4.7 Article

Phosphorus-doped porous perovskite LaFe1-xPxO3-δ nanosheets with rich surface oxygen vacancies for ppb level acetone sensing at low temperature

期刊

CHEMICAL ENGINEERING JOURNAL
卷 431, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.134280

关键词

Perovskite; Phosphorus; Oxygen vacancy; Gas sensor; DFT; Electron orbital

资金

  1. National Natural Science of China [62033002, 61833006, 62071112, 61973058]
  2. 111 Project [B16009]
  3. Fundamental Research Funds for the Central Universities in China [N2004019, N2004028]
  4. Liao Ning Revitalization Talents Program [XLYC1807198]
  5. Hebei Natural Science [F2020501040]
  6. Liaoning Province Natural Science [2020-KF-1104]

向作者/读者索取更多资源

In this study, P-doped perovskite LaFe1-xPxO3-delta with abundant Ov defects were prepared and utilized as sensors for acetone detection. The LaFe0.99P0.01O3-delta sensor exhibited excellent gas-sensitive performance, with nearly twofold improvement in response value and a detection limit at the ppb level. Electron paramagnetic resonance and X-ray photoelectron spectroscopy confirmed the strong correlation between the sensing characteristics and the Ov defects. Theoretical analysis revealed that P doping induced Ov defects and modulated the energy levels of the material, enhancing chemisorbed oxygen species and intermolecular interactions.
Perovskite-type oxide semiconductors (ABO3) with defective conduction properties have been regarded as highly promising gas-sensitive materials due to their abundant structural types. However, pure ABO(3) gas sensors usually have suboptimal sensing response due to low specific surface area and few adsorption sites. Recently, surface oxygen vacancies (O-v) defects have been shown to be a remarkably effective way to enhance the sensing response of gas sensors by increasing the number of adsorption sites and changing the energy level structure. In view of the above, herein, P-doped perovskite LaFe1-xPxO3-delta (x = 0.005, 0.01, 0.03, 0.05) with abundant Ov defects were prepared by sol-gel method and fabricated as sensors for the acetone detection. Characterization and test results show that LaFe0.99P0.01O3-delta with porous nanosheet structure has excellent acetone gas-sensitive performance. Compared to pure LaFeO3 gas sensor, the optimal operating temperature of LaFe0.99P0.01O3-delta is reduced to 180 degrees C and response value is improved nearly twofold, whose limit of detection is even at the ppb level. Crucially, the results of electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS) verify that the sensing characteristics of the LaFe1-xPxO3-delta sensor are strongly correlated with the Ov defect. In addition, further theoretical analysis shows that P doping in LaFeO3 induces Ov defects and modulates frontier electron orbital energy levels of the material, thus increasing the chemisorbed oxygen species and enhancing the intermolecular interactions. In this work, the vital function of Ov defects in perovskite-type gas sensors is highlighted, which also provides an effective and feasible way to improve the performance of gas sensors.

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