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Cited by 136Gas Sensing Nanomaterials and SensorsSpectroscopy and Laser ApplicationsMetal-Organic Frameworks: Synthesis and Applications

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Metal–Organic Framework‐Surface‐Enhanced Infrared Absorption Platform Enables Simultaneous On‐Chip Sensing of Greenhouse Gases

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Zhou, Hong, Hui, Xindan, Li, Dongxiao, Hu, Donglin, Chen, Xin, He, Xianming, Gao, Lingxiao, Huang, He, Lee, Chengkuo, Mu, Xiaojing·2020·Advanced Science
DOI 10.1002/advs.202001173PMC PMC7578855
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Abstract

Simultaneous on‐chip sensing of multiple greenhouse gases in a complex gas environment is highly desirable in industry, agriculture, and meteorology, but remains challenging due to their ultralow concentrations and mutual interference. Porous microstructure and extremely high surface areas in metal–organic frameworks (MOFs) provide both excellent adsorption selectivity and high gases affinity for multigas sensing. Herein, it is described that integrating MOFs into a multiresonant surface‐enhanced infrared absorption (SEIRA) platform can overcome the shortcomings of poor selectivity in multigas sensing and enable simultaneous on‐chip sensing of greenhouse gases with ultralow concentrations. The strategy leverages the near‐field intensity enhancement (over 1500‐fold) of multiresonant SEIRA technique and the outstanding gas selectivity and affinity of MOFs. It is experimentally demonstrated that the MOF–SEIRA platform achieves simultaneous on‐chip sensing of CO 2 and CH 4 with fast response time (<60 s), high accuracy (CO 2: 1.1%, CH 4: 0.4%), small footprint (100 × 100 µm 2), and excellent linearity in wide concentration range (0–2.5 × 10 4 ppm). Additionally, the excellent scalability to detect more gases is explored. This work opens up exciting possibilities for the implementation of all‐in‐one, real‐time, and on‐chip multigas detection as well as provides a valuable toolkit for greenhouse gas sensing applications.

