Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation
Karolina A. Haupa, G. Tarczay, Yuan Pern Lee
Formamide (H2NCHO) is the smallest molecule possessing the biologically important amide bond. Recent interstellar observations have shown a strong correlation between the abundance of formamide and isocyanic acid (HNCO), indicating that they are likely to be chemically related, but no experiment or theory explains this correlation satisfactorily. We performed H + H2NCHO reactions in a para-hydrogen quantum-solid matrix host and identified production of H2NCO and HNCO from hydrogen-abstraction reactions. We identified also D2NCO, DNCO, HDNCO, and HDNCHO from the reaction H + D2NCHO, indicating the presence of hydrogen-addition reactions of DNCO and HDNCO. From the observed temporal profiles of H2NCHO, H2NCO, HNCO, and their deuterium isotopologues, we showed that a dual-cycle consisting of hydrogen abstraction and hydrogen addition can satisfactorily explain the quasi-equilibrium between H2NCHO and HNCO and explain other previous experimental results. Furthermore, this mechanism also indicates that the catalytic formation of H2 from H atoms might occur in interstellar ice grains.
https://doi.org/10.1021/jacs.9b04491
DNCO
Haupa, K. A., Tarczay, G., & Lee, Y. P. (2019). Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation. Journal of the American Chemical Society, 141(29), 11614-11620. https://doi.org/10.1021/jacs.9b04491
Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation. / Haupa, Karolina A.; Tarczay, G.; Lee, Yuan Pern.
Haupa, KA, Tarczay, G & Lee, YP 2019, 'Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation', Journal of the American Chemical Society, vol. 141, no. 29, pp. 11614-11620. https://doi.org/10.1021/jacs.9b04491
Haupa KA, Tarczay G, Lee YP. Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation. Journal of the American Chemical Society. 2019 Jan 1;141(29):11614-11620. https://doi.org/10.1021/jacs.9b04491
Haupa, Karolina A. ; Tarczay, G. ; Lee, Yuan Pern. / Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation. In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 29. pp. 11614-11620.
@article{bc6589919a2f43b885546958478685b7,
title = "Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation",
abstract = "Formamide (H2NCHO) is the smallest molecule possessing the biologically important amide bond. Recent interstellar observations have shown a strong correlation between the abundance of formamide and isocyanic acid (HNCO), indicating that they are likely to be chemically related, but no experiment or theory explains this correlation satisfactorily. We performed H + H2NCHO reactions in a para-hydrogen quantum-solid matrix host and identified production of H2NCO and HNCO from hydrogen-abstraction reactions. We identified also D2NCO, DNCO, HDNCO, and HDNCHO from the reaction H + D2NCHO, indicating the presence of hydrogen-addition reactions of DNCO and HDNCO. From the observed temporal profiles of H2NCHO, H2NCO, HNCO, and their deuterium isotopologues, we showed that a dual-cycle consisting of hydrogen abstraction and hydrogen addition can satisfactorily explain the quasi-equilibrium between H2NCHO and HNCO and explain other previous experimental results. Furthermore, this mechanism also indicates that the catalytic formation of H2 from H atoms might occur in interstellar ice grains.",
author = "Haupa, {Karolina A.} and G. Tarczay and Lee, {Yuan Pern}",
doi = "10.1021/jacs.9b04491",
T1 - Hydrogen Abstraction/Addition Tunneling Reactions Elucidate the Interstellar H2NCHO/HNCO Ratio and H2 Formation
AU - Haupa, Karolina A.
AU - Tarczay, G.
AU - Lee, Yuan Pern
N2 - Formamide (H2NCHO) is the smallest molecule possessing the biologically important amide bond. Recent interstellar observations have shown a strong correlation between the abundance of formamide and isocyanic acid (HNCO), indicating that they are likely to be chemically related, but no experiment or theory explains this correlation satisfactorily. We performed H + H2NCHO reactions in a para-hydrogen quantum-solid matrix host and identified production of H2NCO and HNCO from hydrogen-abstraction reactions. We identified also D2NCO, DNCO, HDNCO, and HDNCHO from the reaction H + D2NCHO, indicating the presence of hydrogen-addition reactions of DNCO and HDNCO. From the observed temporal profiles of H2NCHO, H2NCO, HNCO, and their deuterium isotopologues, we showed that a dual-cycle consisting of hydrogen abstraction and hydrogen addition can satisfactorily explain the quasi-equilibrium between H2NCHO and HNCO and explain other previous experimental results. Furthermore, this mechanism also indicates that the catalytic formation of H2 from H atoms might occur in interstellar ice grains.
AB - Formamide (H2NCHO) is the smallest molecule possessing the biologically important amide bond. Recent interstellar observations have shown a strong correlation between the abundance of formamide and isocyanic acid (HNCO), indicating that they are likely to be chemically related, but no experiment or theory explains this correlation satisfactorily. We performed H + H2NCHO reactions in a para-hydrogen quantum-solid matrix host and identified production of H2NCO and HNCO from hydrogen-abstraction reactions. We identified also D2NCO, DNCO, HDNCO, and HDNCHO from the reaction H + D2NCHO, indicating the presence of hydrogen-addition reactions of DNCO and HDNCO. From the observed temporal profiles of H2NCHO, H2NCO, HNCO, and their deuterium isotopologues, we showed that a dual-cycle consisting of hydrogen abstraction and hydrogen addition can satisfactorily explain the quasi-equilibrium between H2NCHO and HNCO and explain other previous experimental results. Furthermore, this mechanism also indicates that the catalytic formation of H2 from H atoms might occur in interstellar ice grains.
U2 - 10.1021/jacs.9b04491
DO - 10.1021/jacs.9b04491
10.1021/jacs.9b04491