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Confined Pyrolysis within Metal–Organic Frameworks To Form Uniform Ru3 Clusters for Efficient Oxidation of Alcohols
Abstract
Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru 3 (CO) 12 was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru 3 clusters stabilized by nitrogen species (Ru 3 /CN) were obtained. Importantly, we found that Ru 3 /CN exhibits excellent catalytic activity (100% conversion), high chemoselectivity (100% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru 3 /CN (4320 h –1 ) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h –1 ). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.
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Cited by
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The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts
Mitchell, S., Vorobyeva, E., & Pérez‐Ramírez, J. (2018) · Angewandte Chemie International Edition · doi:10.1002/anie.201806936 · Cited by 348
Recent advances in the precise control of isolated single-site catalysts by chemical methods
Li, Z., Wang, D., Wu, Y., & Li, Y. (2018) · National Science Review · doi:10.1093/nsr/nwy056 · Cited by 325
Self-citationUltrasmall MoOx Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution
Zhang, H., Zhang, P., Qiu, M., Dong, J., Zhang, Y., & Lou, X. W. (. (2019) · Advanced Materials · doi:10.1002/adma.201804883 · Cited by 309
Self-citationXu, Z., Zhu, J., Shu, Z., Xia, Y., Chen, R., Chen, S., Wang, Y., Zeng, L., Wang, J., Cai, Y., et al. (2024) · Joule · doi:10.1016/j.joule.2024.03.005 · Cited by 82
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Metadata
- Authors
- Ji, S., Chen, Y., Fu, Q., Chen, Y., Dong, J., Chen, W., Li, Z., Wang, Y., Gu, L., He, W., Chen, C., Peng, Q., Huang, Y., Duan, X., Wang, D., Draxl, C., & Li, Y.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-07-13
- Volume
- 139
- Issue
- 29
- Pages
- 9795-9798
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2735002352
- Cited by
- 354
- References
- 0
- FWCI
- 10.65
- Type
- journal article
- Language
- en
- Open access
- closed
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- Ji, S., Chen, Y., Fu, Q., Chen, Y., Dong, J., Chen, W., Li, Z., Wang, Y., Gu, L., He, W., Chen, C., Peng, Q., Huang, Y., Duan, X., Wang, D., Draxl, C., & Li, Y. (2017). Confined Pyrolysis within Metal–Organic Frameworks To Form Uniform Ru3 Clusters for Efficient Oxidation of Alcohols. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.7b05018
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