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Figure 1 Illustration of the MOF–SEIRA platform for simultaneous sensing of CO2 and CH4 gases. a) Schematic representation of the MOF–SEIRA platform consisting of porous ZIF‐8 and metamaterial perfect absorber. Inset: CO2 and CH4 molecules are simultaneously trapped in the cavity and pore aperture of the ZIF‐8, and the MOF is attached to the surface of the antenna covered by the hotspot. b) A stick diagram showing the structure of ZIF‐8 with zinc–nitrogen tetrahedra. c) The absorber resonance position is engineered to overlap with the vibration signals of both the CO2 and CH4 absorption bands at the same time, achieving the simultaneous sensing of CO2 and CH4 gases.
Figure 1 Illustration of the MOF–SEIRA platform for simultaneous sensing of CO2 and CH4 gases. a) Schematic representation of the MOF–SEIRA platform consisting of porous ZIF‐8 and metamaterial perfect absorber. Inset: CO2 and CH4 molecules are simultaneously trapped in the cavity and pore aperture of the ZIF‐8, and the MOF is attached to the surface of the antenna covered by the hotspot. b) A stick diagram showing the structure of ZIF‐8 with zinc–nitrogen tetrahedra. c) The absorber resonance position is engineered to overlap with the vibration signals of both the CO2 and CH4 absorption bands at the same time, achieving the simultaneous sensing of CO2 and CH4 gases.CC BY · PubMed Central
Figure 2 Simulation, modeling, and proof‐of‐concept demonstration of the MOF–SEIRA platform. a) Schematic of the multiresonant metamaterial absorber. Dimensions: L = 2.3 µm, W = 1 µm, P = 3.5 µm, t 1 = 100 nmL, t 2 = 200 nm, t 3 = 100 nm. b) Simulated absorption spectrum of the MOF–SEIRA platform for the nominal configuration (red curve), and with varying width W (green curves, 0.9 ≤ W ≤ 1.1) and length L (orange curves, 2.27 ≤ L ≤ 2.43). c) Near‐field distribution of the MOF–SEIRA platform parallel (upper) and perpendicular (bottom) to the substrate plane at the CO2 (left) and CH4 (right) bands. d) Generalized absorber model for the metamaterial absorber. I: Schematic of the metamaterial absorber. II: Generalized absorber model. III: Simulated absorption spectra and model fit spectra. e) Extension of generalized model for the MOF–SEIRA platform. f) Corresponding model when CO2 and CH4 are loaded. κ 1, κ 2, κ 3, µ, and υ represent coupling coefficient. g) Measured absorption spectra for bare metamaterial absorber, h) MOF thin film, and i) MOF–SEIRA platform in vacuum and 2000 ppm CO2. The thickness of MOF on both the absorber and the Au/Si were set to 400 nm.
Figure 2 Simulation, modeling, and proof‐of‐concept demonstration of the MOF–SEIRA platform. a) Schematic of the multiresonant metamaterial absorber. Dimensions: L = 2.3 µm, W = 1 µm, P = 3.5 µm, t 1 = 100 nmL, t 2 = 200 nm, t 3 = 100 nm. b) Simulated absorption spectrum of the MOF–SEIRA platform for the nominal configuration (red curve), and with varying width W (green curves, 0.9 ≤ W ≤ 1.1) and length L (orange curves, 2.27 ≤ L ≤ 2.43). c) Near‐field distribution of the MOF–SEIRA platform parallel (upper) and perpendicular (bottom) to the substrate plane at the CO2 (left) and CH4 (right) bands. d) Generalized absorber model for the metamaterial absorber. I: Schematic of the metamaterial absorber. II: Generalized absorber model. III: Simulated absorption spectra and model fit spectra. e) Extension of generalized model for the MOF–SEIRA platform. f) Corresponding model when CO2 and CH4 are loaded. κ 1, κ 2, κ 3, µ, and υ represent coupling coefficient. g) Measured absorption spectra for bare metamaterial absorber, h) MOF thin film, and i) MOF–SEIRA platform in vacuum and 2000 ppm CO2. The thickness of MOF on both the absorber and the Au/Si were set to 400 nm.CC BY · PubMed Central
Figure 3 Material characterization and thickness analysis of MOF–SEIRA platform. SEM micrograph showing details of a) the metamaterial absorber and b) the proposed MOF–SEIRA platform. c) AFM micrograph showing details of the MOF–SEIRA platform. d,e) SEM micrograph showing cross‐sectional views of device corresponding to (a,b). Each layer is marked accordingly to indicate the difference. f) EDS mapping analysis of the MOF. g) Deposition times versus spectrum wavelength map showing the effect of MOF thickness on MOF–SEIRA platform (n = 15). h) Corresponding map when CO2 and CH4 with the concentration of 800 ppm are loaded on the platform (n = 15). i) AFM micrograph showing the final MOF thickness of MOF–SEIRA platform when MOF deposition times are fixed at 10.
Figure 3 Material characterization and thickness analysis of MOF–SEIRA platform. SEM micrograph showing details of a) the metamaterial absorber and b) the proposed MOF–SEIRA platform. c) AFM micrograph showing details of the MOF–SEIRA platform. d,e) SEM micrograph showing cross‐sectional views of device corresponding to (a,b). Each layer is marked accordingly to indicate the difference. f) EDS mapping analysis of the MOF. g) Deposition times versus spectrum wavelength map showing the effect of MOF thickness on MOF–SEIRA platform (n = 15). h) Corresponding map when CO2 and CH4 with the concentration of 800 ppm are loaded on the platform (n = 15). i) AFM micrograph showing the final MOF thickness of MOF–SEIRA platform when MOF deposition times are fixed at 10.CC BY · PubMed Central
Figure 4 Steady characteristics of the proposed MOF–SEIRA platform for simultaneous sensing of CO2 and CH4. a) The measured spectra of MOF–SEIRA platform when CO2 or b) CH4 concentrations change from 0 to 2000 ppm. The insets show the zoomed in spectral change at the CO2 or CH4 absorption peak. c) The measured spectra when CO2 and CH4 are simultaneously loaded on the platform. d–f) Corresponding difference signal showing the change in absorption spectra in (a–c). The spectrum obtained by the platform in vacuum was set as the reference spectrum. g–i) Differential absorption versus concentration profile showing their linear relationship. p < 0.05, not significant. The sensitivity S is defined by the slope angle of the linear fitting curve.
Figure 4 Steady characteristics of the proposed MOF–SEIRA platform for simultaneous sensing of CO2 and CH4. a) The measured spectra of MOF–SEIRA platform when CO2 or b) CH4 concentrations change from 0 to 2000 ppm. The insets show the zoomed in spectral change at the CO2 or CH4 absorption peak. c) The measured spectra when CO2 and CH4 are simultaneously loaded on the platform. d–f) Corresponding difference signal showing the change in absorption spectra in (a–c). The spectrum obtained by the platform in vacuum was set as the reference spectrum. g–i) Differential absorption versus concentration profile showing their linear relationship. p < 0.05, not significant. The sensitivity S is defined by the slope angle of the linear fitting curve.CC BY · PubMed Central
Figure 5 Dynamic characteristics of the proposed MOF–SEIRA platform for simultaneous sensing of CO2 and CH4. a) Scheme showing dynamic sensing behavior of the proposed MOF–SEIRA platform. b) Time‐resolved difference signal profile of 4.25 µm band, showing the absorption and detection of CO2 with concentrations varying from 0 to 1200 ppm repeatedly. The bright band reflects the presence of the asymmetrical stretching mode of C=O=C. c) Time‐resolved difference signal profile of 7.66 µm band. Presence of the υ 4 vibration is indicated accordingly in the bright band. d) Dynamic behavior of MOF–SEIRA platform as CO2 and e) CH4 concentrations increase from 0 to 2400 ppm in 400 ppm increment (n = 200). The inset is an enlarged view of the dotted frame area, showing a response time of 35 s for CO2 and 60 s for CH4. The arrows in (d,e) represent the inflow of CO2 or CH4 at the corresponding concentration. f) Linear characteristics of MOF–SEIRA platform for a wide range of CO2 and g) CH4. Fitting curve for CO2: y = 4.57 × 10−6 x +0.49 × 10−6 with R 2 = 0.98. p < 0.05, not significant. Fitting curve for CH4: y = 1.31 × 10−6 x +0.19 × 10−6 with R 2 = 0.98. p < 0.05, not significant.
Figure 5 Dynamic characteristics of the proposed MOF–SEIRA platform for simultaneous sensing of CO2 and CH4. a) Scheme showing dynamic sensing behavior of the proposed MOF–SEIRA platform. b) Time‐resolved difference signal profile of 4.25 µm band, showing the absorption and detection of CO2 with concentrations varying from 0 to 1200 ppm repeatedly. The bright band reflects the presence of the asymmetrical stretching mode of C=O=C. c) Time‐resolved difference signal profile of 7.66 µm band. Presence of the υ 4 vibration is indicated accordingly in the bright band. d) Dynamic behavior of MOF–SEIRA platform as CO2 and e) CH4 concentrations increase from 0 to 2400 ppm in 400 ppm increment (n = 200). The inset is an enlarged view of the dotted frame area, showing a response time of 35 s for CO2 and 60 s for CH4. The arrows in (d,e) represent the inflow of CO2 or CH4 at the corresponding concentration. f) Linear characteristics of MOF–SEIRA platform for a wide range of CO2 and g) CH4. Fitting curve for CO2: y = 4.57 × 10−6 x +0.49 × 10−6 with R 2 = 0.98. p < 0.05, not significant. Fitting curve for CH4: y = 1.31 × 10−6 x +0.19 × 10−6 with R 2 = 0.98. p < 0.05, not significant.CC BY · PubMed Central

