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Nano Research 2023, 16(5): 7527-7536 https://doi.org/10.1007/s12274-022-5274-6
Research Article | Issue | Published: 21 December 2022

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

Show Author's Information Yanyan Li1,  Keyu Chen1,  Yan Liu1,  Junhao Ma1,  Yaozu Liao2,  Haitao Yang3,  Jinsheng Cheng6,  Qin Yue4( ),  Kaiping Yuan5,  Yuan Ren1,  Yidong Zou1( ),  Yonghui Deng1,2,3( )
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
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620, China
School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063, China
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610051, China
Frontier Institute of Chip and System, Fudan University, Shanghai 200433, China
Henry-Fork School of Food Sciences, Shaoguan University, Shaoguan 512005, China
Keywords:
gas sensor, mesoporous materials, semiconductor metal oxides, gadolinium doping, benzene derivatives
Topics:
Chemical sensors
Cite this article:
Li Y, Chen K, Liu Y, et al. Gadolinium-doped mesoporous tungsten oxides: Rational synthesis, gas sensing performance, and mechanism investigation. Nano Research, 2023, 16(5): 7527-7536. https://doi.org/10.1007/s12274-022-5274-6
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Yanyan Li1, Keyu Chen1, Yan Liu1, Junhao Ma1, Yaozu Liao2, Haitao Yang3, Jinsheng Cheng6, Qin Yue4( ), Kaiping Yuan5, Yuan Ren1, Yidong Zou1( ), Yonghui Deng1,2,3( )
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
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620, China
School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063, China
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610051, China
Frontier Institute of Chip and System, Fudan University, Shanghai 200433, China
Henry-Fork School of Food Sciences, Shaoguan University, Shaoguan 512005, China

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.

Keywords: gas sensor, mesoporous materials, semiconductor metal oxides, gadolinium doping, benzene derivatives

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Publication history
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Acknowledgements

Publication history

Received: 08 September 2022
Revised: 26 October 2022
Accepted: 31 October 2022
Published: 21 December 2022
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

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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