负载催化剂SmMn2O5/γ-Al2O3负载量对NO氧化的影响

doi:10.11944/j.issn.1000-0518.2019.02.180109

摘要/Abstract

摘要：

贵金属催化剂对NO_x催化氧化具有优异的催化性能,但催化剂成本较高,而负载型催化剂及非贵金属催化剂受到了广泛的关注。本文中采用水热法和浸渍法分别制备了SmMn₂O₅纯相催化剂和SmMn₂O₅/γ-Al₂O₃负载催化剂,探索了活性成分SmMn₂O₅含量对NO催化氧化的影响。对负载SmMn₂O₅不同质量分数(5%~100%)的复合催化剂进行了扫描电子显微镜、比表面积、孔径分布、程序升温还原和程序升温脱附的表征以及NO催化氧化的研究。当SmMn₂O₅负载量小于50%(35%、25%、15%、5%)时,负载量为25%的催化剂显示出最低的燃点温度(260 ℃),继续增加负载量到50%和75%,与负载25%的复合催化剂相比,起燃温度降低10 ℃,仅高于纯相催化剂40 ℃。该探索对于SmMn₂O₅催化剂的有效利用将具有一定的指导作用,并为负载型非贵金属催化剂的设计提供一定的思路。

关键词: SmMn₂O₅, 催化剂, NO催化氧化

Abstract:

Noble metal catalyst exhibits excellent effects on the catalytic oxidation of NO_x, but the cost is high. The supported catalysts and non-noble metal catalysts have been widely explored. In this work, SmMn₂O₅(SMO) and SmMn₂O₅/γ-Al₂O₃ catalysts were prepared by hydrothermal method and impregnation method, respectively, and the effect of the content of SmMn₂O₅ on the catalytic oxidation of NO was investigated. Scanning electron microscopy(SEM), specific surface area(BET) and pore size distribution analysis, temperature programmed reduction(TPR) and temperature programmed desorption(TPD) were conducted towards different SmMn₂O₅ loadings(5%100% mass fraction). The catalytic oxidation performance of NO was subsequently carried out. The results indicate that the 25%(mass fraction) SmMn₂O₅/γ-Al₂O₃ catalyst shows the lowest light off temperature(260 ℃) among the load mass fraction of 35%, 25%, 15% and 5%. Continuing increasing SMO loadings mass fraction up to 50% and 75%, it is found that the light off temperature of the two samples only drops off 10℃ relative to 25% SmMn₂O₅/γ-Al₂O₃ catalyst and increases 40 ℃ in regards to the pure phase of mullite SMO. This exploration will provide some guidance for the effective utilization of SmMn₂O₅ catalyst in the future, and introduce certain method for the design of supported non-noble metal catalysts.

Key words: SmMn₂O₅, catalyst, NO catalytic oxidation

杨志. 负载催化剂SmMn₂O₅/γ-Al₂O₃负载量对NO氧化的影响[J]. 应用化学, 2019, 36(2): 195-202.

YANG Zhi. Effect of Different Catalyst Loadings on the Catalytic Performance of SmMn₂O₅/γ-Al₂O₃ in NO Oxidation[J]. Chinese Journal of Applied Chemistry, 2019, 36(2): 195-202.

