A Multitechnique Study of C2H4 Adsorption on Fe3O4(001)

Lena Puntscher; Panukorn Sombut; Chunlei Wang; Manuel Ulreich; Jiri Pavelec; Ali Rafsanjani-Abbasi; Matthias Meier; Adam Lagin; Martin Setvin; Ulrike Diebold; Cesare Franchini; Michael Schmid; Gareth S. Parkinson

doi:10.1021/acs.jpcc.3c03684

A Multitechnique Study of C₂H₄ Adsorption on Fe₃O₄(001)

Lena Puntscher
, Panukorn Sombut
, Chunlei Wang
, Manuel Ulreich
, Jiri Pavelec
, Ali Rafsanjani-Abbasi
, Matthias Meier
, Adam Lagin
, Martin Setvin
, Ulrike Diebold
, Cesare Franchini
, Michael Schmid
, Gareth S. Parkinson (Corresponding author)

Computational Materials Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

The adsorption/desorption of ethene (C2H4), also commonly known as ethylene, on Fe3O4(001) was studied under ultrahigh vacuum conditions using temperature-programmed desorption (TPD), scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory (DFT)-based computations. To interpret the TPD data, we have employed a new analysis method based on equilibrium thermodynamics. C2H4 adsorbs intact at all coverages and interacts most strongly with surface defects such as antiphase domain boundaries and Fe adatoms. On the regular surface, C2H4 binds atop surface Fe sites up to a coverage of 2 molecules per (√2 × √2)R45° unit cell, with every second Fe occupied. A desorption energy of 0.36 eV is determined by analysis of the TPD spectra at this coverage, which is approximately 0.1-0.2 eV lower than the value calculated by DFT + U with van der Waals corrections. Additional molecules are accommodated in between the Fe rows. These are stabilized by attractive interactions with the molecules adsorbed at Fe sites. The total capacity of the surface for C2H4 adsorption is found to be close to 4 molecules per (√2 × √2)R45° unit cell.

Original language	English
Pages (from-to)	18378-18388
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	127
Issue number	37
Early online date	11 Sept 2023
DOIs	https://doi.org/10.1021/acs.jpcc.3c03684
Publication status	Published - 21 Sept 2023

Funding

L.P., G.S.P., J.P., P.S., A.R.-A., and M.M. acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. [864628], Consolidator Research Grant ‘E-SAC’). This work was also supported by the Austrian Science Fund (FWF) under project number F81, Taming Complexity in Materials Modeling (TACO) (M.M., C.W., M.U., J.P., G.S.P., U.D., M.S., and C.F.). The computational results presented have been achieved by using the Vienna Scientific Cluster. Open Access is funded by the Austrian Science Fund (FWF).

Austrian Fields of Science 2012

103020 Surface physics
104017 Physical chemistry

Access to Document

10.1021/acs.jpcc.3c03684Licence: CC BY 4.0

Cite this

@article{54b2ab6712e54a99a494a479677e650b,

title = "A Multitechnique Study of C2H4 Adsorption on Fe3O4(001)",

abstract = "The adsorption/desorption of ethene (C2H4), also commonly known as ethylene, on Fe3O4(001) was studied under ultrahigh vacuum conditions using temperature-programmed desorption (TPD), scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory (DFT)-based computations. To interpret the TPD data, we have employed a new analysis method based on equilibrium thermodynamics. C2H4 adsorbs intact at all coverages and interacts most strongly with surface defects such as antiphase domain boundaries and Fe adatoms. On the regular surface, C2H4 binds atop surface Fe sites up to a coverage of 2 molecules per (√2 × √2)R45° unit cell, with every second Fe occupied. A desorption energy of 0.36 eV is determined by analysis of the TPD spectra at this coverage, which is approximately 0.1-0.2 eV lower than the value calculated by DFT + U with van der Waals corrections. Additional molecules are accommodated in between the Fe rows. These are stabilized by attractive interactions with the molecules adsorbed at Fe sites. The total capacity of the surface for C2H4 adsorption is found to be close to 4 molecules per (√2 × √2)R45° unit cell.",

author = "Lena Puntscher and Panukorn Sombut and Chunlei Wang and Manuel Ulreich and Jiri Pavelec and Ali Rafsanjani-Abbasi and Matthias Meier and Adam Lagin and Martin Setvin and Ulrike Diebold and Cesare Franchini and Michael Schmid and Parkinson, \{Gareth S.\}",

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AU - Puntscher, Lena

AU - Sombut, Panukorn

AU - Wang, Chunlei

AU - Ulreich, Manuel

AU - Pavelec, Jiri

AU - Rafsanjani-Abbasi, Ali

AU - Meier, Matthias

AU - Lagin, Adam

AU - Setvin, Martin

AU - Diebold, Ulrike

AU - Franchini, Cesare

AU - Schmid, Michael

AU - Parkinson, Gareth S.

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N2 - The adsorption/desorption of ethene (C2H4), also commonly known as ethylene, on Fe3O4(001) was studied under ultrahigh vacuum conditions using temperature-programmed desorption (TPD), scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory (DFT)-based computations. To interpret the TPD data, we have employed a new analysis method based on equilibrium thermodynamics. C2H4 adsorbs intact at all coverages and interacts most strongly with surface defects such as antiphase domain boundaries and Fe adatoms. On the regular surface, C2H4 binds atop surface Fe sites up to a coverage of 2 molecules per (√2 × √2)R45° unit cell, with every second Fe occupied. A desorption energy of 0.36 eV is determined by analysis of the TPD spectra at this coverage, which is approximately 0.1-0.2 eV lower than the value calculated by DFT + U with van der Waals corrections. Additional molecules are accommodated in between the Fe rows. These are stabilized by attractive interactions with the molecules adsorbed at Fe sites. The total capacity of the surface for C2H4 adsorption is found to be close to 4 molecules per (√2 × √2)R45° unit cell.

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