Efficient and selective photocatalytic CH4 conversion to CH3OH with O2 by controlling overoxidation on TiO2
| Autor: | Feng Deng, Huiwen Lin, Ningdong Feng, Jinhua Ye, Dai-Ming Tang, Longxiao Yang, Hui Song |
|---|---|
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Materials science
Science General Physics and Astronomy chemistry.chemical_element 02 engineering and technology 010402 general chemistry Photochemistry 01 natural sciences Oxygen General Biochemistry Genetics and Molecular Biology law.invention chemistry.chemical_compound law Fourier transform infrared spectroscopy Electron paramagnetic resonance Nanosheet Multidisciplinary General Chemistry 021001 nanoscience & nanotechnology 0104 chemical sciences chemistry Yield (chemistry) Photocatalysis Methanol 0210 nano-technology Selectivity |
| Zdroj: | Nature Communications, Vol 12, Iss 1, Pp 1-10 (2021) |
| ISSN: | 2041-1723 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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