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Catalytic properties of Sr1−xCexWO4: The role of mixed conduction in methane oxidation
International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2018-07-12 , DOI: 10.1016/j.ijhydene.2018.06.143
Rafael Hernandez Damascena dos Passos , Carlson Pereira de Souza , Christine Leroux , Madjid Arab

The catalytic efficiency of ternary strontium cerium tungstate Sr0.5Ce0.35WO4, for the production of syngas through methane oxidation, was investigated and compared to those of binary strontium tungstate SrWO4. Total and partial oxidation reactions were observed for both samples in the temperature range 600–750 °C under CH4/dry air flux. At high CH4 concentration and low temperature with the ternary tungstate as catalyst, the partial oxidation, leading to CO/H2, prevails. This indicates the potentiality of the new strontium cerium tungstate scheelite compound for the catalysis of CH4. Sr0.5Ce0.35WO4 and SrWO4 exhibit different conduction mechanisms. Conduction in the binary compound is related to the overlapping large polaron tunneling model, whereas conduction in the ternary one is due to a correlated barrier hopping phenomenon. The activation energies, in the low temperature range where the partial oxidation occurs, are significantly lower for the ternary compound than for the binary one. These electrical tendencies favor both partial and total oxidation of methane. The correlated barrier hopping conduction in the ternary compound leads to a better partial oxidation rate than conduction through large polaron tunneling.



中文翻译:

Sr 1-x Ce x WO 4的催化性质:混合传导在甲烷氧化中的作用

研究了钨酸锶锶锶Sr 0.5 Ce 0.35 WO 4通过甲烷氧化生产合成气的催化效率,并与二元钨酸锶锶SrWO 4进行了比较。在CH 4 /干燥空气通量下,在600–750°C的温度范围内,两个样品均观察到全部和部分氧化反应。在高CH 4浓度和低温下,以三价钨酸盐为催化剂,普遍存在导致CO / H 2的部分氧化。这表明新的钨酸锶铈钨白钨化合物具有催化CH 4的潜力。Sr 0.5 Ce0.35 WO 4和SrWO 4表现出不同的传导机制。二元化合物中的传导与重叠的大极化子隧穿模型有关,而三元化合物中的传导归因于相关的势垒跳跃现象。在发生部分氧化的低温范围内,三元化合物的活化能明显低于二元化合物。这些电趋势有利于甲烷的部分和全部氧化。三元化合物中的相关势垒跳跃传导比通过大极化子隧穿的传导导致更好的部分氧化速率。

更新日期:2018-07-12
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