无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ
催化材料

前驱体转化法可控制备γ-二氧化锰及其催化燃烧甲苯性能

  • 唐诗昌 ,
  • 程高 ,
  • 刘琪 ,
  • 叶凡 ,
  • 孙明 ,
  • 余林
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  • 广东工业大学轻工化工学院,广东省教育厅清洁化学技术重点实验室,广东 广州 510006
唐诗昌(1996— ),男,在读硕士,研究方向为环境催化与纳米材料;E-mail:1356957011@qq.com

收稿日期: 2021-11-17

  网络出版日期: 2022-06-22

基金资助

国家自然科学基金项目(21576054);广东省科技创新战略专项项目(2018A030310563);广东省自然科学基金项目(2019B1515120087);广东省普通高校基础研究与应用基础研究重点项目(2018KZDXM031)

Controllable preparation of γ-MnO2 by precursor conversion method and its catalytic combustion performance of toluene

  • Shichang TANG ,
  • Gao CHENG ,
  • Qi LIU ,
  • Fan YE ,
  • Ming SUN ,
  • Lin YU
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  • Key Laboratory of Clean Chemistry Technology of Guangdong Regular Higher Education,School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou 510006,China

Received date: 2021-11-17

  Online published: 2022-06-22

摘要

采用前驱体转化法将四氧化三锰分别与硝酸、硫酸、醋酸进行歧化反应,制备了3组γ-二氧化锰催化剂(Mn-N、Mn-S、Mn-A),研究了不同酸对产物结构和形貌的影响。通过X射线衍射(XRD)、扫描电镜(FE-SEM)、透射电镜(HR-TEM)、氮气吸附-脱附、X射线光电子能谱(XPS)、氢气程序升温还原(H2-TPR)和氧气程序升温脱附(O2-TPD)等表征方法系统分析了各产物的物化性质,并采用甲苯催化燃烧作为探针反应用于评估γ-二氧化锰催化剂的活性。结果表明,经硝酸处理得到的催化剂Mn-N具有最佳的甲苯催化燃烧活性,在质量空速为40 000 mL/(g·h)条件下,起燃温度T10(对应转化率为10%)为190 ℃,完全燃烧温度T90(对应转化率为90%)为229 ℃。这可能与其具有较大比表面积、较高的锰(Ⅲ)和吸附氧物种含量、较好的可还原性和晶格氧流动能力有关。此外,经过连续30 h的稳定性实验,Mn-N仍可保持良好的催化活性。

本文引用格式

唐诗昌 , 程高 , 刘琪 , 叶凡 , 孙明 , 余林 . 前驱体转化法可控制备γ-二氧化锰及其催化燃烧甲苯性能[J]. 无机盐工业, 2022 , 54(6) : 134 -141 . DOI: 10.19964/j.issn.1006-4990.2021-0696

Abstract

Three groups of γ-MnO2 catalysts(Mn-N,Mn-S,Mn-A) were prepared by disproportionation reaction between Mn3O4 and nitric acid,sulfuric acid,and acetic acid,respectively.The effect of different acid on the structure and morphology of the products was studied.The physical and chemical properties of the products were systematically analyzed by X-ray diffraction(XRD),scanning electron microscopy(FE-SEM),transmission electron microscopy(HR-TEM),nitrogen adsorption desorption,X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H2-TPR) and oxygen temperature programmed desorption(O2-TPD).And toluene catalytic combustion was used as a probe reaction to evaluate the activity of γ-MnO2 catalyst.The results showed that the catalyst Mn-N treated with nitric acid had the best catalytic combustion activity for toluene.Under the condition of mass space velocity of 40 000 mL/(g·h),the ignition temperature T10(corresponding conversion of 10%) was 190 ℃,and the complete combustion temperature T90(corresponding conversion of 90%) was 229 ℃.This may be related to its large specific surface area,high content of Mn(Ⅲ) and adsorbed oxygen species,good reducibility and lattice oxygen flow ability.In addition,Mn-N could still maintain good catalytic activity after continuous stability experiments for 30 h.

