李水荣1,
李宗沅1,
王夺1,
叶跃元1,
刘运权1
1.厦门大学能源学院，厦门 361102
基金项目: 国家自然科学基金资助项目（21276214）
福建省科技厅重点项目（2016H6024）
福建省自然科学基金资助项目（2015J05033）
Preparation of three-dimensionally ordered macroporous spinel-type catalysts and their performance for catalytic oxidation of soot
YAN Shuai1,,LI Shuirong1,
LI Zongyuan1,
WANG Duo1,
YE Yueyuan1,
LIU Yunquan1
1.College of Energy, Xiamen University, Xiamen 361102, China
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摘要:三维有序大孔钴锰尖晶石催化剂（3DOM CoMn2O4）以及三维有序大孔镧、铈掺杂的钴锰尖晶石催化剂（3DOM RxCo1-xMn2O4（R=Ce, La））由胶晶模板法成功合成。通过对所得的催化剂在NOx协助下的碳烟催化氧化活性评价，优化了Ce/Co和La/Co的配比。此外，还对目标催化剂进行了XRD、N2吸脱附、Raman、H2-TPR、SEM、XPS等表征。结果表明：3DOM结构增强了催化剂与碳烟颗粒之间的接触，对碳烟氧化等“固-固-气”非均相催化反应具有明显的提升作用。此外，铈和镧的掺杂增大了活性氧物种的浓度，从而增强了钴锰尖晶石催化剂的催化氧化能力。在松散接触工况下，3DOM Ce0.9Co0.1Mn2O4的Tig（起燃温度）和Tm（CO2出口浓度最大时的温度）分别为285 oC和377 oC，3DOM La0.3Co0.7Mn2O4的Tig和Tm分别为287 oC和376 oC。
关键词: 碳烟颗粒/
催化氧化/
三维有序大孔/
钴锰尖晶石
Abstract:Three-dimensionally ordered macroporous (3DOM) CoMn2O4 and 3DOM RxCo1-xMn2O4(R=Ce, La) spinel were successfully synthesized with the colloidal crystal template method. The catalytic activities of these catalysts for NOx-assisted soot combustion were evaluated, and the optimum ratios of Ce/Co and La/Co were determined. XRD, SEM, N2 adsorption-desorption, XPS, Raman and H2-TPR were employed to characterize the prepared samples. It was found that 3DOM structure provides better contact between soot and catalysts compared to other structures，thus promoting the heterogeneous catalytic soot oxidations in solid-solid-gas interfaces. In addition, the doping of cerium or lanthanum improved the catalytic oxidation capability of spinels by increasing the concentrations of active oxygen species. And under loose contact, Tig = 285 oC and Tm = 377 oC were achieved for 3DOM Ce0.9Co0.1Mn2O4 catalysts, while Tig = 287 oC and Tm = 376 oC were achieved for 3DOM La0.3Co0.7Mn2O4, both of which are the enhanced catalytic activities.
Key words:soot particulate/
catalytic oxidation/
three-dimentional ordered macroporous/
CoMn2O4 spinel.
| [1] | SETTEN B,MAKKEE M,MOULIJN J,et al.Science and technology of catalytic diesel particulate filters[J].Catalysis Reviews,2001,43(4):489-564 10.1081/CR-120001810 |
| [2] | SHANGGUAN W, TERAOKA Y, KAGAWA S.Simultaneous catalytic removal of NO, and diesel soot particulates over ternary AB2O4 spinel-type oxides[J].Applied Catalysis B: Environmental,1996,8(2):217-227 10.1016/0926-3373(95)00070-4 |
| [3] | XIAO P, ZHONG L Y, ZHU J J, et al.CO and soot oxidation over macroporous perovskite LaFeO3[J].Catalysis Today,2015,258(2):660-667 10.1016/j.cattod.2015.01.007 |
| [4] | NIU X W, ZHOU L, HE X J, et al.Mesoporous CexCo1-xCr2O4 spinels: Synthesis, characterization and catalytic application in simultaneous removal of soot particulate and NO[J].RSC Advances,2015,(5):52595-52601 10.1039/C5RA04759E |
| [5] | FANG S Q, Wang L, SUN Z C, et al.Catalytic removal of diesel soot particulates over K and Mg substituted La1-xKxCo1-yMgyO3 perovskite oxides [J].Catalysis Communications,2014,49(5):15-19 10.1016/j.catcom.2014.01.029 |
| [6] | ZHAO B, WANG R J, YANG X X.Simultaneous catalytic removal of NOx and diesel soot particulates over La1-xCexNiO3 perovskite oxide catalysts[J].Catalysis Communications,2009,10(7):1029-1033 10.1016/j.catcom.2008.10.024 |
| [7] | GUO X, MENG M, DAI F F, et al.NOx-assisted soot combustion over dually substituted perovskite catalysts La1-xKxCo1-yPdyO3?δ[J].Applied Catalysis B: Environmental,2013,142–143:278-289 10.1016/j.apcatb.2013.05.036 |
| [8] | BENSAID S, RUSSO N, FINO D.CeO2 catalysts with fibrous morphology for soot oxidation: The importance of the soot–catalyst contact conditions[J].Catalysis Today,2013,216(1):57-63 10.1016/j.cattod.2013.05.006 |
| [9] | LEE C, JEON Y, HATA S, et al.Three-dimensional arrangements of perovskite-type oxide nano-fiber webs for effective soot oxidation[J].Applied Catalysis B: Environmental,2016,191(15):157-164 10.1016/j.apcatb.2016.03.001 |
