摘要/Abstract

采用溶胶凝胶法合成了钙钛矿复合氧化物, 负载氧化铜后得钙钛矿负载型催化材料, 通过XRD (X射线衍射分析)、BET(比表面积测试)、H₂-TPR(程序升温还原分析)、XPS (X射线光电子能谱)等手段对催化材料进行了表征, 考察了不同种类钙钛矿负载纳米铜催化材料的结构、性质对甲醇水蒸气重整制氢性能的影响. 结果显示, 钙钛矿负载纳米铜催化材料的催化活性主要与催化剂的铜比表面积、表面晶格氧缺位以及活性组分和载体间的相互作用有关. 其中, CuO/LaCrO₃钙钛矿负载型催化材料的表面氧空穴含量较多, 活性组分与载体间相互作用较强, 因此催化甲醇水蒸气重整制氢活性较好. 当反应温度为360 ℃时, CuO/LaCrO₃钙钛矿型催化剂并未出现明显失活现象, 甲醇转化率为98.6%, 产氢速率为694.9 mL•kg_cat ^–1•s ^–1.
关键词: 钙钛矿, 氧化铜, 催化剂, 甲醇水蒸气重整, 氢气
As an important clean energy, hydrogen energy has the advantages of light weight, high calorific value, and environmental protection. If hydrogen energy can be well developed and stored, it will play more and more important roles in the human production and life. Methanol steam reforming (MSR) hydrogen production technology, which has been used in industry for many years, is the best choice for methanol hydrogen production because of its high hydrogen content in reforming tail gas and mature technology. ABO₃ perovskite oxide is a new type of material. Compared with other materials, due to its unique electronic structure, it has various properties such as electricity, magnetism, optics and chemistry. It have shown great application prospects in many fields. The perovskite composite oxide was synthesized by the sol-gel method. After loading copper oxide, a perovskite-supported catalytic material was obtained. The catalytic material was characterized by XRD (X-ray diffraction), BET (Brunner-Emmet-Teller), H₂-TPR (H₂-temperature programmed reduction) and XPS (X-ray photo- electron spectra). The effect of the structure and properties of perovskite-loaded nano-copper catalytic materials on the performance of methanol steam reforming for hydrogen production were investigated. The results showed that the catalytic activity of the perovskite-loaded nano-copper catalytic material is mainly related to the copper surface area, the catalytic and reductive properties, the oxygen lattice deficiency on the surface of the catalyst, and the interaction between the active component and the carrier. Among them, because the CuO/LaCrO₃ perovskite-supported catalytic materials have the larger copper surface area, the lower reduction temperature, the more oxygen vacancies on the surface, and the stronger interaction between the active component, the catalytic activity of methanol steam reforming for hydrogen production is better than that of the CuO/LaNiO₃, CuO/LaFeO₃ and CuO/La₂Zr₂O₇. When the reaction temperature was 360 ℃, the CuO/LaCrO₃ perovskite catalyst did not show significant deactivation, the methanol conversion rate was 98.6%, and the hydrogen production rate was 694.9 mL•kg_cat ^–1•s ^–1.
Key words: perovskite, CuO, catalyst, steam reforming of methanol, hydrogen


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