参考文献

1 ZOU Weixin, GAO Bin, OK Y S,et al.Integrated adsorption and photocatalytic degradation of volatile organic compounds(VOCs) using carbon?based nanocomposites:A critical review[J].Chemosphere,2019,218:845-859.
2 BAI Bingyang, QIAO Qi, LI Junhua,et al.Progress in research on catalysts for catalytic oxidation of formaldehyde[J].Chinese Journal of Catalysis,2016,37(1):102-122.
3 ZHANG Ling, PENG Yuexin, ZHANG Juan,et al.Adsorptive and catalytic properties in the removal of volatile organic compounds over zeolite?based materials[J].Chinese Journal of Catalysis,2016,37(6):800-809.
4 LI Liping, PAN Yinzhen, CHEN Lijuan,et al.One?dimensional α-MnO2:Trapping chemistry of tunnel structures,structural stability,and magnetic transitions[J].Journal of Solid State Chemistry,2007,180(10):2896-2904.
5 WANG Jian, ZHAO Hainan, SONG Jianfei,et al.Structure?activity relationship of manganese oxide catalysts for the catalytic oxidation of(chloro)-VOCs[J].Catalysts,2019,9(9).Doi:10.3390/ catal9090726 .
6 BOYJOO Y, ROCHARD G, GIRAUDON J M,et al.Mesoporous MnO2 hollow spheres for enhanced catalytic oxidation of formaldehyde[J].Sustainable Materials and Technologies,2019,20.Doi:10.1016/j.susmat.2018.e00091 .
7 WENG Xiaole, LONG Yu, WANG Wanglong,et al.Structural effect and reaction mechanism of MnO2 catalysts in the catalytic oxidation of chlorinated aromatics[J].Chinese Journal of Catalysis,2019,40(5):638-646.
8 YANG Yang, HUANG Jun, WANG Siwen,et al.Catalytic removal of gaseous unintentional POPs on manganese oxide octahedral molecular sieves[J].Applied Catalysis B:Environmental,2013,142-143:568-578.
9 JIANG Yong, CHENG Gao, YANG Runnong,et al.Influence of preparation temperature and acid treatment on the catalytic activity of MnO2 [J].Journal of Solid State Chemistry,2019,272:173- 181
10 WANG Jinlong, LI Jinge, JIANG Chuanjia,et al.The effect of manganese vacancy in birnessite?type MnO2 on room?temperature oxidation of formaldehyde in air[J].Applied Catalysis B:Environmental,2017,204:147-155.
11 YAMAGUCHI Y, AONO R, HAYASHI E,et al.Template?free
11 synthesis of mesoporous β-MnO 2 nanoparticles:Structure,formation mechanism,and catalytic properties[J].ACS Applied Materials & Interfaces,2020,12(32):36004-36013.
12 SI Wenzhe, WANG Yu, PENG Yue,et al.Selective dissolution of A-site cations in ABO3 perovskites:A new path to high?performance catalysts[J].Angewandte Chemie International Edition,2015,54(27):7954-7957.
13 ZENG Xiaohong, CHENG Gao, LIU Qi,et al.Novel ordered mesoporous γ-MnO2 catalyst for high?performance catalytic oxidation of toluene and o-xylene[J].Industrial & Engineering Chemistry Research,2019,58(31):13926-13934.
14 SI Wenzhe, WANG Yu, PENG Yue,et al.A high?efficiency ga? mma-MnO 2 -like catalyst in toluene combustion[J].Chemical Co? mmunications,2015,51(81):14977-14980.
15 DESAI M A, VEDPATHAK A S, BHAPKAR A R,et al.An investigation of chemical and electrochemical conversion of SILAR grown Mn3O4 into MnO2 thin films[J].Journal of Environmental Management,2021,299.Doi:10.1016/j.jenvman.2021.113564 .
16 PAN Jia hong, HUANG Qizhao, KOH Z Y,et al.Scalable synthesis of urchin- and flowerlike hierarchical NiO microspheres and their electrochemical property for lithium storage[J].ACS Applied Materials & Interfaces,2013,5(13):6292-6299.
17 Yue LYU, LI Caiting, DU Xueyu,et al.Catalytic oxidation of toluene over MnO2 catalysts with different Mn(Ⅱ) precursors and the study of reaction pathway[J].Fuel,2020,262.Doi:10.1016/j.fuel.2019.116610 .
18 FENG Chao, XIONG Gaoyan, LI Yaping,et al.High?precision synthesis of α-MnO2 nanowires with controllable crystal facets for propane oxidation[J].CrystEngComm,2021,23(43):7602-7614.
19 GU Wenxiu, LI Chenqi, QIU Jianhao,et al.Facile fabrication of flower?like MnO2 hollow microspheres as high?performance catalysts for toluene oxidation[J].Journal of Hazardous Materials,2021,408.Doi:10.1016/j.jhazmat.2020.124458 .
