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@ARTICLE{Schiller:620134,
      author       = {Schiller, Frederik and Ali, Khadiza and Makarova, Anna A.
                      and Auras, Sabine V. and Garcia Martinez, Fernando and
                      Mohammed Idris Bakhit, Alaa and Castrillo Bodero, Rodrigo
                      and Villar-García, Ignacio J. and Ortega, J. Enrique and
                      Pérez-Dieste, Virginia},
      title        = {{N}ear-{A}mbient {P}ressure {O}xidation of {S}ilver in the
                      {P}resence of {S}teps: {E}lectrophilic {O}xygen and {S}ulfur
                      {I}mpurities},
      journal      = {ACS catalysis},
      volume       = {14},
      number       = {17},
      issn         = {2155-5435},
      address      = {Washington, DC},
      publisher    = {ACS},
      reportid     = {PUBDB-2025-00051},
      pages        = {12865 − 12874},
      year         = {2024},
      abstract     = {The oxidation of Ag crystal surfaces has recently triggered
                      strong controversies around the presence of sulfur
                      impurities that may catalyze reactions, such as the alkene
                      epoxidations, especially the ethylene epoxidation. A
                      fundamental challenge to achieve a clear understanding is
                      the variety of procedures and setups involved as well as the
                      particular history of each sample. Especially, for the
                      often-used X-ray photoemission technique, product detection,
                      or photoemission peak position overlap are problematic. Here
                      we investigate the oxidation of the Ag(111) surface and its
                      vicinal crystal planes simultaneously, using a curved
                      crystal sample and in situ X-ray photoelectron spectroscopy
                      at 1 mbar O$_2$ near-ambient pressure conditions to further
                      investigate surface species. The curved geometry allows a
                      straightforward comparative analysis of the surface
                      oxidation kinetics at different crystal facets, so as to
                      precisely correlate the evolution of different oxygen
                      species, namely nucleophilic and electrophilic oxygen, and
                      the buildup of sulfur as a function of the crystal
                      orientation. We observed that emission from both surface and
                      bulk oxide contributes to the characteristic nucleophilic
                      oxygen core-level peak, which arises during oxygen dosing
                      and rapidly saturates below temperatures of 180 °C. The
                      electrophilic oxygen peak appears later, growing at a slower
                      but constant rate, at the expenses of the surface oxide.
                      Electrophilic oxygen and sulfur core-levels evolve in
                      parallel in all crystal facets, although faster and stronger
                      at vicinal surfaces featuring B-type steps with {111}
                      microfacets. Our study confirms the intimate connection of
                      the electrophilic species with the formation of adsorbed
                      SO$_4$, and points to a higher catalytic activity of B-type
                      stepped silver surfaces for alkene epoxidation or methane to
                      formaldehyde conversion.},
      cin          = {FS-PETRA-S},
      ddc          = {540},
      cid          = {I:(DE-H253)FS-PETRA-S-20210408},
      pnm          = {632 - Materials – Quantum, Complex and Functional
                      Materials (POF4-632) / CURVEO - Selective ethylene oxidation
                      on novel curved model catalysts (101066965)},
      pid          = {G:(DE-HGF)POF4-632 / G:(EU-Grant)101066965},
      experiment   = {EXP:(DE-MLZ)External-20140101},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {pmid:39263542},
      UT           = {WOS:001293062700001},
      doi          = {10.1021/acscatal.4c02985},
      url          = {https://bib-pubdb1.desy.de/record/620134},
}