Preparation of Zr-based perovskite supported Fe2O3 catalyst and its performance in the reverse water gas shift reaction
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摘要: 采用固相反应法制备了钙钛矿结构的BaZr0.9Y0.1O3，并用BaZr0.9Y0.1O3作为载体负载Fe2O3，通过X射线衍射分析（XRD）、扫描电子显微镜（SEM）观察负载型催化剂的晶相结构和微观形貌，同时考察了制备的催化剂的逆水煤气反应催化活性。结果表明，BaZr0.9Y0.1O3粉体1200℃煅烧5h时，负载型催化剂具有较好的催化活性；BaZr0.9Y0.1O3对逆水煤气反应有一定的催化作用，负载少量的Fe2O3催化剂可以明显促进CO2还原，在空速为1.13h-1，温度为650℃时，CO收率可以达到31%；催化剂经过长时间运行催化效果良好，制备的催化剂活性较稳定。Abstract: BaZr0.9Y0.1O3 with perovskite structure was prepared by solid-phase reaction method and used as support to prepare Fe2O3 based catalysts. X-ray diffraction analysis (XRD) and scanning electron microscopy (SEM) were used to observe the crystal phase structure and microscopic morphology of the prepared catalysts. The catalyst performance for the reverse water gas shift reaction was also investigated. The results showed that the supported catalyst has better catalytic activity when the BaZr0.9Y0.1O3 powder was calcined at 1200℃ for 5 h. BaZr0.9Y0.1O3 has an obvious catalytic effect on the reverse water gas reaction, and the Fe2O3-supported catalyst can significantly promote CO2 reduction. Moreover, loading small amount of Fe2O3 has apparent effect on the reactivity of the catalyst. When the space velocity was 1.13 h-1, the CO yield can reach 31% at 650℃. Carbon deposition on the catalyst during the CO2 reduction process was taking place in a low rate, leading to a significant increase in the CO yield in the process of cooling-down experiment. In addition, the activity of the catalyst did not significantly decrease after a long period of reaction, which proved that the activity of the prepared catalyst was relatively stable.
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Key words:
- Fe2O3 /
- catalyst /
- Zr-based catalyst /
- reverse water gas reaction
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图 2 不同焙烧时间下制备BZY的XRD谱图
Figure 2 XRD patterns of BZY prepared with different calcination time
图 4 载体焙烧时间对催化剂性能的影响
Figure 4 Effect of calcination time of the support on catalyst performance
图 5 不同Fe2O3负载量对催化剂性能的影响
Figure 5 Effect of different Fe2O3 loading on catalyst performance
图 6 650 ℃持续反应催化剂的催化性能
Figure 6 Catalytic performance of 650 ℃ continuous reaction catalyst
图 7 升降温序列过程中CO的收率
Figure 7 CO yield during the heating-up process and the cooling-down process
图 8 负载型催化剂反应前后的SEM照片
Figure 8 SEM images of the supported catalysts
(a): fresh catalyst;
(b): used catalyst
图 9 逆水煤气反应过程中CO2转化率和CO收率
Figure 9 CO2 conversion and CO yield during the reverse water gas reaction
表 1 CO收率随负载量的变化
Table 1 CO yield of different Fe2O3 loading catalysts at 650 ℃
Catalyst BZY BZY+3%Fe2O3 BZY+5% Fe2O3 BZY+8% Fe2O3 BZY+15% Fe2O3 BZY+20% Fe2O3 CO yield w/% 12.88 32.24 31.14 31.55 26.03 23.88 
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