4.8 Article

Surface Lattice Oxygen Activation on Sr2Sb2O7 Enhances the Photocatalytic Mineralization of Toluene: from Reactant Activation, Intermediate Conversion to Product Desorption

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 4, Pages 5153-5164

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20996

Keywords

surface lattice oxygen; VOC degradation; toluene; reaction intermediate; photocatalysis

Funding

  1. National Natural Science Foundation of China [21822601, 21777011]
  2. Fundamental Research Funds for the Central Universities [ZYGX2019Z021]
  3. 111 Project [B20030]
  4. Plan for National Youth Talents of the Organization Department of the Central Committee [2020cxyb030]
  5. Southwest Petroleum University Graduate Research Innovation Fund Project [2020cxyb030]

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Sr2Sb2O7 demonstrates superior photocatalytic performance compared to TiO2 in toluene mineralization, attributed to the efficient activation of lattice oxygen. This activation enhances adsorption and activation of O-2 and H2O molecules, leading to increased production of radicals and improved selectivity.
Transition-metal oxide photocatalysis has attracted increasing attention in environmental remediation and solar energy conversion. Surface lattice oxygen is the key active site on the metal oxide, but its role and activation mechanism in the photocatalytic VOC mineralization are still unclear. In this work, we have demonstrated that Sr2Sb2O7 exhibits an excellent photocatalytic activity and stability compared to TiO2 (P25) in gaseous toluene mineralization because the lattice oxygen on Sr2Sb2O7 can be activated efficiently. The lattice oxygen of Sr2Sb2O7 promotes the adsorption and activation of O-2 and H2O molecules and enhances the production of O-center dot(2)- and (OH)-O-center dot radicals, as confirmed by the electron spin resonance and DFT calculations. The in situ diffuse reflectance infrared Fourier transform spectroscopy spectra are applied to dynamically monitor the intermediate activation and selective conversion. Combined with DFT calculation, the role and the mechanism of lattice oxygen in photocatalysis have been revealed. Owing to the promoted surface lattice oxygen, the selectivity for benzoic acid formation is enhanced and final product desorption is promoted, which could largely advance the ring opening and mineralization of toluene. This work reveals the origin of lattice oxygen activation and the role for efficient VOC degradation at the atomic scale.

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