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
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摘要
三维有序大孔钴锰尖晶石催化剂(3DOMCoMn_2O_4)以及三维有序大孔镧、铈掺杂的钴锰尖晶石催化剂(3DOMR_xCo_(1-x)Mn_2O_4(R=Ce, La))由胶晶模板法成功合成。通过对所得的催化剂在NO_x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、H_2-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 Ce_(0.9)Co_(0.1)Mn_2O_4的Tig(起燃温度)和T_m(CO_2出口浓度最大时的温度)分别为285℃和377℃,3DOM La_(0.3)Co_(0.7)Mn_2O_4的T_(ig)和T_m分别为287℃和376℃。
Three-dimensionally ordered macroporous(3DOM) CoMn_2O_4 and 3DOM R_xCo_(1-x)Mn_2O_4(R=Ce, La) spinel were successfully synthesized with the colloidal crystal template method. The catalytic activities of these catalysts for NO_x-assisted soot combustion were evaluated, and the optimum ratios of Ce/Co and La/Co were determined. XRD, SEM,N_2 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 ℃ and Tm= 377 ℃ were achieved for 3 DOM Ce_(0.9)Co_(0.1)Mn_2O_4 catalysts, while T_(ig)= 287 ℃ and T_m= 376 ℃ were achieved for 3 DOM La_(0.3)Co_(0.7)Mn_2O_4, both of which are the enhanced catalytic activities.
Three-dimensionally ordered macroporous(3DOM) CoMn_2O_4 and 3DOM R_xCo_(1-x)Mn_2O_4(R=Ce, La) spinel were successfully synthesized with the colloidal crystal template method. The catalytic activities of these catalysts for NO_x-assisted soot combustion were evaluated, and the optimum ratios of Ce/Co and La/Co were determined. XRD, SEM,N_2 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 ℃ and Tm= 377 ℃ were achieved for 3 DOM Ce_(0.9)Co_(0.1)Mn_2O_4 catalysts, while T_(ig)= 287 ℃ and T_m= 376 ℃ were achieved for 3 DOM La_(0.3)Co_(0.7)Mn_2O_4, both of which are the enhanced catalytic activities.
引文
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[3] XIAO P, ZHONG L Y, ZHU J J, et al. CO and soot oxidation over macroporous perovskite La Fe O3[J]. Catalysis Today,2015,258(2):660-667. DOI:10.1016/j.cattod.2015.01.007.
[4] NIU X W, ZHOU L, HE X J, et al. Mesoporous Ce?Co1-xCr2O4 spinels:Synthesis, characterization and catalytic application in simultaneous removal of soot particulate and NO[J]. RSC Advances,2015,(5):52595-52601. DOI: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-xK?Co1-yMgyO3perovskite oxides[J]. Catalysis Communications,2014,49(5):15-19. DOI:10.1016/j.catcom.2014.01.029.
[6] ZHAO B, WANG R J, YANG X X. Simultaneous catalytic removal of NO?and diesel soot particulates over La1-xCe?Ni O3 perovskite oxide catalysts[J]. Catalysis Communications,2009,10(7):1029-1033. DOI:10.1016/j.catcom.2008.10.024.
[7] GUO X, MENG M, DAI F F, et al. NO?-assisted soot combustion over dually substituted perovskite catalysts La1-xK?Co1-yPdy O3-δ[J].Applied Catalysis B:Environmental,2013,142-143:278-289. DOI:10.1016/j.apcatb.2013.05.036.
[8] BENSAID S, RUSSO N, FINO D. Ce O2 catalysts with fibrous morphology for soot oxidation:The importance of the soot-catalyst contact conditions[J]. Catalysis Today,2013,216(1):57-63. DOI: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. DOI: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 of3DOM Ce-based materials for the combustion of diesel soot[J]. Applied Catalysis B:Environmental,2011,107(3/4):302-315.DOI: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. DOI: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. DOI:10.1016/j.tca.2008.04.015.
[13] LIN X T, LI S J, HE H, et al. Evolution of oxygen vacancies in Mn O?-Ce O2 mixed oxides for soot oxidation[J]. Applied Catalysis B:Environmental,2018,223:91-102. DOI: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. DOI:10.1016/j.apsusc.2013.01.081.
[15] GUO W H, MA X X, ZHANG X L, et al. Spinel Co Mn2O4 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.DOI: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. DOI:10.1016/j.apcatb.2015.06.018.
[17]马红钦,谭欣,朱慧,等. La1-xCe?Fe O3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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