TY  - JOUR
AU  - Liu, Zongyuan
AU  - Huang, Erwei
AU  - Orozco, Ivan
AU  - Liao, Wenjie
AU  - Palomino, Robert M.
AU  - Rui, Ning
AU  - Duchoň, Thomas
AU  - Nemšák, Slavomir
AU  - Grinter, David C.
AU  - Mahapatra, Mausumi
AU  - Liu, Ping
AU  - Rodriguez, José A.
AU  - Senanayake, Sanjaya D.
TI  - Water-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst
JO  - Science
VL  - 368
IS  - 6490
SN  - 0036-8075
CY  - Cambridge, Mass.
PB  - Moses King
M1  - FZJ-2020-01861
SP  - 513 - 517
PY  - 2020
AB  - Highly selective oxidation of methane to methanol has long been challenging in catalysis. Here, we reveal key steps for the pro­motion of this reaction by water when tuning the selectivity of a well-defined CeO2/Cu2O/Cu(111) catalyst from carbon monoxide and carbon dioxide to methanol under a reaction environment with methane, oxygen, and water. Ambient-pressure x-ray photoelectron spectroscopy showed that water added to methane and oxygen led to surface methoxy groups and accelerated methanol production. These results were consistent with density functional theory calculations and kinetic Monte Carlo simulations, which showed that water preferentially dissociates over the active cerium ions at the CeO2–Cu2O/Cu(111) interface. The adsorbed hydroxyl species blocked O-O bond cleavage that would dehydrogenate methoxy groups to carbon monoxide and carbon dioxide, and it directly converted this species to methanol, while oxygen reoxidized the reduced surface. Water adsorption also displaced the produced methanol into the gas phase.
LB  - PUB:(DE-HGF)16
C6  - pmid:32355028
UR  - <Go to ISI:>//WOS:000531178400045
DO  - DOI:10.1126/science.aba5005
UR  - https://juser.fz-juelich.de/record/875191
ER  -