CO Adsorption and Disproportionation on Smooth and Defect-Rich Ir(111)

Overview

Journal J Phys Chem C Nanomater Interfaces

Publisher American Chemical Society

Date 2022 May 2

PMID 35493699

Authors

Xia Li

Thomas Haunold

Stefan Werkovits

Laurence D Marks

Peter Blaha

Gunther Rupprechter

Affiliations

Soon will be listed here.

Abstract

CO adsorption and dissociation on "perfect" and "defect-rich" Ir(111) surfaces were studied by a combination of surface-analytical techniques, including polarization-dependent (PPP and SSP) sum frequency generation (SFG) vibrational spectroscopy, low-energy electron diffraction (LEED), Auger electron spectroscopy, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. CO was found to be ordered and tilted from the surface normal at high coverage on the "perfect" surface (e.g., θ = 30° at 0.70 ML), whereas it was less ordered and preferentially upright (θ = 4-10°) on the "defect-rich" surface for coverages of 0.55-0.70 ML. SFG, LEED, and XPS revealed that CO adsorption at low pressure/high temperature and high pressure/low temperature was reversible. In contrast, upon heating to ∼600 K in near mbar CO pressure, "perfect" and even more "defect-rich" Ir(111) surfaces were irreversibly modified by carbon deposits, which, according to DFT, result from CO disproportionation.

References

Blaha P, Schwarz K, Tran F, Laskowski R, Madsen G, Marks L . WIEN2k: An APW+lo program for calculating the properties of solids. J Chem Phys. 2020; 152(7):074101. DOI: 10.1063/1.5143061. View

Haghofer A, Sonstrom P, Fenske D, Fottinger K, Schwarz S, Bernardi J . Colloidally prepared Pt nanowires versus impregnated Pt nanoparticles: comparison of adsorption and reaction properties. Langmuir. 2010; 26(21):16330-8. DOI: 10.1021/la1015912. View

Roiaz M, Falivene L, Rameshan C, Cavallo L, Kozlov S, Rupprechter G . Roughening of Copper (100) at Elevated CO Pressure: Cu Adatom and Cluster Formation Enable CO Dissociation. J Phys Chem C Nanomater Interfaces. 2019; 123(13):8112-8121. PMC: 6453259. DOI: 10.1021/acs.jpcc.8b07668. View

Liu W, Zhang L, Shen Y . Interfacial structures of methanol:water mixtures at a hydrophobic interface probed by sum-frequency vibrational spectroscopy. J Chem Phys. 2006; 125(14):144711. DOI: 10.1063/1.2354088. View

Gleissner R, Creutzburg M, Noei H, Stierle A . Interaction of Water with Graphene/Ir(111) Studied by Vibrational Spectroscopy. Langmuir. 2019; 35(35):11285-11290. DOI: 10.1021/acs.langmuir.9b01205. View

Lane I, King D, Arnolds H . The determination of an inhomogeneous linewidth for a strongly coupled adsorbate system. J Chem Phys. 2007; 126(2):024707. DOI: 10.1063/1.2408413. View

M da Silva K, Bernardi F, Abarca G, Baptista D, Leite Santos M, Fernandez Barquin L . Tuning the structure and magnetic behavior of Ni-Ir-based nanoparticles in ionic liquids. Phys Chem Chem Phys. 2018; 20(15):10247-10257. DOI: 10.1039/c8cp00164b. View

Vogel D, Spiel C, Schmid M, Stoger-Pollach M, Schlogl R, Suchorski Y . The Role of Defects in the Local Reaction Kinetics of CO Oxidation on Low-Index Pd Surfaces. J Phys Chem C Nanomater Interfaces. 2013; 117(23):12054-12060. PMC: 3683887. DOI: 10.1021/jp312510d. View

Chen K, Guo S, Liu H, Li X, Zhang Z, Lu T . Strong Visible-Light-Absorbing Cuprous Sensitizers for Dramatically Boosting Photocatalysis. Angew Chem Int Ed Engl. 2020; 59(31):12951-12957. DOI: 10.1002/anie.202003251. View

10.

