TY - JOUR
T1 - Charge Transfer-Driven Conversion of Molecular Oxygen to Doublet State on Vanadium Diselenide (VSe2) Surface at Room Temperature
AU - Boukhvalov, Danil W.
AU - Stefan, Mariana
AU - Joita, Alexandra C.
AU - Kuo, Chia-Nung
AU - Shan Lue, Chin
AU - Politano, Antonio
N1 - Publisher Copyright:
© 2024 The Author(s). Advanced Materials Interfaces published by Wiley-VCH GmbH.
PY - 2024
Y1 - 2024
N2 - Oxygen in the excited state is essential for organic synthesis and medical treatment. Herein, a novel phenomenon is reported in which the magnetic ground state of molecular oxygen undergoes a transition at room temperature from S = 1 to S = 1/2, corresponding to the transition of O2 from a triplet to a doublet state after stable physical adsorption on the defect-free surface of bulk VSe2. This density functional theory (DFT) calculations demonstrate the stable physical adsorption of O2 on both 1T- and 2H-VSe2 surfaces without further decomposition. Electron spin resonance (ESR) measurements confirm the spin state transition. Theoretical simulations reveal the charge transfer from entangled V-3d and Se-4p bands to oxygen as the leading cause of the spin state transition. This mechanism has not been previously proposed and offers multiple potential applications, from organic synthesis to medicine. Moreover, this approach can be extended to reveal new aspects of known catalytic materials and to design novel catalysts.
AB - Oxygen in the excited state is essential for organic synthesis and medical treatment. Herein, a novel phenomenon is reported in which the magnetic ground state of molecular oxygen undergoes a transition at room temperature from S = 1 to S = 1/2, corresponding to the transition of O2 from a triplet to a doublet state after stable physical adsorption on the defect-free surface of bulk VSe2. This density functional theory (DFT) calculations demonstrate the stable physical adsorption of O2 on both 1T- and 2H-VSe2 surfaces without further decomposition. Electron spin resonance (ESR) measurements confirm the spin state transition. Theoretical simulations reveal the charge transfer from entangled V-3d and Se-4p bands to oxygen as the leading cause of the spin state transition. This mechanism has not been previously proposed and offers multiple potential applications, from organic synthesis to medicine. Moreover, this approach can be extended to reveal new aspects of known catalytic materials and to design novel catalysts.
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U2 - 10.1002/admi.202400656
DO - 10.1002/admi.202400656
M3 - Article
AN - SCOPUS:85211787759
SN - 2196-7350
JO - Advanced Materials Interfaces
JF - Advanced Materials Interfaces
ER -