Department of Chemistry and Applied Biosciences, ETH Zürich, Hönggerberg-HCI, CH-8093 Zürich, Switzerland.
Phys Chem Chem Phys. 2010 Mar 14;12(10):2288-91. doi: 10.1039/b924001b. Epub 2010 Feb 8.
Pd/Al(2)O(3) catalysts showed an oscillatory behaviour during the catalytic partial oxidation (CPO) of methane, which was investigated simultaneously by IR-thermography, X-ray absorption spectroscopy, and online mass-spectrometry to correlate the temperature, state of the catalyst and catalytic performance. The following stages were observed: (i) build-up of a temperature maximum in the first half of the catalyst bed, (ii) reduction of palladium in the end zone of the catalyst bed with a front moving toward the entrance zone, (iii) strong hot spot formation accompanied by reduction of palladium due to self-reduction leading to extinction of the process. The latter was the key driver for the oscillations and thus gave additional insight into the mechanism of partial methane oxidation.
Pd/Al(2)O(3) 催化剂在甲烷的催化部分氧化 (CPO) 过程中表现出振荡行为,通过红外热成像、X 射线吸收光谱和在线质谱法同时进行研究,以将温度、催化剂状态和催化性能相关联。观察到以下阶段:(i) 催化剂床的前半部分温度达到最大值,(ii) 钯在催化剂床的末端区域还原,前沿向入口区域移动,(iii) 由于自还原导致钯的强烈热点形成和还原,从而导致过程终止。后者是振荡的关键驱动因素,因此为部分甲烷氧化的机制提供了更多的见解。