Ab initio molecular dynamics simulation study of successive hydrogenation reactions of carbon monoxide producing methanol

Abstract

Doing ab initio molecular dynamics simulations, we demonstrate a possibility of hydrogenation of carbon monoxide producing methanol step by step. At first, the hydrogen atom reacts with the carbon monoxide molecule at the excited state forming the formyl radical. Formaldehyde was formed after adding one more hydrogen atom to the system. Finally, absorption of two hydrogen atoms to formaldehyde produces methanol molecule. This study is performed by using the all-electron mixed basis approach based on the time dependent density functional theory within the adiabatic local density approximation for an electronic ground-state configuration and the one-shot GW approximation for an electronic excited state configuration.

Photochemistry in Hot H2-dominated Exoplanet Atmospheres

“…Alternatively, carbon formed by equation R2 can react with H2 or H or CO, initiating the formation of the precursors CH and C2O, leading to the formation of complex organics as well as methane. Literature studies determined that in the ground-state CO + H reaction has a barrier of about 4 kcal/mol ( (Pham et al 2016) and references therein) and concluded that HCO formation must occur in CO* excited state, leading all the way to the formation of H2CO and CH3OH (not observed in our experiments).…”

“…The gas-phase HCO radical has also strong absorption at 2434 cm -1 (Jacox 2004). Although its formation from H2 and CO would not be surprising (Pham, et al 2016), its persistence at 1473 K in the chamber and subsequently on the sapphire window at room temperature is unlikely. One explanation is that HCO could be etched into the sapphire window and trapped through chemisorption.…”

Toward Efficient GW Calculations Using Numerical Atomic Orbitals: Benchmarking and Application to Molecular Dynamics Simulations

“…In subsections 3.1, 3.2, and 3.3, we describe the treatment of real-space variables by means of NAOs and an efficient method of computing the response function. Moreover, we report the methods to realize AIMD simulations and the frozen-phonon approximation for the normal-mode coupling coefficients (20) in the Supporting Information.…”

Carbon Monoxide Hydrogenation on Ice Surfaces

“…In interstellar clouds, small dusts covered with ice provide substrates to produce simple organic molecules, where chemical reactions proceed efficiently compared to gas phase . The reaction of H+CO→HCO is the first step towards the production of simple organic molecules such as H 2 CO and CH 3 OH . This reaction is considered important on ice surfaces to reproduce the observed abundance of these molecules .…”