Selective photooxidation of methane to C1 oxygenates by constructing heterojunction photocatalyst with mild oxidation ability

doi:10.1016/S1872-2067(24)60136-1

Abstract

Abstract:

Selective photocatalytic aerobic oxidation of methane to value-added chemicals offers a promising pathway for sustainable chemical industry, yet remains a huge challenge owing to the consecutive overoxidation of primary products. Here, a type II heterojunction were constructed in Ag-AgBr/ZnO to reduce the oxidation potential of stimulated holes and prevent the undesirable CH₄ overoxidation side reactions. For photocatalytic oxidation of methane under ambient temperature, the products yield of 1499.6 μmol g_cat^-1 h^-1 with a primary products selectivity of 77.9% was achieved over Ag-AgBr/ZnO, which demonstrate remarkable improvement compared to Ag/ZnO (1089.9 μmol g_cat^-1 h^-1, 40.1%). The superior activity and selectivity result from the promoted charge separation and the redox potential matching with methane activation after introducing AgBr species. Mechanism investigation elucidated that the photo-generated holes transferred from the valence band of ZnO to that of AgBr, which prevent H₂O oxidation and enhance the selective generation of •OOH radical.

Key words: Selective methane oxidation, Photocatalysis, Heterojunction, Ag-AgBr/ZnO catalyst

Hantao Gong, Caihao Deng, Peipei He, Mingjie Liu, Yiliang Cai, Yiwen Yang, Qiwei Yang, Zongbi Bao, Qilong Ren, Siyu Yao, Zhiguo Zhang. Selective photooxidation of methane to C1 oxygenates by constructing heterojunction photocatalyst with mild oxidation ability[J]. Chinese Journal of Catalysis, 2024, 67: 61-70.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60136-1

https://www.cjcatal.com/EN/Y2024/V67/I12/61

Figures/Tables 5

Fig. 1. Performances evaluation of selective photocatalytic oxidation of methane. (a) catalytic performances of ZnO, Ag/ZnO and a series of Ag-X/ZnO catalysts (AgX = AgCl, AgBr AgI, Ag2WO4, Ag2MoO4, Ag3PO4). (b) Influence of Ag loadings on the photocatalytic methane oxidation reaction over Ag-AgBr/ZnO catalysts. (c) Influence of light source on the photocatalytic methane oxidation reaction.

Fig. 2. (a) XRD spectra of Ag/ZnO and Ag-AgBr/ZnO with different loadings. (b) UV-vis DRS spectra of ZnO, Ag/ZnO and Ag-AgBr/ZnO. HR-TEM (c,d), HADDF (e) and EDX mapping images (f) of Ag-AgBr/ZnO.

Fig. 3. (a) PL spectra of ZnO, Ag/ZnO and Ag-AgBr/ZnO. (b) Photocurrent measurement with ZnO, Ag/ZnO and Ag-AgBr/ZnO as catalysts under light irradiation. Transformed Kubelka-Munk function (c) and XPS valence spectra (d) of AgBr and ZnO. (e) Band structure of ZnO, AgBr, AgCl, AgI, Ag2WO4, Ag2MoO4 and Ag3PO4 catalysts determined by XPS valence spectra and Mott-Schottky plots.

Fig. 4. (a) EPR spectra of ZnO, Ag/ZnO and Ag-AgBr/ZnO under light irradiation for 5 min under O2 dissolved in methanol (left) and O2 dissolved in water (right). DMPO was added to the solution as the radical trapping agent. (b) Intensity of double integral of DMPO-OOH and DMPO-OH in EPR spectra. (c) Product yields after adding scavengers in reaction system for trapping h+, e-, •OH and •OOH, respectively. (d) HCHO yield of photocatalytic oxidation of methanol over Ag/ZnO and Ag-AgBr/ZnO catalysts (10 mg catalyst, 10 mL water, 0.2 μmol CH3OH, 25 ± 3 °C reaction temperature, light source: 300 W Xe lamp (300-1100 nm, light intensity 200 mW cm−2)). In situ DRIFTS spectra for CH4 photooxidation over Ag/ZnO (e) and Ag-AgBr/ZnO (f) during light irradiation time from 1 to 30 min.

Fig. 5. Proposed catalytic mechanism of photocatalytic methane conversion over Ag-AgBr/ZnO.

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