Integrated Transmission Electron and Single‐Molecule Fluorescence Microscopy Correlates Reactivity with Ultrastructure in a Single Catalyst Particle

Hendriks, Frank C.; Mohammadian, Sajjad; Ristanović, Zoran; Kalirai, Sam; Meirer, Florian; Vogt, Eelco T. C.; Bruijnincx, Pieter C. A.; Gerritsen, Hans C.; Weckhuysen, Bert M.

doi:10.1002/ange.201709723

Cited by 19 publications

(13 citation statements)

References 37 publications

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“…For example, SRM has been used to unveil the photophysical and electronic properties of devices made of conductive polymers 43 or perovskite 104 . SRM has had also a dramatic impact in the field of catalysis, in which single reactivity events have been probed with nanometric accuracy in catalytic reactors such as zeolites 84,[105][106][107][108][109] . Finally, SRM mild imaging conditions allow one to study biomaterials in situ, for example in cellular environments.…”

Section: [H1] Imaging Materials In Actionmentioning

confidence: 99%

Super-resolution microscopy as a powerful tool to study complex synthetic materials

et al. 2019

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Section: [H1] Imaging Materials In Actionmentioning

confidence: 99%

Super-resolution microscopy as a powerful tool to study complex synthetic materials

et al. 2019

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“…40,42 The correlated ultrastructure-reactivity information obtained by integration of transmission electron and single-molecule fluorescence microscopy (SFM-TEM) confirmed the existence of intrinsic differences in reactivity of the acid sites in different HZSM-5 crystal particles or even within the same zeolite crystal particle. 43 Very recently, a tip-enhanced fluorescence microscopy method was developed to provide direct two-dimensional hyperspectral information (without the complex post process of data required in SFM), and the results also recognized the nonuniform spatial distribution of Brønsted acidity within individual zeolite crystals. 44 Therefore, the investigation of acid distribution on the level of crystal grains is necessary and valuable.…”

Section: Introductionmentioning

confidence: 99%

Unraveling the spatial distribution of the acidity of HZSM‐5 zeolite on the level of crystal grains

et al. 2021

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Here we developed a new method to quantitatively characterize the spatial distribution of the Brønsted acidity of HZSM-5 zeolite on the crystal grains level indirectly. The Brønsted acid sites of HZSM-5 zeolite completely covered or blocked by previous coke deposition were released gradually from the outer surface to the center of the crystal grains via shrinking core mode isothermal oxidation with high temperature and low oxygen concentration. The spatial distribution of the coke was obtained based on the one-dimensional position coordinate L rp through building and solving an enhanced shrinking core model. Then the released acidity characterized by npropylamine temperature-programmed decomposition was correlated to the specific position of L rp. The results show that the acid density is roughly homogenous while the acid strength is heterogeneous within the crystal grains. From the outer surface to the center of the crystal grains, the strength of the Brønsted acid sites increase gradually.

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“…Correlative light and electron microscopy (CLEM) is a powerful tool that combines the high sensitivity and large field of view of fluorescence (light) microscopy with the high resolution of electron microscopy to study structures and molecular distributions with nanometre resolution. The use of integrated CLEM is relatively new and is mainly used to investigate biological samples (Su et al, 2010;De Boer et al, 2015), but also finds application in material science (Karreman et al, 2012;Hendriks et al, 2018). Fiducial markers which can be detected with both light and electron microscopy can be used to correlate the images obtained with both microscopes.…”

Section: Introductionmentioning

confidence: 99%

Towards robust and versatile single nanoparticle fiducial markers for correlative light and electron microscopy

Hest

Agronskaia

Fokkema

et al. 2019

Journal of Microscopy

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SummaryFiducial markers are used in correlated light and electron microscopy (CLEM) to enable accurate overlaying of fluorescence and electron microscopy images. Currently used fiducial markers, e.g. dye‐labelled nanoparticles and quantum dots, suffer from irreversible quenching of the luminescence after electron beam exposure. This limits their use in CLEM, since samples have to be studied with light microscopy before the sample can be studied with electron microscopy. Robust fiducial markers, i.e. luminescent labels that can (partially) withstand electron bombardment, are interesting because of the recent development of integrated CLEM microscopes. In addition, nonintegrated CLEM setups may benefit from such fiducial markers. Such markers would allow switching back from EM to LM and are not available yet.Here, we investigate the robustness of various luminescent nanoparticles (NPs) that have good contrast in electron microscopy; 130 nm gold‐core rhodamine B‐labelled silica particles, 15 nm CdSe/CdS/ZnS core–shell–shell quantum dots (QDs) and 230 nm Y2O3:Eu3+ particles. Robustness is studied by measuring the luminescence of (single) NPs after various cycles of electron beam exposure. The gold‐core rhodamine B‐labelled silica NPs and QDs are quenched after a single exposure to 60 ke− nm–2 with an energy of 120 keV, while Y2O3:Eu3+ NPs are robust and still show luminescence after five doses of 60 ke− nm–2. In addition, the luminescence intensity of Y2O3:Eu3+ NPs is investigated as function of electron dose for various electron fluxes. The luminescence intensity initially drops to a constant value well above the single particle detection limit. The intensity loss does not depend on the electron flux, but on the total electron dose. The results indicate that Y2O3:Eu3+ NPs are promising as robust fiducial marker in CLEM.Lay DescriptionLuminescent particles are used as fiducial markers in correlative light and electron microscopy (CLEM) to enable accurate overlaying of fluorescence and electron microscopy images. The currently used fiducial markers, e.g. dyes and quantum dots, loose their luminescence after exposure to the electron beam of the electron microscope. This limits their use in CLEM, since samples have to be studied with light microscopy before the sample can be studied with electron microscopy. Robust fiducial markers, i.e. luminescent labels that can withstand electron exposure, are interesting because of recent developments in integrated CLEM microscopes. Also nonintegrated CLEM setups may benefit from such fiducial markers. Such markers would allow for switching back to fluorescence imaging after the recording of electron microscopy imaging and are not available yet.Here, we investigate the robustness of various luminescent nanoparticles (NPs) that have good contrast in electron microscopy; dye‐labelled silica particles, quantum dots and lanthanide‐doped inorganic particles. Robustness is studied by measuring the luminescence of (single) NPs after various cycles of electron beam exposure. The dye‐labelle...

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Integrated Transmission Electron and Single‐Molecule Fluorescence Microscopy Correlates Reactivity with Ultrastructure in a Single Catalyst Particle

Cited by 19 publications

References 37 publications

Super-resolution microscopy as a powerful tool to study complex synthetic materials

Super-resolution microscopy as a powerful tool to study complex synthetic materials

Unraveling the spatial distribution of the acidity of HZSM‐5 zeolite on the level of crystal grains

Towards robust and versatile single nanoparticle fiducial markers for correlative light and electron microscopy

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