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000875191 1001_ $$0P:(DE-HGF)0$$aLiu, Zongyuan$$b0
000875191 245__ $$aWater-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst
000875191 260__ $$aCambridge, Mass.$$bMoses King$$c2020
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000875191 520__ $$aHighly 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.
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000875191 7001_ $$00000-0003-2690-3788$$aHuang, Erwei$$b1
000875191 7001_ $$00000-0003-0866-1615$$aOrozco, Ivan$$b2
000875191 7001_ $$00000-0001-5095-4409$$aLiao, Wenjie$$b3
000875191 7001_ $$00000-0003-4476-3512$$aPalomino, Robert M.$$b4
000875191 7001_ $$00000-0001-6234-7075$$aRui, Ning$$b5
000875191 7001_ $$0P:(DE-Juel1)165376$$aDuchoň, Thomas$$b6
000875191 7001_ $$0P:(DE-Juel1)164137$$aNemšák, Slavomir$$b7
000875191 7001_ $$00000-0001-6089-119X$$aGrinter, David C.$$b8
000875191 7001_ $$00000-0002-7544-9457$$aMahapatra, Mausumi$$b9
000875191 7001_ $$00000-0001-8363-070X$$aLiu, Ping$$b10$$eCorresponding author
000875191 7001_ $$0P:(DE-HGF)0$$aRodriguez, José A.$$b11$$eCorresponding author
000875191 7001_ $$0P:(DE-HGF)0$$aSenanayake, Sanjaya D.$$b12$$eCorresponding author
000875191 773__ $$0PERI:(DE-600)2066996-3$$a10.1126/science.aba5005$$gVol. 368, no. 6490, p. 513 - 517$$n6490$$p513 - 517$$tScience$$v368$$x0036-8075$$y2020
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