| 孔令朋,苗杰,李明航,谈冠希,靳广洲.CuMnCeLa-O/γ-Al2O3催化剂助燃脱硝性能研究[J].分子催化,2018,32(4):295-304 |
| CuMnCeLa-O/γ-Al2O3催化剂助燃脱硝性能研究 |
| Performances of Selective Catalytic Reduction of NO with CO over CuMnCeLa-O/γ-Al2O3 Catalyst |
| 投稿时间：2018-04-08 修订日期：2018-06-06 |
| DOI： |
| 中文关键词: 催化剂 H2-TPR XPS 氧空位 CO+NO 氧化 还原 |
| 英文关键词:catalyst H2-TPR XPS oxygen vacancy CO+NO oxidation reduction |
| 基金项目:国家重点基础研究发展计划资助项目（"973"计划2012CB215002） |
|
| 摘要点击次数: 1479 |
| 全文下载次数: 1649 |
| 中文摘要: |
| 采用等体积浸渍法制备了CuMn-O/γ-Al2O3、CuMnCe-O/γ-Al2O3和CuMnCeLa-O/γ-Al2O3催化剂.用XRD、BET、SEM、XPS和H2-TPR技术对其物相和表面性质进行了表征.在连续固定床微反装置上评价了催化剂的CO+O2和CO+NO反应性能.结果表明，催化剂样品中观测不到CuO、MnOx、CeO2和La2O3的XRD晶相峰，活性组分在γ-Al2O3载体表面呈高度分散状态.Ce、La的引入对催化剂的比表面积、孔容和孔径分布影响不大.SEM谱图中未观测到活性组分的形貌，金属氧化物在载体表面均匀分布.Ce3+↔；Ce4+之间的可变价转换，引起CuMnCe-O/γ-Al2O3催化剂表相CuO中具有非完整结构的[Cu1-x2+Cux+][O1-（1/2）x□（1/2）x]增多，Cu+/Cu2+比例增大，表相氧空位增多，H2-TPR还原峰温度向低温区偏移.Ce4+、La3+之间不平衡电荷以及共生过程中Cu-Mn-Ce-La-O之间的强相互作用，加大了CuO和MnOx结构的不完整性，导致CuMnCeLa-O/γ-Al2O3催化剂样品表相产生更多的Cu+、Mn2+、Mn3+和氧空位，相应的H2-TPR还原峰温度进一步向低温区偏移.催化氧化CO和CO催化还原NO实验结果表明，在反应空速20 000 h-1，350℃反应温度下，CuMnCeLa-O/γ-Al2O3催化剂CO催化还原NO反应的CO转化率达到88.2%，NO转化率达到了96.1%，表现出了较好的氧化还原活性. |
| 英文摘要: |
| CuMn-O/γ-Al2O3、CuMnCe-O/γ-Al2O3 and CuMnCeLa-O/γ-Al2O3 catalysts were prepared by incipient wetness impregnation, and characterized by XRD, XPS and H2-TPR techniques. Catalytic activities of the catalysts were investigated in CO + O2 and NO + CO model reactions by a continuous fixd bed reactor. The XRD patterns indicated that no diffraction peaks of crystalline CuO, MnOx, CeO2 and La2O3 were observed in the catalysts, and showed that the active component was highly dispersed on the surface of γ-Al2O3 supporter. The BET results indicated that Ce and La had little effect on the specific surface area, pore volume and pore size distribution of the catalyst. The active component was not observed in the SEM images. The valence transition between Ce3+ and Ce4+ resulted in the growth of imperfect structure[Cu1-x2+Cux+][O1-(1/2)x□(1/2)x], ratio of Cu+/Cu2+ and oxygen vacancy in the epiphase CuO of CuMnCe-O/γ-Al2O3 catalyst, and caused the H2-TPR profile shifts to low temperature. The higher Cu+, Mn2+, Mn3+ and the oxygen vacancy generated by charges unbalance of Ce4+/La3+ and the strong interaction between Cu-Mn-Ce-La-O during the intergrowth process of the CuMnCeLa-O/γ-Al2O3 sample, and lead the H2-TPR profile shifts to lower temperature. The conversion of CO oxidation and NO reduction of CuMnCeLa-O/γ-Al2O3 catalyst reached to 88.2% and 96.1% by using catalytic reduction of NO with CO under the reaction conditions of 350℃ and gas hourly space velocity 20 000 h-1, respectively. |
| HTML 查看全文 查看/发表评论 下载PDF阅读器 |