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Metadata

Authors
Zhou, H., Hui, X., Li, D., Hu, D., Chen, X., He, X., Gao, L., Huang, H., Lee, C., & Mu, X.
Affiliations
  • Chongqing University (CN)
  • National University of Singapore (SG)
Corresponding author
  • Lee, Chengkuo
  • Mu, Xiaojing
ORCID
Venue
Advanced Science
Publisher
Wiley
Published
2020-09-18
Volume
7
Issue
20
Pages
2001173-2001173
ISSN
2198-3844 (ISSN-L)
DOI
10.1002/advs.202001173
PMC
PMC7578855
OpenAlex
W3087008916
Cited by
136
References
47
Citations by year
2026: 10 · 2025: 29 · 2024: 26 · 2023: 28 · 2022: 20 · 2021: 19 · 2020: 4
FWCI
6.10
Type
journal article
Language
en
Open access
Licence
Locations
  • Advanced Science (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • National University of Singapore (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • National Key Research and Development Program of China (2019YFB2004800, 2019YFB2004803, 2016YFB0402702)
  • Fundamental Research Funds for the Central Universities (2019CDCGGD320)
Topics
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Gas Sensing Nanomaterials and Sensors
  • Physical Sciences › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
  • Physical Sciences › Chemistry › Inorganic Chemistry › Metal-Organic Frameworks: Synthesis and Applications
Keywords
metal-organic frameworks, surface-enhanced infrared absorption, carbon dioxide detection, methane detection, gas selectivity

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