一步固相合成铈钴固溶体低温催化氧化甲苯
One-Step Solid-Phase Synthesis of Ce-Co Solid Solution for Low-Temperature Catalytic Oxidation of Toluene
DOI: 10.12677/NAT.2022.123014, PDF,    科研立项经费支持
作者: 刘毓炜, 周 兵：南通大学化学化工学院，江苏 南通；刘敬印, 刘立忠*：南通大学化学化工学院，江苏 南通；南通大学–云汇科技环境科学联合研发中心，江苏 南通
关键词: 固相合成；催化氧化；VOC；固溶体； Solid Phase Synthesis； Catalytic Oxidation； VOCs； Solid Solution
摘要: 将硝酸铈、硝酸钴和柠檬酸以固体形式进行混合，无需添加任何溶剂，直接通过程序升温焙烧制备一系列不同Ce/Co比的γCoOx-CeOy (γ = 6，5，4，3；记作6CoOx-CeOy，5CoOx-CeOy，4CoOx-CeOy，3CoOx-CeOy)固溶体催化剂，并以甲苯作为模拟挥发性有机化合物(VOC)，评估了不同固溶体催化性能。X射线衍射(XRD)测试表明复合催化剂的晶体结构出现明显松弛畸变。程序升温氢气还原(H2-TPR)测试表明复合后的催化剂晶格氧的可迁移性变得到很大改善。在所有固溶体催化剂中，5CoOx-CeOy取得了最好的最低的甲苯总氧化表观活化能93.06 kJ∙mol−1和二氧化碳收率表观活化能111.62 kJ∙mol−1，其甲苯总氧化和二氧化碳收率的T90%可低至206℃和207℃。此外，也探讨了水蒸汽含量及空速对催化剂稳定性的影响。
Abstract: A series of γCoOx-CeOy (γ = 6, 5, 4, 3; denoted as 6CoOx-CeOy, 5CoOx-CeOy, 4CoOx-CeOy, and 3CoOx- CeOy) were directly prepared by temperature-programmed calcination, wherein the cerium nitrate, cobalt nitrate and citric acid were mixed by solid form and no need to add any solvent. Toluene was used as a simulated volatile organic compound (VOC) to evaluate the catalytic performance of catalysts. X-ray diffraction (XRD) test showed that the crystal structure of the composite showed obvious relaxation distortion. Temperature-programmed hydrogen reduc-tion (H2-TPR) test showed that the mobility of lattice oxygen was greatly improved. Among all, 5CoOx-CeOy achieved the lowest apparent activation energy for total toluene oxidation of 93.06 kJ/mol and carbon dioxide yield of 111.62 kJ/mol, which of T90% for total toluene oxidation and car-bon dioxide yield can be as low as 206˚C and 207˚C. In addition, the effects of water vapor content and space velocity on the stability were also investigated.
文章引用：刘毓炜, 周兵, 刘敬印, 刘立忠. 一步固相合成铈钴固溶体低温催化氧化甲苯[J]. 纳米技术, 2022, 12(3): 115-123. https://doi.org/10.12677/NAT.2022.123014

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