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How Do Structurally Distinct Au/α‐Fe 2 O 3 Interfaces Determine Surface OH/H 2 O reactivity, Intermediate Evolution, and Product Formation in Low‐temperature Water‐gas Shift Reaction?
Author(s) -
Gu Lingli,
Zeng Yiqiang,
Feng Yina,
Jiang Wu,
Ji Weijie,
Arandiyan Hamidreza,
Au ChakTong
Publication year - 2019
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201900576
Subject(s) - reactivity (psychology) , chemistry , adsorption , catalysis , x ray photoelectron spectroscopy , reaction intermediate , oxygen , substrate (aquarium) , crystallography , chemical engineering , organic chemistry , medicine , oceanography , alternative medicine , pathology , engineering , geology
Three structurally distinct interfaces, i. e. Au/α‐Fe 2 O 3 ‐THB‐Air, Au/α‐Fe 2 O 3 ‐HS‐Air, and Au/α‐Fe 2 O 3 ‐QC‐Air, with the major substrate facet being {113}, {001}, and {012} respectively, were controllably prepared. The low temperature water gas shift (WGS) reaction (100–260 °C) was applied to these unique systems to reveal how these structurally distinct interfaces can impact on the reaction behavior. With the detailed performance evaluation plus the characterizations of CO‐TPSR, XPS, and in situ‐FTIR in particular, the correlations between the evolution of different intermediates and the distinct catalytic behaviors have been established. The substrate facet structure and the Au entity largely determine the form and reactivity of surface OH/H 2 O species which in turn determine the formation of different intermediates and eventually the product formation. The Au/α‐Fe 2 O 3 ‐THB‐Air is enriched with oxygen vacant sites, favorable for dissociative adsorption of H 2 O, carboxyl intermediate formation and H 2 production. The Au/α‐Fe 2 O 3 ‐HS‐Air is enriched with surface lattice oxygen, favorable for molecular adsorption of H 2 O, formate intermediate formation, and CO 2 production. The Au/α‐Fe 2 O 3 ‐QC‐Air interface is enriched with surface Fe sites, favorable for dissociative adsorption of H 2 O and evolution of stable carboxyl intermediate as well as isolated OH species at low reaction temperatures. The findings are informative to control the interfacial structure for the WGS and other reactions.