参考文献

[1]	Ban-Weiss G A,McLaughlin J P,Harley R A,et al. Long-Term Changes in Emissions of Nitrogen Oxides and Particulate Matter from On-road Gasoline and Diesel Vehicles[J]. Atmos Environ,2008,42(2):220-232.
[2]	Pope III C A. Review: Epidemiological Basis for Particulate Air Pollution Health Standards[J]. Aerosol Sci Technol,2000,32(1):4-14.
[3]	Koebel M,Madia G,Elsener M.Selective Catalytic Reduction of NO and NO2 at Low Temperatures[J]. Catal Today,2002,73(3/4):239-247.
[4]	Koebel M,Elsener M,Madia G.Reaction Pathways in the Selective Catalytic Reduction Process with NO and NO2 at Low Temperatures[J]. Ind Eng Chem Res,2001,40(1):52-59.
[5]	Wu C,Schmidt D J,Wolverton C,et al. Accurate Coverage-Dependence Incorporated into First-principles Kinetic Models:Catalytic NO Oxidation on Pt(111)[J]. J Catal,2012,286(7):88-94.
[6]	Schmitz P J,Kudla R J,Drews A R,et al. NO Oxidation over Supported Pt:Impact of Precursor, Support, Loading, and Processing Conditions Evaluated via High Throughput Experimentation[J]. Appl Catal B,2006,67(3/4):246-256.
[7]	Xue E,Seshan K,Ross J R H. Roles of Supports, Pt Loading and Pt Dispersion in the Oxidation of NO to NO2 and of SO2 to SO3[J]. Appl Catal,B,1996,11(1):65-79.
[8]	Tang X F,Li J H,Wei L S,et al. MnOx-SnO2 Catalysts Synthesized by a Redox Coprecipitation Method for Selective Catalytic Reduction of NO by NH3[J]. Chinese J Catal,2008,29(6):531-536.
[9]	Li J,Chen J,Ke R,et al. Effects of Precursors on the Surface Mn Species and the Activities for NO Reduction over MnOx/TiO2 Catalysts[J]. Catal Commun,2007,8(12): 1896-1900.
[10]	Smirniotis P G,Sreekanth P M,Pena D A,et al. Manganese Oxide Catalysts Supported on TiO2, Al2O3, and SiO2:A Comparison for Low-temperature SCR of NO with NH3[J]. Ind Eng Chem Res,2006,45(19):6436-6443.
[11]	Zhao B,Ran R,Wu X,et al. Phase Structures, Morphologies, and NO Catalytic Oxidation Activities of Single-phase MnO2 Catalysts[J]. Appl Catal,A,2016,514:24-34
[12]	Qi G,Li W.NO Oxidation to NO2 over Manganese-Cerium Mixed Oxides[J]. Catal Today,2015,258(1):205-213.
[13]	Cui M S,Li Y,Wang X Q,et al. Effect of Preparation Method on MnOx-CeO2 Catalysts for NO Oxidation[J]. J Rare Earth,2013,31(6):572-576.
[14]	Wang W,McCool G,Kapur N,et al. Mixed-phase Oxide Catalyst Based on Mn-mullite(Sm,Gd) Mn2O5 for NO Oxidation in Diesel Exhaust[J]. Science,2012,337(6096):832-835.
[15]	Li H B,Yang Z,Liu J Y,et al. Electronic Properties and Native Point Defects of High Efficient NO Oxidation Catalysts SmMn2O5[J]. Appl Phys Lett,2016,109(21):211903.
[16]	Huang S J,Walters A B,Vannice M A.TPD, TPR and DRIFTS Studies of Adsorption and Reduction of NO on La2O3 Dispersed on Al2O3[J]. Appl Catal,B,2000,26(2):101-118.
[17]	Feng Z,Wang J,Liu X,et al. Promotional Role of La Addition in the NO Oxidation Performance of a SmMn2O5 Mullite Catalyst[J]. Catal Sci Technol,2016,6(14):5580-5589.
[18]	Machocki A,Ioannides T,Stasinska B,et al. Manganese-Lanthanum Oxides Modified with Silver for the Catalytic Combustion of Methane[J]. J Catal,2004,227(2):282-296.
[19]	Cimino S,Lisi L,De Rossi S,et al. Methane Combustion and CO Oxidation on LaAl1-xMnxO3 Perovskite-type Oxide Solid Solutions[J]. Appl Catal B,2003,43(4):397-406.
[20]	Zhu Y,Sun Y,Niu X,et al. Preparation of La-Mn-O Perovskite Catalyst by Microwave Irradiation Method and Its Application to Methane Combustion[J]. Catal Lett,2010,135(1/2):152-158.
[21]	Trawczyński J,Bielak B,Mista W O. Oxidation of Ethanol over Supported Manganese Catalysts-Effect of the Carrier[J]. Appl Catal B,2005,55(4):277-285.
[22]	Szabo V,Bassir M,Van Neste A.Perovskite-type Oxides Synthesized by Reactive Grinding: Part II: Catalytic Properties of LaCo(1-x)FexO3 in VOC Oxidation[J]. Appl Catal,B,2002,37(2):175-180
[23]	Huang L,Bassir M,Kaliaguine S.Reducibility of Co3+ in Perovskite-type LaCoO3 and Promotion of Copper on the Reduction of Co3+ in Perovskite-type Oxides[J]. Appl Surf Sci,2005,243(1-4):360-375.
[24]	Chen Z Z,Liu X,Cho K,et al. Density Functional Theory Study of the Oxygen Chemistry and NO Oxidation Mechanism on Low-index Surfaces of SmMn2O5 Mullite[J]. ACS Catal,2015,5(8):4913-4926.

