High-spin active center enables magnetic-field-enhanced photocatalytic overall water splitting

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ID: 325142
2026
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Abstract
Abstract Photocatalytic reaction efficiency is governed by the spin states of active center and reaction intermediates, as it allows selective formation of desired products through spin-dependent reaction pathways. As a representative process, photocatalytic overall water splitting remains limited by water oxidation reaction, where spin-dependent formation of triplet-state O2 is thermodynamically and kinetically unfavorable. This work describes an atom-specific spin modulation strategy by selectively substituting tetrahedral Co2+ with Ni2+ in spinel Co3O4 to form NiCo2O4, which reconstructs the local coordination environment and charge distribution of octahedral Co3+, constructing a high-spin configuration with increased eg occupancy. Under the constraint of external magnetic field, high-spin Co3+ atom generates aligned parallel ·OH radicals, favoring the formation of triplet-state O2 while suppressing singlet byproducts. Meanwhile, the enhanced eg occupancy weakens the adsorption of oxygenated intermediates, lowering the Gibbs free energy barrier of the rate-determining step and accelerating water oxidation. Hence, the NiCo2O4/BiVO4 photocatalyst achieves a water oxidation rate of 148.5 ± 3.7 μmol h−1, which is 5.6 times higher than the pristine BiVO4. Furthermore, it enables near-stoichiometric overall water splitting with a solar-to-hydrogen efficiency of up to 0.309 ± 0.003%. This work underscores the importance of atom-specific spin state regulation to promote spin-polarization-dependent photocatalytic water splitting.
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Authors Yuchen Guo, Liang Mao, Yanfang Li, Sai Chen, Xin Tan, Tao Yu, Jinlong Gong
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Journal national science review
Year 2026
DOI
10.1093/nsr/nwag495
URL
https://doi.org/10.1093/nsr/nwag495
Keywords Keywords not found

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