. In Manometric Techniques; Burgess: Minneapolis, Minnesota, 1957; pp 188–201.Google Scholar