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Theoretical Study of Carbon Adsorption on Re Surfaces: Morphological Instability

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Abstract

We report results from new experiments on C/Re(\(11\bar{2}1\)) to identify threshold conditions for morphological instability of Re(\(11\bar{2}1\)). We have found that adsorption of carbon from 0.35 to 0.85 ML (0.3–6.0 L exposure of C2H2) at T ≥ 800 K leads to faceting of Re(\(11\bar{2}1\)) with formation of three-sided pyramids. Using density functional theory we have investigated binding sites and binding energies of C on planar and faceted Re surfaces as well as generated a surface phase diagram of C/Re to obtain an atomistic understanding of C-induced pyramidal faceting of Re(\(11\bar{2}1\)). The calculations reveal that at low to intermediate coverage, C atoms prefer binding at four-fold sites on the Re surfaces and formation of three-sided pyramids is thermodynamically favored.

Graphical Abstract

Using density functional theory and thermodynamic considerations as well as AES and LEED measurements we studied the structure of Re(11–21) surfaces in contact with C2H2. The experiments show that adsorption of carbon from 0.35 to 0.85 ML (0.3–6.0 L exposure of C2H2) at T ≥ 800 K leads to faceting of Re(11–21) with formation of three-sided pyramids. The calculations reveal that at low to intermediate coverage, C atoms prefer binding at four-fold sites on the Re surfaces and formation of three-sided pyramids is thermodynamically favored.

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Acknowledgments

P. K. and T. J. gratefully acknowledge support from the “Bundesministerium für Bildung und Forschung” (BMBF) and the bw-grid for computing resources. Further, support by the Deutsche Forschungsgemeinschaft (DFG) (Grant Nos. JA1072/9-2 and KO 576/28-1) as well as by the European Research Council (ERC-StG THEOFUN, Grant Agreement No. 259608) is gratefully acknowledged. B.E.K. acknowledges support of this work by the National Science Foundation (Grant No. CHE-1129417). W.C. and R.A.B. acknowledge support of this work by the U.S. Department of Energy, Office of Basic Energy Sciences (Grant No. DE-FG02-93ER14331).

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Correspondence to Payam Kaghazchi or Wenhua Chen.

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Kaghazchi, P., Jacob, T., Yang, X. et al. Theoretical Study of Carbon Adsorption on Re Surfaces: Morphological Instability. Catal Lett 144, 1667–1673 (2014). https://doi.org/10.1007/s10562-014-1324-3

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  • DOI: https://doi.org/10.1007/s10562-014-1324-3

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