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Regulating Spin Polarization through Cationic Vacancy Defects in Bi<sub>4</sub>Ti<sub>3</sub>O<sub>12</sub> for Enhanced Molecular Oxygen Activation

Dongpeng Zhang, Yanxiao Li, Yanxiao Li, Pengfei Wang, Jinyong Qu, Sihui Zhan, Yi Li, Yi Li

2023Angewandte Chemie12 citationsDOIOpen Access PDF

Abstract

Abstract Molecular oxygen (O 2 ) activation technology is of great significance in environmental purification due to its eco‐friendly operation and cost‐effective nature. However, the activation of O 2 is limited by spin‐forbidden transitions, and efficient molecular oxygen activation depends on electronic behavior and surface adsorption. Herein, we prepared cationic defect‐rich Bi 4 Ti 3 O 12 (BTO‐MV2) catalysts containing Ti vacancies ( V Ti ) for O 2 activation in water purification. The V Ti on BTO nanosheets can induce electron spin polarization, increasing the number of spin‐down photogenerated electrons and reducing the recombination of electron‐hole pairs. An active surface V Ti is also formed, serving as a center for adsorbing O 2 and extracting electrons, effectively generating ⋅OH, O 2 .− and 1 O 2 . The degradation rate constant of tetracycline achieved by BTO‐MV2 is 3.3 times faster than BTO, indicating a satisfactory prospect for practical application. This work provides an efficient pathway to activate molecular oxygen by constructing new active sites through cationic vacancy modification technology.

Topics & Concepts

Cationic polymerizationOxygenCatalysisPhotochemistryChemistryElectronAdsorptionVacancy defectPolarization (electrochemistry)Materials scienceChemical physicsPhysical chemistryCrystallographyPhysicsOrganic chemistryQuantum mechanicsAdvanced Photocatalysis TechniquesElectronic and Structural Properties of OxidesCatalytic Processes in Materials Science