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Updated: May 22, 2026
Magnetometric Characterization of Intermediates in the Solid-State Electrochemistry of Redox-Active Metal-Organic Frameworks
Published on: June 9, 2023
Synergistic and Antagonistic Controlled Charge Transfer in In2S3/Bi2O3/Mo2S3 by Magnetic Field and P-Doping
Chunmei Li1, Bo Peng1, Donghai Qiu1
1College of Physics and Optoelectronic Engineering, Chongqing Normal University, Chongqing 401331, P. R. China.
Abstract:
The O-O bond formation during water oxidation involves a spin transition from diamagnetic hydroxides to paramagnetic O2, suggesting spin states critically influence photoelectrochemical water splitting. Herein, we develop a sequential dual-modulation strategy by integrating phosphorus doping and external magnetic field (MF) into In2S3/Bi2O3/Mo2S3 heterostructures. Phosphorus doping narrows the band gap and passivates sulfur vacancies, delivering a photocurrent of 6.0 mA cm-2 at 1.23 V vs RHE and a charge separation efficiency (ηsep) of 75%, which is far surpassing the pristine heterostructure (3.6 mA cm-2, 30%). Under an external MF, spin polarization is enhanced via increased localized magnetic moments, accelerating charge separation and transfer of In2S3/Bi2O3/Mo2S3-MF, as evidenced by the prolonged carrier lifetime (4152 ns) and the lowered Gibbs free energies of the oxygen evolution intermediates (1.69 eV). Conversely, due to the phosphorus doping disrupting the magnetic moment landscape, the MF-assisted photoanode decreases the ηsep (58%) and photocurrent (5.0 mA cm-2). This work identifies the coupling of defect engineering and spin manipulation in photoanodes, establishing a spintronic framework for high-efficiency, magneto-responsive water oxidation.
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