Interaction of sulfur dioxide and near-ambient pressures of water vapor with cuprous oxide surfaces

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Interaction of sulfur dioxide and near-ambient pressures of water vapor with cuprous oxide surfaces. / Soldemo, Markus; Stenlid, Joakim Halldin; Besharat, Zahra; Johansson, Niclas; Önsten, Anneli; Knudsen, Jan; Schnadt, Joachim; Göthelid, Mats; Brinck, Tore; Weissenrieder, Jonas.

In: Journal of Physical Chemistry C, Vol. 121, No. 43, 2017, p. 24011–24024.

Research output: Contribution to journalArticle

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Soldemo, M, Stenlid, JH, Besharat, Z, Johansson, N, Önsten, A, Knudsen, J, Schnadt, J, Göthelid, M, Brinck, T & Weissenrieder, J 2017, 'Interaction of sulfur dioxide and near-ambient pressures of water vapor with cuprous oxide surfaces' Journal of Physical Chemistry C, vol 121, no. 43, pp. 24011–24024. DOI: 10.1021/acs.jpcc.7b06486

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Soldemo, Markus; Stenlid, Joakim Halldin; Besharat, Zahra; Johansson, Niclas; Önsten, Anneli; Knudsen, Jan; Schnadt, Joachim; Göthelid, Mats; Brinck, Tore; Weissenrieder, Jonas / Interaction of sulfur dioxide and near-ambient pressures of water vapor with cuprous oxide surfaces.

In: Journal of Physical Chemistry C, Vol. 121, No. 43, 2017, p. 24011–24024.

Research output: Contribution to journalArticle

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TY - JOUR

T1 - Interaction of sulfur dioxide and near-ambient pressures of water vapor with cuprous oxide surfaces

AU - Soldemo,Markus

AU - Stenlid,Joakim Halldin

AU - Besharat,Zahra

AU - Johansson,Niclas

AU - Önsten,Anneli

AU - Knudsen,Jan

AU - Schnadt,Joachim

AU - Göthelid,Mats

AU - Brinck,Tore

AU - Weissenrieder,Jonas

PY - 2017

Y1 - 2017

N2 - The interaction of water vapor and sulfur dioxide (SO2) with single crystal cuprous oxide (Cu2O) surfaces of (100) and (111) termination was studied by photoelectron spectroscopy (PES) and density functional theory (DFT). Exposure to near-ambient pressures of water vapor, at 5 × 10-3 %RH and 293 K, hydroxylates both Cu2O surfaces with OH coverage up to 0.38 copper monolayers (ML) for (100) and 0.25 ML for (111). O 1s surface core level shifts indicate that the hydroxylation lifts the (3,0;1,1) reconstruction of the clean (100) surface. On both clean Cu2O terminations, SO2 adsorbs to unsaturated surface oxygen atoms to form SO3 species with coverage, after a saturating SO2 dose, corresponding to 0.20 ML on the Cu2O(100) surface and 0.09 ML for the Cu2O(111) surface. Our combined DFT and PES results suggest that the SO2 to SO3 transformation is largely facilitated by unsaturated copper atoms at the Cu2O(111) surface. SO3-terminated surfaces exposed to low doses of water vapor (=100 langmuirs) in ultrahigh vacuum show no adsorption or reaction. However, during exposure to near-ambient pressures of water vapor, the SO3 species dissociate, and sulfur replaces a Cu2O lattice oxygen in a reaction that forms Cu2S. The hydroxylation of the Cu2O surfaces is believed to play a central role in the reaction.

AB - The interaction of water vapor and sulfur dioxide (SO2) with single crystal cuprous oxide (Cu2O) surfaces of (100) and (111) termination was studied by photoelectron spectroscopy (PES) and density functional theory (DFT). Exposure to near-ambient pressures of water vapor, at 5 × 10-3 %RH and 293 K, hydroxylates both Cu2O surfaces with OH coverage up to 0.38 copper monolayers (ML) for (100) and 0.25 ML for (111). O 1s surface core level shifts indicate that the hydroxylation lifts the (3,0;1,1) reconstruction of the clean (100) surface. On both clean Cu2O terminations, SO2 adsorbs to unsaturated surface oxygen atoms to form SO3 species with coverage, after a saturating SO2 dose, corresponding to 0.20 ML on the Cu2O(100) surface and 0.09 ML for the Cu2O(111) surface. Our combined DFT and PES results suggest that the SO2 to SO3 transformation is largely facilitated by unsaturated copper atoms at the Cu2O(111) surface. SO3-terminated surfaces exposed to low doses of water vapor (=100 langmuirs) in ultrahigh vacuum show no adsorption or reaction. However, during exposure to near-ambient pressures of water vapor, the SO3 species dissociate, and sulfur replaces a Cu2O lattice oxygen in a reaction that forms Cu2S. The hydroxylation of the Cu2O surfaces is believed to play a central role in the reaction.

U2 - 10.1021/acs.jpcc.7b06486

DO - 10.1021/acs.jpcc.7b06486

M3 - Article

VL - 121

SP - 24011

EP - 24024

JO - Journal of Physical Chemistry C

T2 - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 43

ER -