The DOI matches its Crossref record; 3 of the 3 references it cites were found in a registry or an index.
Boosting Oxygen Evolution Kinetics by Mn–N–C Motifs with Tunable Spin State for Highly Efficient Solar‐Driven Water Splitting
Abstract
Solar‐driven water splitting is in urgent need for sustainable energy research, for which accelerating oxygen evolution kinetics along with charge migration is the key issue. Herein, Mn 3+ within π‐conjugated carbon nitride (C 3 N 4) in form of Mn–N–C motifs is coordinated. The spin state (eg orbital filling) of Mn centers is regulated by controlling the bond strength of Mn–N. It is demonstrated that Mn serves as intrinsic oxygen evolution reaction (OER) site and the kinetics is dependent on its spin state with an optimized eg occupancy of ≈0.95. Specifically, the governing role of eg occupancy originates from the varied binding strength between Mn and OER intermediates. Benefiting from the rapid spin state‐mediated OER kinetics, as well as extended optical absorption (to 600 nm) and accelerated charge separation by intercalated metal‐to‐ligand state, Mn–C 3 N 4 stoichiometrically splits pure water with H 2 production rate up to 695.1 µmol g−1 h−1 under simulated sunlight irradiation (AM1.5), and achieves an apparent quantum efficiency of 4.0% at 420 nm, superior to most solid‐state based photocatalysts to date. This work for the first time correlates photocatalytic redox kinetics with the spin state of active sites, and suggests a nexus between photocatalysis and spin theory.
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Cites
A fast and robust algorithm for Bader decomposition of charge density
Henkelman, G., Arnaldsson, A., & Jónsson, H. (2006) · Computational Materials Science · doi:10.1016/j.commatsci.2005.04.010 · Cited by 10,723
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
Hong, W. T., Risch, M., Stoerzinger, K. A., Grimaud, A., Suntivich, J., & Shao-Horn, Y. (2015) · Energy & Environmental Science · doi:10.1039/c4ee03869j · Cited by 2,089
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Cited by
Manipulating spin polarization of titanium dioxide for efficient photocatalysis
Pan, L., Ai, M., Huang, C., Yin, L., Liu, X., Zhang, R., Wang, S., Jiang, Z., Zhang, X., Zou, J.-J., et al. (2020) · Nature Communications · doi:10.1038/s41467-020-14333-w · Cited by 543
Self-citationMiao, J., Zhu, Y., Lang, J., Zhang, J., Cheng, S., Zhou, B., Zhang, L., Alvarez, P. J. J., & Long, M. (2021) · ACS Catalysis · doi:10.1021/acscatal.1c02031 · Cited by 428
Density Functional Theory for Electrocatalysis
Liao, X., Lu, R., Xia, L., Liu, Q., Wang, H., Zhao, K., Wang, Z., & Zhao, Y. (2022) · ENERGY & ENVIRONMENTAL MATERIALS · doi:10.1002/eem2.12204 · Cited by 420
Li, X., Wang, W., Dong, F., Zhang, Z., Han, L., Luo, X., Huang, J., Feng, Z., Chen, Z., Jia, G., et al. (2021) · ACS Catalysis · doi:10.1021/acscatal.0c05354 · Cited by 357
Advances in Oxygen Evolution Electrocatalysts for Proton Exchange Membrane Water Electrolyzers
Chen, Z., Guo, L., Pan, L., Yan, T., He, Z., Li, Y., Shi, C., Huang, Z., Zhang, X., & Zou, J. (2022) · Advanced Energy Materials · doi:10.1002/aenm.202103670 · Cited by 298
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Metadata
- Authors
- Sun, S., Shen, G., Jiang, J., Mi, W., Liu, X., Pan, L., Zhang, X., & Zou, J.
- Venue
- Advanced Energy Materials
- Publisher
- Wiley
- Published
- 2019-07-04
- Volume
- 9
- Issue
- 30
- ISSN
- 1614-6832 (ISSN-L)
- 1614-6840
- OpenAlex
- W2954832201
- Cited by
- 176
- References
- 3
- FWCI
- 4.48
- Type
- journal article
- Language
- en
- Open access
- closed
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