负载催化剂SmMn₂O₅/γ-Al₂O₃负载量对NO氧化的影响

Effect of Different Catalyst Loadings on the Catalytic Performance of SmMn₂O₅/γ-Al₂O₃ in NO Oxidation

RichHTML

PDF

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	张毅城, 查飞, 唐小华, 常玥, 田海锋, 郭效军. 非均相催化制备有机过氧化物的研究进展[J]. 应用化学, 2023, 40(6): 769-788.
[2]	于宜辰, 张雨宸, 张耀远, 吴芹, 史大昕, 陈康成, 黎汉生. 本体金属氧化物在丙烷无氧脱氢中的研究进展[J]. 应用化学, 2023, 40(6): 789-805.
[3]	李冰, 刘军辉, 宋亚坤, 李想, 郭旭明, 熊健. 金属-有机骨架材料在催化氨硼烷水解释氢中的研究进展[J]. 应用化学, 2023, 40(3): 329-340.
[4]	王路飞, 甄蒙蒙, 沈伯雄. 贫电解液下电催化剂对调控锂硫电池性能的研究进展[J]. 应用化学, 2023, 40(2): 188-209.
[5]	曹蓉, 夏杰桢, 廖漫华, 赵路超, 赵晨, 吴琪. 单原子催化剂在电化学合成氨中的理论研究进展[J]. 应用化学, 2023, 40(1): 9-23.
[6]	张丹, 尚润梅, 赵振涛, 李君华, 邢锦娟. V/Ce-Al₂O₃催化甲醇选择性氧化制备二甲氧基甲烷[J]. 应用化学, 2022, 39(9): 1429-1436.
[7]	王显, 杨小龙, 马荣鹏, 刘长鹏, 葛君杰, 邢巍. 单原子分散的Ir-N-C燃料电池阳极抗中毒催化剂[J]. 应用化学, 2022, 39(8): 1202-1208.
[8]	刘也, 郭少波, 梁艳莉, 葛红光, 马剑琪, 刘智峰, 刘波. 核壳型纳米复合材料CuFe₂O₄@NH₂@Pt的制备及催化性能[J]. 应用化学, 2022, 39(8): 1237-1245.
[9]	张超. 单原子催化剂电催化还原二氧化碳研究进展[J]. 应用化学, 2022, 39(6): 871-887.
[10]	李世帅, 刘佳奇, 王佳一, 杨江峰. 多级孔Beta沸石合成研究进展[J]. 应用化学, 2022, 39(6): 912-926.
[11]	王岩, 张树聪, 汪兴坤, 刘志承, 王焕磊, 黄明华. 电解海水析氢反应过渡金属基催化剂的研究进展[J]. 应用化学, 2022, 39(6): 927-940.
[12]	李锋, 路世玉, 张宇, 郭丽君, 翟雪, 李翠勤. 硅烷基Schiff碱共价修饰纳米二氧化硅负载过渡金属催化乙烯齐聚性能[J]. 应用化学, 2022, 39(6): 949-959.
[13]	曹维锦, 白璐, 武兰兰, 李敬德, 宋术岩. 多壳层中空镍钴双金属磷化物纳米球用于高效电催化析氧[J]. 应用化学, 2022, 39(4): 666-672.
[14]	王雪, 王意波, 王显, 祝建兵, 葛君杰, 刘长鹏, 邢巍. 酸性电解水过程中氧析出反应的机理及铱基催化剂的研究进展[J]. 应用化学, 2022, 39(4): 616-628.
[15]	徐迪, 戴力, 姚文志, 杨光瑞, 王海荣, 宋鹏飞, 朱岩松. 烯烃聚合催化剂的研究进展[J]. 应用化学, 2022, 39(3): 355-373.