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Mixed‐Valence Single‐Atom Catalyst Derived from Functionalized Graphene
Open accessAbstract
Single‐atom catalysts (SACs) aim at bridging the gap between homogeneous and heterogeneous catalysis. The challenge is the development of materials with ligands enabling coordination of metal atoms in different valence states, and preventing leaching or nanoparticle formation. Graphene functionalized with nitrile groups (cyanographene) is herein employed for the robust coordination of Cu(II) ions, which are partially reduced to Cu(I) due to graphene‐induced charge transfer. Inspired by nature's selection of Cu(I) in enzymes for oxygen activation, this 2D mixed‐valence SAC performs flawlessly in two O 2‐mediated reactions: the oxidative coupling of amines and the oxidation of benzylic CH bonds toward high‐value pharmaceutical synthons. High conversions (up to 98%), selectivities (up to 99%), and recyclability are attained with very low metal loadings in the reaction. The synergistic effect of Cu(II) and Cu(I) is the essential part in the reaction mechanism. The developed strategy opens the door to a broad portfolio of other SACs via their coordination to various functional groups of graphene, as demonstrated by successful entrapment of Fe III/Fe II single atoms to carboxy‐graphene.
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Cites
Fei, H., Dong, J., Feng, Y., Allen, C. S., Wan, C., Volosskiy, B., Li, M., Zhao, Z., Wang, Y., Sun, H., et al. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0008-y · Cited by 1,973
Atomic cobalt on nitrogen-doped graphene for hydrogen generation
Fei, H., Dong, J., Arellano-Jiménez, M. J., Ye, G., Dong Kim, N., Samuel, E. L. G., Peng, Z., Zhu, Z., Qin, F., Bao, J., et al. (2015) · Nature Communications · doi:10.1038/ncomms9668 · Cited by 1,621
Catalysis by Supported Single Metal Atoms
Liu, J. (2017) · ACS Catalysis · doi:10.1021/acscatal.6b01534 · Cited by 1,331
Zhang, C., Sha, J., Fei, H., Liu, M., Yazdi, S., Zhang, J., Zhong, Q., Zou, X., Zhao, N., Yu, H., et al. (2017) · ACS Nano · doi:10.1021/acsnano.7b02148 · Cited by 545
Jiang, K., Siahrostami, S., Akey, A. J., Li, Y., Lu, Z., Lattimer, J., Hu, Y., Stokes, C., Gangishetty, M., Chen, G., et al. (2017) · Chem · doi:10.1016/j.chempr.2017.09.014 · Cited by 406
Cited by
General synthesis of single-atom catalysts with high metal loading using graphene quantum dots
Xia, C., Qiu, Y., Xia, Y., Zhu, P., King, G., Zhang, X., Wu, Z., Kim, J. Y., Cullen, D. A., Zheng, D., et al. (2021) · Nature Chemistry · doi:10.1038/s41557-021-00734-x · Cited by 699
Single atom electrocatalysts supported on graphene or graphene-like carbons
Fei, H., Dong, J., Chen, D., Hu, T., Duan, X., Shakir, I., Huang, Y., & Duan, X. (2019) · Chemical Society Reviews · doi:10.1039/c9cs00422j · Cited by 673
Sarma, B. B., Maurer, F., Doronkin, D. E., & Grunwaldt, J.-D. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00495 · Cited by 291
Pedireddy, S., Jimenez‐Sandoval, R., Ravva, M. K., Nayak, C., Anjum, D. H., Jha, S. N., Katuri, K. P., & Saikaly, P. E. (2021) · Advanced Functional Materials · doi:10.1002/adfm.202010916 · Cited by 20
Metadata
- Authors
- Bakandritsos, A., Kadam, R. G., Kumar, P., Zoppellaro, G., Medved', M., Tuček, J., Montini, T., Tomanec, O., Andrýsková, P., Drahoš, B., Varma, R. S., Otyepka, M., Gawande, M. B., Fornasiero, P., & Zbořil, R.
- Venue
- Advanced Materials
- Publisher
- Wiley
- Published
- 2019-02-27
- Volume
- 31
- Issue
- 17
- Pages
- e1900323-e1900323
- ISSN
- 0935-9648 (ISSN-L)
- 1521-4095
- OpenAlex
- W2918365253
- Cited by
- 194
- References
- 5
- FWCI
- 8.86
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Bakandritsos, A., Kadam, R. G., Kumar, P., Zoppellaro, G., Medved', M., Tuček, J., Montini, T., Tomanec, O., Andrýsková, P., Drahoš, B., Varma, R. S., Otyepka, M., Gawande, M. B., Fornasiero, P., & Zbořil, R. (2019). Mixed‐Valence Single‐Atom Catalyst Derived from Functionalized Graphene. Advanced Materials. https://doi.org/10.1002/adma.201900323
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Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