Su , Cremer , Shen , Somorjai . Pressure Dependence (10(-10)-700 Torr) of the Vibrational Spectra of Adsorbed CO on Pt(111) Studied by Sum Frequency Generation. Phys Rev Lett. 1996; 77(18):3858-3860. DOI: 10.1103/PhysRevLett.77.3858. View

11.

Pramhaas V, Roiaz M, Bosio N, Corva M, Rameshan C, Vesselli E . Interplay between CO Disproportionation and Oxidation: On the Origin of the CO Reaction Onset on Atomic Layer Deposition-Grown Pt/ZrO Model Catalysts. ACS Catal. 2021; 11(1):208-214. PMC: 7783867. DOI: 10.1021/acscatal.0c03974. View

12.

Perdew , Burke , Ernzerhof . Generalized Gradient Approximation Made Simple. Phys Rev Lett. 1996; 77(18):3865-3868. DOI: 10.1103/PhysRevLett.77.3865. View

13.

Corva M, Ferrari A, Rinaldi M, Feng Z, Roiaz M, Rameshan C . Vibrational fingerprint of localized excitons in a two-dimensional metal-organic crystal. Nat Commun. 2018; 9(1):4703. PMC: 6224418. DOI: 10.1038/s41467-018-07190-1. View

14.

Symonds J, Arnolds H, Zhang V, Fukutani K, King D . Broadband femtosecond sum-frequency spectroscopy of CO on Ru1010 in the frequency and time domains. J Chem Phys. 2004; 120(15):7158-64. DOI: 10.1063/1.1669377. View

15.

KOCH , Borbonus , HAASE , RIEDER . New aspects on the Ir(110) reconstruction: Surface stabilization on mesoscopic scale via (331) facets. Phys Rev Lett. 1991; 67(24):3416-3419. DOI: 10.1103/PhysRevLett.67.3416. View

16.

Li X, Pramhaas V, Rameshan C, Blaha P, Rupprechter G . Coverage-Induced Orientation Change: CO on Ir(111) Monitored by Polarization-Dependent Sum Frequency Generation Spectroscopy and Density Functional Theory. J Phys Chem C Nanomater Interfaces. 2020; 124(33):18102-18111. PMC: 7444014. DOI: 10.1021/acs.jpcc.0c04986. View

17.

Yang T, Wang Y, Wei W, Ding X, He M, Yu T . Synthesis of octahedral Pt-Ni-Ir yolk-shell nanoparticles and their catalysis in oxygen reduction and methanol oxidization under both acidic and alkaline conditions. Nanoscale. 2019; 11(48):23206-23216. DOI: 10.1039/c9nr07235g. View

18.

Ng M, Abild-Pedersen F, Kaya S, Mbuga F, Ogasawara H, Nilsson A . Low Barrier Carbon Induced CO Dissociation on Stepped Cu. Phys Rev Lett. 2015; 114(24):246101. DOI: 10.1103/PhysRevLett.114.246101. View

19.

Anic K, Bukhtiyarov A, Li H, Rameshan C, Rupprechter G . CO Adsorption on Reconstructed Ir(100) Surfaces from UHV to mbar Pressure: A LEED, TPD, and PM-IRAS Study. J Phys Chem C Nanomater Interfaces. 2016; 120(20):10838-10848. PMC: 4885107. DOI: 10.1021/acs.jpcc.5b12494. View

20.

Li X, Roiaz M, Pramhaas V, Rameshan C, Rupprechter G . Polarization-Dependent SFG Spectroscopy of Near Ambient Pressure CO Adsorption on Pt(111) and Pd(111) Revisited. Top Catal. 2018; 61(9):751-762. PMC: 6010505. DOI: 10.1007/s11244-018-0949-7. View