Dry reforming activity due to ionic Ru in La1.99Ru0.01O3: the role of specific carbonates
| Autor: | Phanikumar Pentyala, Krishanu Biswas, Bhanu P. Gangwar, Sudhanshu Sharma, Parag A. Deshpande, Khushubo Tiwari |
|---|---|
| Rok vydání: | 2019 |
| Předmět: |
Carbon dioxide reforming
Doping Inorganic chemistry General Physics and Astronomy Ionic bonding chemistry.chemical_element 02 engineering and technology Active surface 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Oxygen Methane 0104 chemical sciences Catalysis chemistry.chemical_compound chemistry Carbonate Physical and Theoretical Chemistry 0210 nano-technology |
| Zdroj: | Physical Chemistry Chemical Physics. 21:16726-16736 |
| ISSN: | 1463-9084 1463-9076 |
| DOI: | 10.1039/c9cp02337b |
| Popis: | Dry reforming of methane was carried out over La2−2xRu2xO3 (x = 0.005, 0.01). Substitution of just 0.5 atom% of Ru in La2O3 enhanced the activity by 20 times in terms of conversion when compared to the activity exhibited by La2O3. The oxygen storage capacity of the Ru doped sample was considerably higher than undoped La2O3, which resulted in higher conversions of CH4 and CO2. The measured conversion of CH4 and CO2 was 72 and 80%, respectively, at 850 °C. The same was merely 4% with La2O3 under the same experimental conditions. DRIFTS studies demonstrated the role of a specific type of carbonates in promoting the activity of the catalyst. DFT calculations provided the rationale behind the selection of the Ru-in-La2O3 methane dry reforming catalyst. The surface structures of the pure and Ru-substituted compounds were determined, corroborating the experimental observation of enhanced oxygen storage capacity on Ru substitution. Different active surface oxygen species were identified and their roles in improving reducibilities and improving reactivities were established. The experimentally observed surface carbonate species were also identified using calculations. The combined experiment + calculation approach proved ionic Ru in La2−2xRu2xO3 to be a novel and efficient dry reforming catalyst. |
| Databáze: | OpenAIRE |
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