| [10] | ZHANG G Z, ZHAO Z, Xu J F, et al.Comparative study on the preparation, characterization and catalytic performances of 3DOM Ce-based materials for the combustion of diesel soot[J].Applied Catalysis B: Environmental,2011,107(3/4):302-315 10.1016/j.apcatb.2011.07.029 |
| [11] | WAGLOEHNER S, NITZER-NOSKI M, KURETI S.Oxidation of soot on manganese oxide catalysts[J].Chemical Engineering Journal,2015,259(1):492-504 10.1016/j.cej.2014.08.021 |
| [12] | TANG C W, WANG C B, CHEN S H.Characterization of cobalt oxides studied by FT-IR, Raman, TPR and TG-MS[J].Thermochimica Acta,2008,473(1/2):68-73 10.1016/j.tca.2008.04.015 |
| [13] | LIN X T, LI S J, HE H, et al.Evolution of oxygen vacancies in MnOx-CeO2 mixed oxides for soot oxidation[J].Applied Catalysis B: Environmental,2018,223:91-102 10.1016/j.apcatb.2017.06.071 |
| [14] | AMRI A, DUAN X F, YIN C Y, et al.Solar absorptance of copper–cobalt oxide thin film coatings with nano-size, grain-like morphology: Optimization and synchrotron radiation XPS studies[J].Applied Surface Science,2013,275(15):127-135 10.1016/j.apsusc.2013.01.081 |
| [15] | GUO W H,MA X X,ZHANG X L,et al.Spinel CoMn2O4 nanoparticles supported on a nitrogen and phosphorus dual doped graphene aerogel as efficient electrocatalysts for the oxygen reduction reaction[J].RSC Advances,2016, 99 (6):96436-96444 10.1039/C6RA16337H |
| [16] | PIUMETTI M, BENSAID S, RUSSO N, et al.Investigations into nanostructured ceria–zirconia catalysts for soot combustion[J].Applied Catalysis B: Environmental,2016,180:271-282 10.1016/j.apcatb.2015.06.018 |
| [17] | 马红钦, 谭欣, 朱慧, 等.La1-xCexFeO3 钙钛石高变催化剂的 XPS研究[J].中国稀土学报,2003,2(4):445-448 |
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基于碳烟颗粒催化氧化的三维有序大孔催化剂制备及性能
闫帅1,,李水荣1,
李宗沅1,
王夺1,
叶跃元1,
刘运权1
1.厦门大学能源学院，厦门 361102
基金项目: 国家自然科学基金资助项目（21276214） 福建省科技厅重点项目（2016H6024） 福建省自然科学基金资助项目（2015J05033）
关键词: 碳烟颗粒/
催化氧化/
三维有序大孔/
钴锰尖晶石
摘要:三维有序大孔钴锰尖晶石催化剂（3DOM CoMn2O4）以及三维有序大孔镧、铈掺杂的钴锰尖晶石催化剂（3DOM RxCo1-xMn2O4（R=Ce, La））由胶晶模板法成功合成。通过对所得的催化剂在NOx协助下的碳烟催化氧化活性评价，优化了Ce/Co和La/Co的配比。此外，还对目标催化剂进行了XRD、N2吸脱附、Raman、H2-TPR、SEM、XPS等表征。结果表明：3DOM结构增强了催化剂与碳烟颗粒之间的接触，对碳烟氧化等“固-固-气”非均相催化反应具有明显的提升作用。此外，铈和镧的掺杂增大了活性氧物种的浓度，从而增强了钴锰尖晶石催化剂的催化氧化能力。在松散接触工况下，3DOM Ce0.9Co0.1Mn2O4的Tig（起燃温度）和Tm（CO2出口浓度最大时的温度）分别为285 oC和377 oC，3DOM La0.3Co0.7Mn2O4的Tig和Tm分别为287 oC和376 oC。
English Abstract
Preparation of three-dimensionally ordered macroporous spinel-type catalysts and their performance for catalytic oxidation of soot
YAN Shuai1,,LI Shuirong1,
LI Zongyuan1,
WANG Duo1,
YE Yueyuan1,
LIU Yunquan1
1.College of Energy, Xiamen University, Xiamen 361102, China
Keywords: soot particulate/
catalytic oxidation/
three-dimentional ordered macroporous/
CoMn2O4 spinel
Abstract:Three-dimensionally ordered macroporous (3DOM) CoMn2O4 and 3DOM RxCo1-xMn2O4(R=Ce, La) spinel were successfully synthesized with the colloidal crystal template method. The catalytic activities of these catalysts for NOx-assisted soot combustion were evaluated, and the optimum ratios of Ce/Co and La/Co were determined. XRD, SEM, N2 adsorption-desorption, XPS, Raman and H2-TPR were employed to characterize the prepared samples. It was found that 3DOM structure provides better contact between soot and catalysts compared to other structures，thus promoting the heterogeneous catalytic soot oxidations in solid-solid-gas interfaces. In addition, the doping of cerium or lanthanum improved the catalytic oxidation capability of spinels by increasing the concentrations of active oxygen species. And under loose contact, Tig = 285 oC and Tm = 377 oC were achieved for 3DOM Ce0.9Co0.1Mn2O4 catalysts, while Tig = 287 oC and Tm = 376 oC were achieved for 3DOM La0.3Co0.7Mn2O4, both of which are the enhanced catalytic activities.
