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Efficient and selective photocatalytic CH₄ conversion to CH₃OH with O₂ by controlling overoxidation on TiO₂.

ABSTRACT: The conversion of photocatalytic methane into methanol in high yield with selectivity remains a huge challenge due to unavoidable overoxidation. Here, the photocatalytic oxidation of CH₄ into CH₃OH by O₂ is carried out on Ag-decorated facet-dominated TiO₂. The {001}-dominated TiO₂ shows a durable CH₃OH yield of 4.8 mmol g^-1 h^-1 and a selectivity of approximately 80%, which represent much higher values than those reported in recent studies and are better than those obtained for {101}-dominated TiO₂. Operando Fourier transform infrared spectroscopy, electron spin resonance, and nuclear magnetic resonance techniques are used to comprehensively clarify the underlying mechanism. The straightforward generation of oxygen vacancies on {001} by photoinduced holes plays a key role in avoiding the formation of •CH₃ and •OH, which are the main factors leading to overoxidation and are generally formed on the {101} facet. The generation of oxygen vacancies on {001} results in distinct intermediates and reaction pathways (oxygen vacancy → Ti-O₂^• → Ti-OO-Ti and Ti-(OO) → Ti-O^• pairs), thus achieving high selectivity and yield for CH₄ photooxidation into CH₃OH.

SUBMITTER: Feng N

PROVIDER: S-EPMC8329221 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:TiO2 nanofibers were fabricated by combination of sol-gel and electrospinning techniques. Ag-doped TiO2 nanofibers with different Ag contents were prepared by two different methods (in situ electrospinning or wetness impregnation of Ag on TiO2 nanofibers) and heat treated at 500 °C for 2 h under an air or N2 atmosphere. The obtained catalysts were characterized by field emission scanning electron microscopy, X-ray diffraction, photoluminescence, and N2 adsorption analyzed by the Brunauer-Emmett-Teller (BET) method. Photocatalytic glucose conversions with electrospun TiO2 and Ag-doped TiO2 nanofibers for production of high-value products were carried out. From different doping methods, the results indicated that 1 wt % Ag-TiO2 nanofibers prepared by an in situ method with calcination under N2 achieved the highest glucose conversion (85.49%). From several Ag loading contents (i.e., 0, 1, 2, and 4 wt %) in Ag-doped TiO2 nanofibers, the nanofibers exhibited different glucose conversions [in order of 2 wt % (99.65%) > 1 wt % (85.49%) > 4 wt % (77.72%) > 0 wt % (29.64%)]. Arabinose, xylitol, gluconic acid, and formic acid were found as the high-value chemicals with the photocatalytic reaction of TiO2 and Ag-doped TiO2 nanofibers under UVA irradiation. Product yields of each converted chemicals from different photocatalysts from different Ag loading contents showed relatively same trends with the glucose conversion. From all results, it can be concluded that the good characteristics of 2 wt % Ag-TiO2 nanofibers such as the smallest anatase crystallite size (8.25 nm) and the highest specific surface area (S BET = 53.69 m2/g) promoted the highest photocatalytic activity. Additionally, TiO2 and Ag-doped TiO2 nanofibers exhibited higher photocatalytic performance for glucose conversion than commercial TiO2 (P25) and synthesized TiO2 nanoparticles. Finally, Ag-doped TiO2 nanofibers showed recycling ability with high photocatalytic glucose conversion after four-time use.

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Efficient and selective photocatalytic CH₄ conversion to CH₃OH with O₂ by controlling overoxidation on TiO₂.

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