20 SHI Fengjuan, WANG Fang, DAI Hongxing,et al.Rod-,flower-,and dumbbell?like MnO2:Highly active catalysts for the combustion of toluene[J].Applied Catalysis A:General,2012,433-434:206-213.
21 LI Luming, LUO Jingjie, LIU Yuefeng,et al.Self?propagated flaming synthesis of highly active layered CuO-δ-MnO2 hybrid composites for catalytic total oxidation of toluene pollutant[J].ACS Applied Materials & Interfaces,2017,9(26):21798-21808.
22 ZHANG Chuanhui, HUANG He, LI Genqin,et al.Zeolitic acidity as a promoter for the catalytic oxidation of toluene over MnO x /HZSM-5 catalysts[J].Catalysis Today,2019,327:374-381.
23 LI Xinwei, DAI Hongxing, DENG Jiguang,et al.In situ PMMA-templating preparation and excellent catalytic performance of Co3O4/3DOM La0.6Sr0.4CoO3 for toluene combustion[J].Applied Catalysis A:General,2013,458:11-20.
24 ZHAO Jiuhu, TANG Zhicheng, DONG Fang,et al.Controlled porous hollow Co3O4 polyhedral nanocages derived from metal?organic frameworks(MOFs) for toluene catalytic oxidation[J].Molecular Catalysis,2019,463:77-86.
25 DU Yucheng, MENG Qi, WANG Jinshu,et al.Three?dimensional mesoporous manganese oxides and cobalt oxides:High?efficiency catalysts for the removal of toluene and carbon monoxide[J].Microporous and Mesoporous Materials,2012,162:199-206.
26 XIE Shaohua, DAI Hongxing, DENG Jiguang,et al.Preparation and high catalytic performance of Au/3DOM Mn2O3 for the oxidation of carbon monoxide and toluene[J].Journal of Hazardous Materials,2014,279:392-401.
27 XIE Shaohua, DAI Hongxing, DENG Jiguang,et al.Au/3DOM Co3O4:Highly active nanocatalysts for the oxidation of carbon mo?
27 noxide and toluene[J].Nanoscale,2013,5(22):11207-11219.
28 CHAN Z M, KITCHAEV D A, NELSON WEKER J,et al.Electrochemical trapping of metastable Mn3+ ions for activation of MnO2 oxygen evolution catalysts[J].Proceedings of the National Academy of Sciences of the United States of America,2018,115(23):E5261-E5268.
29 DONG Cui, QU Zhenping, JIANG Xiao,et al.Tuning oxygen vacancy concentration of MnO2 through metal doping for improved toluene oxidation[J].Journal of Hazardous Materials,2020,391.Doi:10.1016/j.jhazmat.2020.122181 .
30 JIA Jingbo, ZHANG Pengyi, CHEN Long.Catalytic decomposition of gaseous ozone over manganese dioxides with different crys?
30 tal structures[J].Applied Catalysis B:Environmental,2016,189:210-218.
31 GENUINO H C, MENG Yongtao, HORVATH D T,et al.Enhancement of catalytic activities of octahedral molecular sieve manganese oxide for total and preferential CO oxidation through vanadium ion framework substitution[J].ChemCatChem,2013,5(8):2306-2317.
32 SUN Liang, CAO Qingqing, HU Bingqing,et al.Synthesis,characterization and catalytic activities of vanadium?cryptomelane man?
32 manganese oxides in low?temperature NO reduction with NH 3[J].Applied Catalysis A:General,2011,393(1/2):323-330.
33 MO Shengpeng, ZHANG Qi, LI Jiaqi,et al.Highly efficient mesoporous MnO2 catalysts for the total toluene oxidation:Oxygen?Vacancy defect engineering and involved intermediates using in situDRIFTS[J].Applied Catalysis B:Environmental,2020,264.Doi:10.1016/j.apcatb.2019.118464 .
34 ZHANG Runduo, VILLANUEVA A, ALAMDARI H,et al.Reduction of NO by CO over nanoscale LaCo1- x Cu x O3 and LaMn1- x Cu x O3 perovskites[J].Journal of Molecular Catalysis A:Chemical,2006,258(1/2):22-34.
35 HUANG Na, QU Zhenping, DONG Cui,et al.Superior performance of α@β-MnO2 for the toluene oxidation:Active interface and oxygen vacancy[J].Applied Catalysis A:General,2018,560:
35 195-205.
36 孙梦婷,黄碧纯,马杰文,等.二氧化锰在低温NH3-SCR催化反应上的形貌效应[J].物理化学学报,2016,32(6):1501-1510.
36 SUN Mengting, HUANG Bichun, MA Jiewen,et al.Morphological effects of manganese dioxide on catalytic reactions for low?temperature NH3-SCR[J].Acta Physico-Chimica Sinica,2016,32(6):1501-1510.
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