Nanocarbon oxidation in the environmental transmission electron microscope - Disentangling the role of the electron beamShow others and affiliations
2024 (English)In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 218, article id 118686Article in journal (Refereed) Published
Abstract [en]
Environmental transmission electron microscopy (ETEM) can provide unique insights into nanocarbon oxidation processes through atomic resolution and real time imaging of materials at high temperatures in reactive atmospheres. However, the electron beam can also influence the reaction rates, and even alter the processes entirely, complicating the interpretation of the in situ observations. Many mechanisms have been proposed to account for the impact of the electron beam, predominantly involving ionization of the oxidative gases to form more reactive species. However, these mechanisms have not been critically evaluated and compared to predictions from theory. Here, we evaluate the impact of the electron beam both qualitatively (oxidation mode and spatial extent) and quantitatively (oxidation rates), using high resolution imaging and electron energy loss spectroscopy, at different electron energies and dose rates. We demonstrate that transient defects generated by elastic scattering, forming highly active sites for carbon abstraction by oxygen, is the main mechanism for the enhanced oxidation rates observed in situ. This is evident from an insensitivity to electron energy and saturation of the effects at high electron dose rates. To avoid undue influence of the electron beam in future ETEM studies, we therefore recommend conditions where the intrinsic oxidation dominates over the beam-enhanced oxidation (note that no conditions are completely “safe”) and extensive comparisons with other methods. © 2023 The Author(s)
Place, publisher, year, edition, pages
Elsevier Ltd , 2024. Vol. 218, article id 118686
Keywords [en]
Carbon black; Dissociation; Electron beams; Electron energy levels; Electron scattering; Electrons; Energy dissipation; High resolution transmission electron microscopy; Impact ionization; Ionization of gases; Oxidation; Reaction rates; Condition; Dose rate; Electron beam effects; Electron dose; Electron-beam; Electrons energy; Environmental transmission electron microscopes; Environmental transmission electron microscopy; Nanocarbons; Oxidation rates; Electron energy loss spectroscopy
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
URN: urn:nbn:se:ri:diva-68780DOI: 10.1016/j.carbon.2023.118686Scopus ID: 2-s2.0-85178132166OAI: oai:DiVA.org:ri-68780DiVA, id: diva2:1827669
Funder
Swedish Research Council, 2020-04453Swedish Research Council, 2017-04902
Note
We thank Jens Kling for assistance of, and discussion regarding, the operation of the ETEM at DTU, Vesna Mirosavljevic at Trelleborg AB for supplying CB, and Hugo Selling for assistance with the preliminary quantification of the oxidation rate at low pressures. The authors acknowledge support from NanoLund and funding from the Swedish Research Council (grant numbers 2020-04453 and 2017-04902 ).
2024-01-152024-01-152025-09-23Bibliographically approved