Oxidative steam reforming of ethanol over MxLa2−xCe1.8Ru0.2O7−δ (M = Mg, Ca) catalysts: effect of alkaline earth metal substitution and support on stability and activity
| Autor: | Yu-Chun Chuang, Yuan Chia Chang, Ping Wen Tsai, Sheng Feng Weng, Hwo Shuenn Sheu, Chi Shen Lee, Ho Chen Hsieh |
|---|---|
| Rok vydání: | 2019 |
| Předmět: |
Alkaline earth metal
X-ray absorption spectroscopy Ethylene General Chemical Engineering Inorganic chemistry Oxide chemistry.chemical_element 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Oxygen 0104 chemical sciences Catalysis Steam reforming chemistry.chemical_compound chemistry 0210 nano-technology Hydrogen production |
| Zdroj: | RSC Advances. 9:39932-39944 |
| ISSN: | 2046-2069 |
| Popis: | Alkaline earth metal substitutions on the A-site of pyrochlore oxide MxLa2−xCe1.8Ru0.2O7−δ (M = Mg, Ca) were studied as catalyst materials for oxidative/autothermal steam reforming of ethanol (OSRE/ATR). The as-prepared oxides were synthesized by a combustion method and characterized using powder X-ray diffraction (PXRD), and X-ray photoelectron and absorption spectroscopy (XPS and XAS). PXRD Rietveld analysis and elemental analysis (ICP-AES) support the formation of a pyrochlore-type structure (space group Fdm) with a distorted coordination environment. The substitution of Mg2+ and Ca2+ ions affects the oxidation states of Ce4+/3+ and Run+ ions and creates oxygen vacancies, which leads to enhanced catalytic activity and reduced ethylene selectivity. A long-term stability test showed optimized catalysts Mg0.3La1.7Ce1.8Ru0.2O7−δ and Ca0.2La1.8Ce1.8Ru0.2O7−δ with SH2 = 101(1)% and SH2 = 91(2)% under OSRE conditions. The initial operation temperatures were lower than that of the unsubstituted catalyst La2Ce1.8Ru0.2O7−δ. Catalysts supported on La2Zr2O7 showed stable OSRE/ATR performance and low carbon deposition compared to catalysts supported on Al2O3. We ascribe the enhanced activity to well-dispersed alkaline earth metal and Ru ions in a solid solution structure, synergistic effects of (Mg, Ca)2+/Ce3+/4+/Run+ ions, and a strong catalyst–support interaction that optimized the ethanol conversion and hydrogen production. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|