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Spin-Magnetic Effect of d-π Conjugation Polymer Enhanced O-H Cleavage in Water Oxidation.
- Source :
-
Journal of the American Chemical Society [J Am Chem Soc] 2024 Mar 20; Vol. 146 (11), pp. 7363-7372. Date of Electronic Publication: 2024 Mar 07. - Publication Year :
- 2024
-
Abstract
- A deep understanding of the mechanism for the spin-magnetic effect on O-H cleavage is crucial for the development of new catalysts for water oxidation. Herein, we designed and synthesized the crystalline Fe-DABDT and Co-DABDT (DABDT = 2,5-diaminobenzene-1,4-dithiol) and optimized an effective magnetic moment to explore the role of the spin-magnetic effect in the regulation of water oxidation activity. It can be found that the OER activity of the catalyst is positively correlated with its effective magnetic moment. Under the external magnetic field, Fe-DABDT with more spin single electrons has a stronger spin-magnetic response to water oxidation than Fe/Co-DABDT and Co-DABDT. The increase in OER current of Fe-DABDT is nearly 2 times higher than that of Co-DABDT. Experimental and density functional theory studies show that magnetized Fe sites could realize nucleophilic reaction, accelerate the polarization of electron spin states, and promote the polar decomposition of O-H and the formation of the O-O bond. This study provides mechanistic insight into the spin-magnetic effect of oxygen evolution reaction and further understanding of the spin origin of catalytic activity, which is expected to improve the energy efficiency of hydrogen production.
Details
- Language :
- English
- ISSN :
- 1520-5126
- Volume :
- 146
- Issue :
- 11
- Database :
- MEDLINE
- Journal :
- Journal of the American Chemical Society
- Publication Type :
- Academic Journal
- Accession number :
- 38452363
- Full Text :
- https://doi.org/10.1021/jacs.3c11907