| 一步水热合成Cu-SAPO-34选择性催化丙烯还原氮氧化物 | |
| Selective Catalytic Reduction of Nitric Oxide with Propylene over One-Step Synthesized Cu-SAPO-34 Catalysts | |
| 摘要: 采用一步法水热合成不同Cu/Al比的Cu-SAPO-34催化剂，并对其丙烯选择性催化还原NO（C3H6-SCR）性能进行了研究。通过N2吸附-脱附、X射线衍射（XRD）、X射线光电子能谱（XPS）、程序升温还原（H2-TPR）和原位漫反射傅里叶变换红外光谱（In situ DRIFTS）等研究手段对催化剂进行表征，考察Cu-SAPO-34中Cu物种含量对催化剂的物理化学性质和反应活性的影响。结果表明，当铜负载量为2.76%~4.12%（w/w）时，Cu-SAPO-34催化剂在富氧条件下300~400℃内表现出非常有吸引力的C3H6-SCR活性，可实现~100%的脱硝效率和~100%的N2选择性。原位红外光谱研究表明，Cu-SAPO-34分子筛骨架上孤立的Cu2+离子是NO吸附和活化形成NO2-/NO3-中间物种的主要活性位，并通过C3H6-SCR反应过程中Cu2+/Cu+氧化还原循环来实现Cu2+离子的持续供给。 | |
| 关键词: Cu-SAPO-34 选择性催化还原 NO 丙烯 Cu2+离子 | |
| 基金项目: 江苏省自然科学基金（No.BK20181161）、国家自然科学基金（No.51278095）、江苏省高校“青蓝工程”项目（2017）和江苏省“333工程”科研项目（2018）资助 | |
| Abstract: To investigate the performance of Cu-chabazite for selective catalytic reduction of NO with propylene (C3H6-SCR), a series of Cu-SAPO-34 catalysts with varied Cu/Al ratio have been synthesized by the one-pot hydrothermal method. These catalysts were characterized using N2 adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction by H2 (H2-TPR), and in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) techniques. The effect of Cu component on physicochemical properties and C3H6-SCR activity were investigated. Cu-SAPO-34 catalysts with Cu loading (22.76%~ 4.12%(w/w)) exhibited attractive activities, with nearly 100% NOx conversion and 100% N2 selectivity at the temperatures (300~400℃) in the excess of oxygen. Based on in situ DRIFT studies, the formation of NO2-/NO3- intermediates requires the presence of isolated Cu2+ ions in Cu-SAPO-34, which undergo a periodic Cu2+/Cu+ redox cycle during C3H6-SCR. | |
| Keywords: Cu-SAPO-34 selective catalytic reduction NO C3H6 Cu2+ ions | |
| 投稿时间：2020-03-31 修订日期：2020-06-15 | |
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| 周皞,杨迪,王聪颖,赵辉爽,伍士国,苏亚欣.一步水热合成Cu-SAPO-34选择性催化丙烯还原氮氧化物[J].无机化学学报,2020,36(10):1997-2004. | |
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