Direct dioxygen evolution in collisions of carbon dioxide with surfaces

Abstract

The intramolecular conversion of CO 2 to molecular oxygen is an exotic reaction, rarely observed even with extreme optical or electronic excitation means. Here we show that this reaction occurs readily when CO 2 ions scatter from solid surfaces in a two-step sequential collision process at hyperthermal incidence energies. The produced O 2 is preferentially ionized by charge transfer from the surface over the predominant atomic oxygen product, leading to direct detection of both O 2 + and O 2 − . First-principles simulations of the collisional dynamics reveal that O 2 production proceeds via strongly-bent CO 2 configurations, without visiting other intermediates. Bent CO 2 provides dynamic access to the symmetric dissociation of CO 2 to C+O 2 with a calculated yield of 1 to 2% depending on molecular orientation. This unexpected collision-induced transformation of individual CO 2 molecules provides an accessible pathway for generating O 2 in astrophysical environments and may inspire plasma-driven electro- and photo-catalytic strategies for terrestrial CO 2 reduction.

Conversion of CO2 by non- thermal inductively-coupled plasma catalysis

“…the use of Zn, Cu, etc. for catalytic reaction) [35][36][37][38][39]. This work will investigate multiple experimental conditions in order to discover unknown effects and features about CO2 splitting.…”

Towards a density functional theory of molecular fragments. What is the shape of atoms in molecules?

“…Embedding methods provide the most promising route to truly calculate ab-initio electronic structures of large, complex, molecular systems (Yao, et al, 2019;Lee, et al, 2019;Mi&Pavanello, 2020). Although Partition-DFT has been applied so far only to model systems (Elliot, et al, 2010), diatomic molecules (Nafziger & Wasserman, 2014) and small hydrogen-bonded clusters (Gómez, et al, 2017;Gómez, et al, 2019), an ongoing implementation into the Psi4 package (Chávez, et al, 2020) will allow more for more widespread application.…”

Selective CO2 Conversion into Fuels on Nanochannels

“…Other methods to reduce carbon dioxide are; radiochemical, chemical reduction, thermochemical, photochemical, biochemical, etc. Photochemical and electrochemical methods have been popular in recent research (a review article), including recent publications with an exotic view with the purpose of CO 2 conversion in astrophysical environments . Coupling the electrochemical reduction of CO 2 with photovoltaics, has several advantages; the cost of photovoltaics is improving, these processes would be cleaner than for example oil refining, and less energy intensive.…”