| 原位合成的Cu-SSZ-13催化剂：结晶时间对NH3-SCR性能的影响 |
| In-Situ Synthesis of Cu-SSZ-13 Catalyst: Effect of Crystallization Time on NH3-SCR Performance |
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| 摘要: 通过一步法原位合成Cu-SSZ-13分子筛催化剂，考察了结晶反应时间对NH3选择性催化还原（NH3-SCR）催化性能的影响，利用H2程序升温还原（H2-TPR）、X射线衍射（XRD）、电子顺磁共振光谱（EPR）和X射线电子能谱（XPS）等分析手段表征催化剂。结果表明，结晶时间不同会影响到Cu-SSZ-13分子筛中活性Cu物种的含量和分布，结晶时间为4 d时Cu-SSZ-13分子筛的NH3-SCR催化性能最佳。高温水热条件下，Cu-SSZ-13分子筛中不稳定的CuA2+物种会发生迁移而形成相对稳定的CuB2+物种；Cu2+物种发生团聚而造成分子筛结构破坏，部分Cu2+物种也因分子筛骨架坍塌而被包埋，这是导致催化活性下降的主要原因。 |
| 关键词: 环境化学 分子筛 水热合成 |
| 基金项目: 浙江省科技厅重点科研计划（No.2018C03037）资助项目。 |
| Abstract: Different Cu-SSZ-13 catalysts are prepared by one-pot synthesis by changing the crystallization time during the reaction and characterized using various analytical techniques, including H2-temperature program reduction (H2-TPR), X-ray diffraction (XRD), electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS). The result demonstrated that the crystallization time had an important impact on the content and distribution of active copper species. The catalysts with proper crystallization time showed excellent activity and hydrothermal stability for the NH3 selective catalytic reduction (NH3-SCR) reaction and the best crystallization time was about 4 d. In the zeolite, the unstable CuA2+ species may be converted to stable CuB2+ species and the Cu2+ species agglomerated together under high-temperature hydrothermal conditions. In conclusion, the collapse of the zeolite structure and the agglomeration of active Cu2+ species were the main reason for the deterioration of the hydrothermal stability. |
| Keywords: environmental chemistry zeolites hydrothermal synthesis |
| 投稿时间：2018-05-29 修订日期：2018-09-24 |
| 摘要点击次数: 1964 |
| 全文下载次数: 1464 |
| 陈佳炜,赵茹,周仁贤.原位合成的Cu-SSZ-13催化剂：结晶时间对NH3-SCR性能的影响[J].无机化学学报,2018,34(12):2135-2142. |
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