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Gadolinium-doped mesoporous tungsten oxides: Rational synthesis, gas sensing performance, and mechanism investigation

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Abstract

As a typical family of volatile toxic compounds, benzene derivatives are massive emission in industrial production and the automobile field, causing serious threat to human and environment. The reliable and convenient detection of low concentration benzene derivatives based on intelligent gas sensor is urgent and of great significance for environmental protection. Herein, through heteroatomic doping engineering, rare-earth gadolinium (Gd) doped mesoporous WO3 with uniform mesopores (15.7–18.1 nm), tunable high specific surface area (52–55 m2·g−1), and customized crystalline pore walls, was designed and utilized to fabricate highly sensitive gas sensors toward benzene derivatives, such as ethylbenzene. Thanks to the high-density oxygen vacancies (OV) and significantly increased defects (W5+) produced by Gd atoms doping into the lattice of WO3 octahedron, Gd-doped mesoporous WO3 exhibited excellent ethylbenzene sensing performance, including high response (237 vs. 50 ppm), rapid response—recovery dynamic (13 s/25 s vs. 50 ppm), and extremely low theoretical detection limit of 24 ppb. The in-situ diffuse reflectance infrared Fourier transform and gas chromatograph-mass spectrometry results revealed the gas sensing process underwent a catalytic oxidation conversion of ethylbenzene into alcohol species, benzaldehyde, acetophenone, and carboxylate species along with the resistance change of the Gd-doped mesoporous WO3 based sensor. Moreover, a portable smart gas sensing module was fabricated and demonstrated for real-time detecting ethylbenzene, which provided new ideas to design heteroatom doped mesoporous materials for intelligent sensors.

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Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2020YFB2008600), the National Natural Science Foundation of China (Nos. 21875044, 22125501, and 22105043), the Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 20JC1415300), the China Postdoctoral Science Foundation (Nos. 2021TQ0066 and 2021M690660), the Fundamental Research Funds for the Central Universities (No. 20720220010), the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, the young scientist project of MOE innovation platform, Donghua University (No. KF2120), and the Foshan Science and Technology Innovation Program (No. 2017IT100121).

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  1. Department of Chemistry, Department of Gastroenterology and Hepatology, Zhongshan Hospital, Zhangjiang Fudan International Innovation Center, State Key Laboratory of Molecular Engineering of Polymers, iChEM, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200433, China

    Yanyan Li, Keyu Chen, Yan Liu, Junhao Ma, Yuan Ren, Yidong Zou & Yonghui Deng

  2. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai, 201620, China

    Yaozu Liao & Yonghui Deng

  3. School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang, 330063, China

    Haitao Yang & Yonghui Deng

  4. Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 610051, China

    Qin Yue

  5. Frontier Institute of Chip and System, Fudan University, Shanghai, 200433, China

    Kaiping Yuan

  6. Henry-Fork School of Food Sciences, Shaoguan University, Shaoguan, 512005, China

    Jinsheng Cheng

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  1. Yanyan Li
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Li, Y., Chen, K., Liu, Y. et al. Gadolinium-doped mesoporous tungsten oxides: Rational synthesis, gas sensing performance, and mechanism investigation. Nano Res. 16, 7527–7536 (2023). https://doi.org/10.1007/s12274-022-5274-6

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