Study on combustion solution prepared Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 and their photocatalytic performance
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摘要: 以硝酸钴（Co(NO3)2·6H2O）、硝酸铁（Fe(NO3)3·9H2O）、硝酸镍（Ni(NO3)2·6H2O）、硝酸锰（Mn(NO3)2·4H2O）、硝酸铜（Cu(NO3)2·3H2O）为原料，甘氨酸为燃料，通过溶液燃烧合成法制备Co0.25Ni0.25Cu0.25Mn0.25Fe2O4，探究不同甘氨酸的量对Co0.25Ni0.25Cu0.25Mn0.25Fe2O4粉末的制备以及光催化性能的影响，并以有机溶剂亚甲基蓝为污染源，测试其光催化性能。对粉末样品进行了XRD检测，并找到甘氨酸的最佳用量。结果表明：当甘氨酸与硝酸铁的摩尔比为4时，对亚甲基蓝的光催化性能最好，完全降解初始浓度0.002%、0.004%、0.006%亚甲基蓝的时间分别为40、60、70 min，并进行了动力学分析，认为降解过程受扩散步骤控制。以葡萄糖作为添加剂可有效提高Co0.25Ni0.25Cu0.25Mn0.25Fe2O4粉末的催化活性，当添加量为1 g时，完全降解初始浓度为0.004%的亚甲基蓝所需时间缩短至50 min，降解效率提高了16.7%。Abstract: Using cobalt nitrate (Co(NO3)2·6H2O), iron nitrate (Fe(NO3)3·9H2O), nickel nitrate (Ni(NO3)2·6H2O), manganese nitrate (Mn(NO3)2·4H2O), copper nitrate (Cu(NO3)2·3H2O) as raw materials and glycine as fuel, Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 was prepared by solution combustion synthesis. The preparation and catalytic performance of Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 powder with different mount of glycine were investigated. The organic solvent methylene blue was used as the pollution source to test its photocatalytic performance. The powder samples were detected by XRD, and the optimum amount of glycine was found. The results showed that when the molar ratio of glycine to iron nitrate was 4, of methylene blue achieved the best photocatalytic performance. The time for complete degradation of 0.002%, 0.004%, and 0.006% methylene blue was 40 minutes, 60 minutes, and 70 minutes, respectively. The kinetic analysis was also carried out. Glucose as the additives can effectively improve Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 powder in the catalytic activity. When the adding glucose amount is 1 g, the required time for fully biodegradable initial concentration of 0.004% MB is 50 minutes, and degradation efficiency increased by 16.7%.
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Key words:
- high entropy oxides /
- solution combustion /
- photocatalysis /
- degradation rate
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图 1 （a）产物的X射线衍射图谱（φ=4），（b）尖晶石型结构
Figure 1. (a)X-ray diffraction pattern of product（φ=4）, (b) a spinel structure
图 3 φ=4的Co0.25Ni0.25Cu0.25Mn0.25Fe2O4降解初始浓度为0.004%的亚甲基蓝
Figure 3. Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 （φ=4）degradation of initial concentration of 0.004% MB
图 4 （a）Co0.25Ni0.25Cu0.25Mn0.25Fe2O4降解初始浓度为0.002%的亚甲基蓝； (b) Co0.25Ni0.25Cu0.25Mn0.25Fe2O4降解初始浓度为0.006%的亚甲基蓝
Figure 4. Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 （φ=4）degradation of different initial concentration of MB: (a) 0.002%, (b) 0.006%
图 5 Co0.25Ni0.25Cu0.25Mn0.25Fe2O4降解不同初始浓度亚甲基蓝溶液的动力学曲线
Figure 5. The kinetics curve for Co0.25Ni0.25Cu0.25Mn0.25Fe2O4 degradation of different initial concentration
图 6 不同葡萄糖添加量改性后的Co0.25Ni0.25Cu0.25Mn0.25Fe2O4降解初始浓度0.004%的亚甲基蓝
Figure 6. Degradation of initial concentration of 0.004%MB by adding different amounts of glucose modified Co0.25Ni0.25Cu0.25Mn0.25Fe2O4
表 1 试验原料及配比
Table 1. The raw materials and ratio
编号 甘氨酸与硝酸铁
的摩尔比φ加量/g 硝酸铁 硝酸锰 硝酸钴 硝酸镍 硝酸铜 甘氨酸 1 3 4.04 0.474 0.364 0.363 0.302 2.25 2 4 4.04 0.474 0.364 0.363 0.302 3.00 3 5 4.04 0.474 0.364 0.363 0.302 3.75 4 6 4.04 0.474 0.364 0.363 0.302 4.50 
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