The DOI matches its Crossref record; 3 of the 3 references it cites were found in a registry or an index.
Disordered, Sub-Nanometer Ru Structures on CeO2 are Highly Efficient and Selective Catalysts in Polymer Upcycling by Hydrogenolysis
Abstract
Nondegradable polyolefin plastics pose severe environmental threats and thus demand efficient upcycling technologies. In this work, we discovered that low-loading (≤0.25 wt %) Ru/CeO 2 exhibits remarkable catalytic performance in the hydrogenolysis of polypropylene (PP), polyethylene (PE), and n -C 16 H 34 that is superior to high-loading (≥0.5 wt %) Ru/CeO 2 . They possess high PP conversion efficiency (sevenfold increase over current literature reports), low selectivity toward undesired CH 4, and good isomerization ability. In the low-loading range, the intrinsic activity of Ru in PP hydrogenolysis increases as the particle size decreases, opposite of the trend in the high-loading range. Detailed characterization revealed that the abrupt changes in catalytic behaviors coincide with Ru species transitioning from well-defined to highly disordered structures in the low-loading domain. The disordered Ru species were shown to be sub-nanometer in size and cationic. Mechanistically, the regioselectivity and the rate dependence on hydrogen pressure of C–C bond cleavage are different on low- and high-loading Ru/CeO 2, both explained by the higher coverage of adsorbed hydrogen (*H) on low-loading Ru/CeO 2 . This work reveals the remarkable catalytic performance of highly disordered, sub-nanometer, cationic Ru species in polyolefin hydrogenolysis, opening immense opportunities to develop effective, selective, and versatile catalysts for plastic upcycling.
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Cites
Production, use, and fate of all plastics ever made
Geyer, R., Jambeck, J. R., & Law, K. L. (2017) · Science Advances · doi:10.1126/sciadv.1700782 · Cited by 18,606
Accumulation and fragmentation of plastic debris in global environments
Barnes, D. K. A., Galgani, F., Thompson, R. C., & Barlaz, M. (2009) · Philosophical Transactions of the Royal Society B: Biological Sciences · doi:10.1098/rstb.2008.0205 · Cited by 6,126
Polyethylene upcycling to long-chain alkylaromatics by tandem hydrogenolysis/aromatization
Zhang, F., Zeng, M., Yappert, R. D., Sun, J., Lee, Y.-H., LaPointe, A. M., Peters, B., Abu-Omar, M. M., & Scott, S. L. (2020) · Science · doi:10.1126/science.abc5441 · Cited by 882
Cited by
Dong, Z., Chen, W., Xu, K., Liu, Y., Wu, J., & Zhang, F. (2022) · ACS Catalysis · doi:10.1021/acscatal.2c04915 · Cited by 269
Mason, A. H., Motta, A., Das, A., Ma, Q., Bedzyk, M. J., Kratish, Y., & Marks, T. J. (2022) · Nature Communications · doi:10.1038/s41467-022-34707-6 · Cited by 82
Metadata
- Authors
- Chen, L., Meyer, L. C., Kovarik, L., Meira, D., Pereira-Hernandez, X. I., Shi, H., Khivantsev, K., Gutiérrez, O. Y., & Szanyi, J.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-04-05
- Volume
- 12
- Issue
- 8
- Pages
- 4618-4627
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W4223498063
- Cited by
- 213
- References
- 3
- FWCI
- 14.05
- Type
- journal article
- Language
- en
- Open access
- closed
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