Please use this identifier to cite or link to this item: http://hdl.handle.net/10995/111334
Title: Carbon Atom Reactivity with Amorphous Solid Water: H2O-Catalyzed Formation of H2CO
Authors: Molpeceres, G.
Kästner, J.
Fedoseev, G.
Qasim, D.
Schömig, R.
Linnartz, H.
Lamberts, T.
Issue Date: 2021
Publisher: American Chemical Society
American Chemical Society (ACS)
Citation: Carbon Atom Reactivity with Amorphous Solid Water: H2O-Catalyzed Formation of H2CO / G. Molpeceres, J. Kästner, G. Fedoseev et al. — DOI 10.21538/0134-4889-2020-26-3-154-170 // Journal of Physical Chemistry Letters. — 2021. — Vol. 12. — Iss. 44. — P. 10854-10860.
Abstract: We report new computational and experimental evidence of an efficient and astrochemically relevant formation route to formaldehyde (H2CO). This simplest carbonylic compound is central to the formation of complex organics in cold interstellar clouds and is generally regarded to be formed by the hydrogenation of solid-state carbon monoxide. We demonstrate H2CO formation via the reaction of carbon atoms with amorphous solid water. Crucial to our proposed mechanism is a concerted proton transfer catalyzed by the water hydrogen bonding network. Consequently, the reactions 3C + H2O → 3HCOH and 1HCOH → 1H2CO can take place with low or without barriers, contrary to the high-barrier traditional internal hydrogen migration. These low barriers (or the absence thereof) explain the very small kinetic isotope effect in our experiments when comparing the formation of H2CO to D2CO. Our results reconcile the disagreement found in the literature on the reaction route C + H2O → H2CO. © 2021 The Authors. Published by American Chemical Society.
Keywords: AMORPHOUS CARBON
CARBON MONOXIDE
HYDROGEN
HYDROGEN BONDS
AMORPHOUS SOLID WATER
CARBON ATOMS
CARBONYLIC COMPOUNDS
COMPLEX ORGANICS
EXPERIMENTAL EVIDENCE
FORMATION ROUTES
HYDROGEN BONDING NETWORK
INTERSTELLAR CLOUDS
SIMPLE++
SOLID-STATE CARBON
CATALYSIS
URI: http://hdl.handle.net/10995/111334
Access: info:eu-repo/semantics/openAccess
SCOPUS ID: 85119067187
PURE ID: 28958972
ISSN: 1948-7185
DOI: 10.21538/0134-4889-2020-26-3-154-170
metadata.dc.description.sponsorship: Ko-Ju Chuang and Melissa McClure are greatly thanked for stimulating discussions. We also thank the anonymous reviewers for their suggestions. Computer time was granted by the state of Baden-Württemberg through bwHPC and the German Research Foundation (DFG) through grant no. INST 40/467-1FUGG is greatly acknowledged. G.M thanks the Alexander von Humboldt Foundation for a postdoctoral research grant. We thank the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for supporting this work by funding EXC 2075-390740016 under Germany’s Excellence Strategy. T.L. is grateful for support from the Dutch Research Council (NWO) via a VENI fellowship (Grant No. 722.017.008). Astrochemistry in Leiden is supported by the Dutch Astrochemistry Network (DAN) II (Project No. 648.000.029). G.F. acknowledges financial support from the Russian Ministry of Science and Higher Education via the State Assignment Contract. FEUZ-2020-0038. This work has been supported in part by the Danish National Research Foundation through the Center of Excellence “InterCat” (Grant Agreement No.: DNRF150).
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