MgO Nanostructures on Cu(111): Understanding Size- and Morphology-Dependent CO2 Binding and Hydrogenation

Reddy, Kasala Prabhakar; Islam, Arephin; Tian, Yi; Lim, Hojoon; Kim, Jeongjin; Kim, Dongwoo; Hunt, Adrian; Waluyo, Iradwikanari; Rodriguez, José A.

doi:10.1021/acs.jpcc.4c02049

Title: MgO Nanostructures on Cu(111): Understanding Size- and Morphology-Dependent CO₂ Binding and Hydrogenation

Journal Article · 17 April 2024 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.4c02049 · OSTI ID:2372823

Reddy, Kasala Prabhakar ^[1];

^[1]; Tian, Yi ^[2];

^[3];

^[4]; Kim, Dongwoo ^[5];

^[3];

^[6]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
State Univ. of New York (SUNY), Stony Brook, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Gwangju Institute of Science and Technology (GIST) (Korea, Republic of)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

To design and optimize cost-effective technologies for the capture, utilization, and storage of carbon dioxide (CO₂), we need a fundamental knowledge and control of chemical interactions associated with the capture and conversion of the molecule into high-value chemicals, minerals, and all kinds of materials. Bulk magnesium oxide (MgO) is frequently used for the trapping and storage of CO₂ by generation of magnesium carbonates. In this study, the growth and reactivity of MgO nanostructures on a Cu₂O/Cu(111) substrate were investigated using scanning tunneling microscopy (STM) and synchrotron-based ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). For extremely small concentrations of Mg (~ 0.01 monolayer (ML)), a well-ordered film of copper oxide with small clusters (0.2-0.5 nm in width, 0.4-0.6 Å in height) of embedded MgO was seen. At a coverage of 0.1 ML, MgO nanoparticles with a width of 0.4 to 1 nm and a height of ~ 1.5 Å were randomly distributed on the copper oxide. Further, random distribution was also observed when the MgO coverage was raised to 0.25 ML, with the width of the MgO particles increasing to 2-2.5 nm and the height reaching 2 Å. These oxide nanostructures displayed a high reactivity towards CO₂ and H₂ that is not seen for bulk MgO. Dissociation of H₂ was observed at room temperature with reaction of the H adatoms with CuO_x and C-containing groups. On the small MgO nanostructures (< 1 nm in width), instead of plain carbonate formation, there was dissociation of CO₂ into CO and C species, opening reaction channels for the conversion of this harmful molecule into oxygenates and light alkanes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0012704

OSTI ID:: 2372823

Report Number(s):: BNL--225715-2024-JAAM

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 17 Vol. 128; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: MgO Nanostructures on Cu(111): Understanding Size- and Morphology-Dependent CO2 Binding and Hydrogenation

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Title: MgO Nanostructures on Cu(111): Understanding Size- and Morphology-Dependent CO₂ Binding and Hydrogenation