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On the contribution of oxygen from Co3O4 to the Pd-catalyzed methane combustion
Catalysis Today ( IF 5.3 ) Pub Date : 2019-12-27 , DOI: 10.1016/j.cattod.2019.12.041
Jing Shen , Robert E. Hayes , Natalia Semagina

The high oxygen storage capacity of exhaust gas treatment catalysts is a desirable feature for stabilizing fuel conversion at lambda variations for stoichiometric engine performance. Pd catalysts supported on Co3O4, Al2O3, CeO2 and ZrO2, as well as Pd-free Co3O4, were evaluated using methane combustion at sub-stoichiometric oxygen-to-fuel ratios at temperatures below 550 °C. The product analysis was performed with an online mass spectrometer calibrated for CH4, O2, CO2, H2O, CO and H2. Only both cobalt catalysts demonstrated the insensitivity of the methane conversion to O2/CH4 variations. The Pd/Co3O4 catalyst was the only catalyst that produced a 40 % increase in exit gas flow above the feed gas mass flow rate at ignition (light-off) between 400 °C and 550 °C, with the same decrease upon extinction. The oxygen from the catalyst participated in the combustion, even while the molecular oxygen supplies lasted. Selected catalysts were analyzed by temperature-programmed desorption, reduction in H2 and surface reaction with CH4. In the absence of O2 in the feed, Pd/Co3O4 supplied a “tithe” of its bulk oxygen at temperatures of 400−550 °C for the formation of CO2 and H2O, while Pd/Al2O3 provided only PdO-associated low oxygen for the CO and H2 formation. Co3O4 surpasses CeO2 in its oxygen-donating properties at low temperatures and at the conditions tested and, thus, is potentially capable of widening the operational lambda window of stoichiometric combustion to a larger extent than ceria.



中文翻译:

Co 3 O 4中氧气对Pd催化甲烷燃烧的贡献

排气处理催化剂的高储氧能力是在化学计量的发动机性能下以λ变化稳定燃料转化率的理想特征。在低于550的温度下使用亚化学计量的氧/燃料比燃烧甲烷,评估了负载在Co 3 O 4,Al 2 O 3,CeO 2和ZrO 2上的Pd催化剂以及不含Pd的Co 3 O 4。 ℃。使用在线质谱仪对CH 4,O 2,CO 2,H 2 O,CO和H 2进行校准,对产品进行分析。仅两种钴催化剂均显示甲烷转化为O 2 / CH 4变化的不敏感性。Pd / Co 3 O 4催化剂是唯一在400°C至550°C之间着火(起燃)时,进料气质量流速以上,出气量增加40%的催化剂,当温度升高时,出气量增加40%灭绝。即使分子氧供应持续,来自催化剂的氧气也参与了燃烧。通过程序升温脱附,H 2还原和与CH 4的表面反应来分析选定的催化剂。在进料中没有O 2的情况下,Pd / Co 3 O 4在400-550°C的温度下,其供应的大量氧气“滴定”以形成CO 2和H 2 O,而Pd / Al 2 O 3仅提供了与PdO相关的低氧来形成CO 2和H 2。在低温和测试条件下,Co 3 O 4的供氧性能超过了CeO 2,因此,与二氧化铈相比,Co 3 O 4有可能在更大的程度上扩大化学计量燃烧的操作λ窗口。

更新日期:2019-12-27
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