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1 DOI: /NCHEM.1245 Non-lattice surface oxygen species implicated in the catalytic partial oxidation of decane to oxygenated aromatics Sivaram Pradhan, Jonathan K. Bartley, Donald Bethell, Albert F. Carley, Marco Conte, Stan Golunski, Matthew P. House, Robert L. Jenkins, Rhys Lloyd and Graham J. Hutchings* Cardiff Catalysis Institute, School of Chemistry, Cardiff University, CF10 3AT, UK Contents Figure S1: TPR of iron molybdate catalyst Table S1: Surface analysis (atomic composition) of iron molybdate catalyst by XPS Table S2: Estimation of lattice oxygen consumed during reaction Table S3: Crystalline phase composition of iron molybdate catalyst Table S4: BET surface area of iron molybdate catalyst after different pre-treatments Table S5: Product speciation NATURE CHEMISTRY 1

2 Figure S1: TPR of iron molybdate catalyst Measured TPR profile: Interpretation of TPR profile: Reduction peak Measured peak temperature ( o C) Reported [22] peak temperature ( o C) Phases formed [ref 22 in manuscript] As prepared Fe 2 (MoO 4 ) 3 and MoO MoO 3, α- FeMoO 4, β-femoo 4, Mo 4 O MoO 2, α- FeMoO 4, β-femoo 4, Mo 4 O MoO 2, Fe 3 O 4, Fe 2 Mo 3 O 8, α- FeMoO 4, β-femoo MoO 2, Fe 3 O 4, Fe 2 Mo 3 O 8, Fe 3 Mo (minor) 5 > Mo o, Fe 3 Mo alloy NATURE CHEMISTRY 2

3 Table S1: Surface analysis (atomic composition) of iron molybdate catalyst by XPS Pre-treatment % Fe % Mo % O Fe/Mo Mo/Fe None (as prepared) ºC / 12 h oxidative reaction ºC / 12 h oxidative reaction / 12 reaction without O ºC / 12 h oxidative reaction / 12 reaction without O 2 / 12 h oxidative reaction Table S2: Estimation of lattice oxygen consumed during reaction NATURE CHEMISTRY 3

4 Table S3: Crystalline phase composition of iron molybdate catalyst Pre-treatment Fe 2 (MoO 4 ) 3 MoO 3 FeMoO 4 MoO 2 Mo 4 O 11 (wt %) (wt %) (wt %) (wt %) (wt %) None (as prepared) C / 12 h oxidative reaction C / 12 h oxidative reaction / 12h reaction without O C / 12 h oxidative reaction / 12h without O 2 / 12 h with O 2 restored C / 12 h oxidative reaction conditions C / 12 h oxidative reaction / 12h reaction without O C / 12 h oxidative reaction / 12h without O 2 / 12 h with O 2 restored Table S4: BET surface area of iron molybdate catalyst after different pre-treatments Pre-treatment Surface area (m 2 g -1 ) None (as prepared) C / 12 h oxidative reaction C / 12 h oxidative reaction / 12h reaction without O C / 12 h oxidative reaction conditions C / 12 h oxidative reaction / 12h reaction without O 2 22 NATURE CHEMISTRY 4

5 Table S5: Product speciation Conversion and selectivity of n-decane during oxidative reaction in blank reactor, 0.80% n-decane, C:O = 14.8:1 Selectivity (%) Temp ( o C) C (%) C 1 -C 7 Decene Oxygenated aromatics Others CO CO Conversion and selectivity of n-decane during oxidative reaction over iron molybdate catalyst, 1% n-decane, C:O = 11.8:1. Temperature (ºC) Conversion (%) Ethane/ene Propane/ene Butane Pentane Hexane Methanol Propanol Butanol Pentanol Pentanoic Acid Decene Phthalic Anhydride Coumarin Napthol Fluorenone Xanthone Napthalene Ethyl Napthalene Fluorene C 10 Aromatics( All having Molecular weight 132) Other C 10 Aromatic Oxygenates CO CO C Balance (%) NATURE CHEMISTRY 5

6 Conversion and selectivity of n-decane during oxidative reaction over iron molybdate catalyst at 460 C, 0.92% n-decane,c:o = 11.7:1. Time (h) Conversion (%) Methane Ethane/ene Propane/ene Butane Pentane Hexane Heptane Octane Methanol Propanol Butanone Propionic Acid Pentanol Pentanoic Acid Hexanol Hexanoic Acid Heptanol Decene Toluene Styrene Phthalic Anhydride Indanone Coumarin Napthol Fluorenone Xanthone Napthalene Ethyl Napthalene C 10 Aromatics( All having Molecular weight 132) Other C 10 Aromatic Oxygenates CO CO C Balance (%) NATURE CHEMISTRY 6

7 Conversion and selectivity of n-decane during oxidative reaction over iron molybdate catalyst at 460 C, 0.92% n-decane. Time (h) Conversion (%) Methane Ethane/ene Propane/ene Butane Pentane Hexane Heptane Octane Methanol Propanol Propionic Acid Pentanol Pentanoic Acid Hexanone Heptanone Decene Toluene Styrene Napthalene C 10 Aromatics( All having Molecular weight 132) C Balance (%) NATURE CHEMISTRY 7

8 Conversion and selectivity of n-decane during oxidative reaction after 12 h under aerobic conditions then 12 h under anaerobic conditions over iron molybdate catalyst at 460 C, C:O = 11.7:1, 0.92% n-decane Time (h) Conversion (%) Methane Ethane/ene Propane/ene Butane Pentane Hexane Heptane Octane Methanol Propanol Butanol Propionic Acid Pentanol Pentanoic Acid Hexanoic Acid Heptanone Decene Toluene Styrene Phthalic Anhydride Indanone Coumarin Napthol Fluorenone Xanthone Napthalene Ethyl Napthalene C 10 Aromatics( All having Molecular weight 132) Other C 10 Aromatic Oxygenates CO CO C Balance (%) NATURE CHEMISTRY 8

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