| 曾哲,朱志新,郭伟琦,江治,上官文峰.有序介孔CuFe2O4同时催化去除碳烟与NOx[J].分子催化,2021,35(1):13-21 |
| 有序介孔CuFe2O4同时催化去除碳烟与NOx |
| Simultaneous Catalytic Removal of Soot and NOx by Ordered Mesoporous CuFe2O4 |
| 投稿时间：2020-11-25 修订日期：2020-12-12 |
| DOI：10.16084/j.issn1001-3555.2021.01.002 |
| 中文关键词: CuFe2O4 介孔材料 催化 碳烟 氮氧化合物 |
| 英文关键词:CuFe2O4 mesoporous materials catalysis soot NO |
| 基金项目:国家自然科学基金（U1832155）；国家重点基础研究发展规划项目（2017YFE0127500）. |
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| 中文摘要: |
| 采用纳米复刻（浇筑）法制备一系列介孔CuFe2O4.通过X射线衍射（XRD）、N2物理吸附、透射电镜（TEM）等研究了不同制备条件对有序介孔CuFe2O4结构形成的影响.研究发现，作为对比，柠檬酸法仅能合成普通的四方相CuFe2O4纳米颗粒，但是硬模板法则能合成出高温淬火才能形成的立方晶相介孔结构CuFe2O4.进一步研究了该催化剂同时催化去除碳烟和氮氧化合物（NOx）的性能，研究发现，与柠檬酸法合成的普通CuFe2O4催化剂相比，介孔结构CuFe2O4不仅大幅降低了碳烟起燃温度（324降低到278℃），而且将N2的最高产率从5.9%提升到了92.2%.基于原位漫反射红外（in-situ DRIFTS）的机理分析研究表明，合成过程中采用NaOH除去硬模板的过程中会在介孔CuFe2O4表面造成大量残留的钠盐，这种高分散的钠物种促进了NOx的吸附并转化为硝酸盐物种，从而促进碳烟氧化以及NOx转化.但是与表面Na修饰的CuFe2O4相比，体相Na掺杂的CuFe2O4虽然具有更好的有序介孔结构，但是其氧化性能下降，进一步也导致了NOx的催化还原性能的下降. |
| 英文摘要: |
| A series of mesoporous CuFe2O4 was prepared by nanocasting method. The effects of different synthesis conditions on the formation of ordered mesoporous CuFe2O4 have been investigated by X-ray diffraction (XRD), N2 physical adsorption, and transmission electron microscopy (TEM). CuFe2O4 with tetragonal structure was synthesized by the citrate acid method, but mesoporous CuFe2O4 with cubic crystal phase structure which can be formed only under high-temperature quenching condition, was synthesized by the nanocasting method. The performance of simultaneous catalytic removal of soot and nitrogen oxides (NOx) by a series of CuFe2O4 catalysts was further evaluated. Compared with the CuFe2O4 nanoparticles synthesized by the citrate acid method, mesoporous CuFe2O4 not only reduced the soot ignition temperature from 324.6 to 278.2 ℃ but also significantly increased the maximum N2 yield from 5.92% to 92.24%. Mechanism analysis based on in-situ DRIFTS showed that removing the hard template by NaOH during the synthesis process would cause a large amount of residual sodium salt on the surface of the mesoporous CuFe2O4. Highly dispersed sodium species promoted the adsorption of NOx on the surface of mesoporous CuFe2O4 and conversion of NOx into nitrate species, thus facilitated soot oxidation and NOx conversion. However, compared with CuFe2O4 modified with Na, Na-doped CuFe2O4 showed a better ordered mesoporous structure, but its oxidation performance was reduced coupling with a worse catalytic reduction performance of NOx. |
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