The DOI matches its Crossref record; 62 of the 62 references it cites were found in a registry or an index.
Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites
Open accessAbstract
Exploration of efficient water oxidation catalysts (WOCs) is the primary challenge in conversion of renewable energy into fuels. Here we report a molecularly well-defined heterogeneous WOC with Aza-fused, π-conjugated, microporous polymer (Aza-CMP) coordinated single cobalt sites (Aza-CMP-Co). The single cobalt sites in Aza-CMP-Co exhibited superior activity under alkaline and near-neutral conditions. Moreover, the molecular nature of the isolated catalytic sites makes Aza-CMP-Co a reliable model for studying the heterogeneous water oxidation mechanism. By a combination of experimental and theoretical results, a pH-dependent nucleophilic attack pathway for O-O bond formation was proposed. Under alkaline conditions, the intramolecular hydroxyl nucleophilic attack (IHNA) process with which the adjacent -OH group nucleophilically attacks Co 4+=O was identified as the rate-determining step. This process leads to lower activation energy and accelerated kinetics than those of the intermolecular water nucleophilic attack (WNA) pathway. This study provides significant insights into the crucial function of electrolyte pH in water oxidation catalysis and enhancement of water oxidation activity by regulation of the IHNA pathway.
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Cited by
Shih, A. J., Monteiro, M. C. O., Dattila, F., Pavesi, D., Philips, M., da Silva, A. H. M., Vos, R. E., Ojha, K., Park, S., van der Heijden, O., et al. (2022) · Nature Reviews Methods Primers · doi:10.1038/s43586-022-00164-0 · Cited by 521
Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application
Gao, Y., Liu, B., & Wang, D. (2023) · Advanced Materials · doi:10.1002/adma.202209654 · Cited by 319
Luo, N., Cai, A., Pei, J., Zeng, X., Wang, X., & Yao, N. (2025) · Advanced Functional Materials · doi:10.1002/adfm.202425503 · Cited by 42
Metadata
- Authors
- Yang, H., Li, F., Zhan, S., Liu, Y., Li, W., Meng, Q., Kravchenko, A., Liu, T., Yang, Y., Fang, Y., Wang, L., Guan, J., Furó, I., Ahlquist, M. S. G., & Sun, L.
- Venue
- Nature Catalysis
- Published
- 2022-05-25
- Volume
- 5
- Issue
- 5
- Pages
- 414-429
- ISSN
- 2520-1158 (ISSN-L)
- OpenAlex
- W4281479548
- Cited by
- 282
- References
- 62
- FWCI
- 10.69
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Yang, H., Li, F., Zhan, S., Liu, Y., Li, W., Meng, Q., Kravchenko, A., Liu, T., Yang, Y., Fang, Y., Wang, L., Guan, J., Furó, I., Ahlquist, M. S. G., & Sun, L. (2022). Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites. Nature Catalysis. https://doi.org/10.1038/s41929-022-00783-6
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