Hydrogen production from a combination of the water-gas shift and redox cycle process of methane partial oxidation via lattice oxygen over LaFeO3 perovskite catalyst | |
Dai, Xiao Ping; Wu, Qiong; Li, Ran Jia; Yu, Chang Chun; Hao, Zheng Ping | |
刊名 | JOURNAL OF PHYSICAL CHEMISTRY B |
2006 | |
卷号 | 110期号:51页码:25856-25862 |
英文摘要 | A redox cycle process, in which CH4 and air are periodically brought into contact with a solid oxide packed in a fixed-bed reactor, combined with the water-gas shift (WGS) reaction, is proposed for hydrogen production. The sole oxidant for partial oxidation of methane (POM) is found to be lattice oxygen instead of gaseous oxygen. A perovskite-type LaFeO3 oxide was prepared by a sol-gel method and employed as an oxygen storage material in this process. The results indicate that, under appropriate reaction conditions, methane can be oxidized to CO and H-2 by the lattice oxygen of LaFeO3 perovskite oxide with a selectivity higher than 95% and the consumed lattice oxygen can be replenished in a reoxidation procedure by a redox operation. It is suggested that the POM to H-2/CO by using the lattice oxygen of the oxygen storage materials instead of gaseous oxygen should be possibly applicable. The LaFeO3 perovskite oxide maintained relatively high catalytic activity and structural stability, while the carbonaceous deposits, which come from the dissociation of CH4 in the pulse reaction, occurred due to the low migration rate of lattice oxygen from the bulk toward the surface. A new dissociation-oxidation mechanism for this POM without gaseous oxygen is proposed based on the transient responses of the products checked at different surface states via both pulse reaction and switch reaction over the LaFeO3 catalyst. In the absence of gaseous-phase oxygen, the rate-determining step of methane conversion is the migration rate of lattice oxygen, but the process can be carried out in optimized cycles. The product distribution for POM over LaFeO3 catalyst in the absence of gaseous oxygen was determined by the concentration of surface oxygen, which is relevant with the migration rate of lattice oxygen from the bulk toward the surface. This process of hydrogen production via selective oxidation of methane by lattice oxygen is better in avoiding the deep oxidation (to CO2) and enhancing the selectivity. Therefore, this new route is superior to general POM in stability (resistance to carbonaceous deposition), safety (effectively avoiding accidental explosion), ease of operation and optimization, and low cost (making use of air not oxygen). |
WOS记录号 | WOS:000242974300050 |
内容类型 | 期刊论文 |
源URL | [http://ir.rcees.ac.cn/handle/311016/22956] |
专题 | 生态环境研究中心_环境纳米材料实验室 |
推荐引用方式 GB/T 7714 | Dai, Xiao Ping,Wu, Qiong,Li, Ran Jia,et al. Hydrogen production from a combination of the water-gas shift and redox cycle process of methane partial oxidation via lattice oxygen over LaFeO3 perovskite catalyst[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2006,110(51):25856-25862. |
APA | Dai, Xiao Ping,Wu, Qiong,Li, Ran Jia,Yu, Chang Chun,&Hao, Zheng Ping.(2006).Hydrogen production from a combination of the water-gas shift and redox cycle process of methane partial oxidation via lattice oxygen over LaFeO3 perovskite catalyst.JOURNAL OF PHYSICAL CHEMISTRY B,110(51),25856-25862. |
MLA | Dai, Xiao Ping,et al."Hydrogen production from a combination of the water-gas shift and redox cycle process of methane partial oxidation via lattice oxygen over LaFeO3 perovskite catalyst".JOURNAL OF PHYSICAL CHEMISTRY B 110.51(2006):25856-25862. |
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