基于泡沫镍的MnO<sub>2</sub>整体式催化剂构筑及其催化氧化甲苯性能研究

赵朴臻; 柳楚; 黄前霖; 吕路

doi:10.13205/j.hjgc.202304010

基于泡沫镍的MnO₂整体式催化剂构筑及其催化氧化甲苯性能研究

doi: 10.13205/j.hjgc.202304010

赵朴臻¹,
柳楚²,
黄前霖¹,
吕路^1, ,

1. 南京大学环境学院污染控制与资源化研究国家重点实验室, 南京 210046;
2. 江西省九江市生态环境应急预警管控中心, 江西九江 332000

基金项目:

国家重大科技专项(2017ZX07204001)

详细信息

作者简介:
赵朴臻(1997-),男,硕士,主要研究方向为环境催化材料。854381829@qq.com

通讯作者:
吕路(1975-),男,教授,主要研究方向为环境功能材料及污染控制技术。esellu@nju.edu.cn

计量
- 文章访问数: 88
- HTML全文浏览量: 1
- PDF下载量: 13
- 被引次数: 0
出版历程
- 收稿日期: 2022-05-14
- 网络出版日期: 2023-05-26
- 刊出日期: 2023-04-01

FABRICATION OF NICKEL FOAM BASED MnO₂ MONOLITHIC CATALYSTS AND ITS APPLICATION IN CATALYTIC ELIMINATION OF TOLUENE

1. State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, Nanjing 210046, China;
2. Jiujiang Ecological Environment Early Warning Emergency Control Center, Jiujiang 332000, China

摘要

摘要: 开发兼具良好催化活性和优异稳定性的整体式催化剂是VOCs催化燃烧技术工业化应用的关键。传统的整体式催化剂通过在陶瓷载体上进行涂覆、浸渍等工艺制备而成,会导致活性组分分布不均、利用率低甚至失活等问题,从而降低整体式催化剂的性能。因此,利用泡沫镍与KMnO₄之间的氧化还原反应,原位合成了MnO₂整体式催化剂MnO₂/NF-IS,考察了其催化氧化甲苯的性能,并通过XRD、SEM、TEM、H₂-TPR、O₂-TPD、XPS等手段对催化剂进行表征,并对MnO₂/NF-IS催化氧化甲苯的反应路径进行探究。结果表明:基于泡沫镍原位合成的MnO₂/NF-IS具有最佳的催化性能 (T₉₀=248 ℃),优于粉末催化剂MnO₂ (T₉₀=271 ℃) 以及涂覆法制备的整体式催化剂MnO₂/NF-WC (T₉₀=293 ℃)。通过表征发现,MnO₂/NF-IS具有特殊的多孔纳米片阵列的形貌和更高的氧空位含量,这可能是其性能优势的重要原因。研究成果为制备基于泡沫镍的MnO₂整体式催化剂提供了新思路。
- MnO₂ /
- 泡沫镍 /
- VOCs /
- 催化氧化 /
- 纳米阵列 /
- 整体式催化剂
Abstract: The crucial point of the industrial application of VOCs catalytic oxidation is to develop efficient and stable monolithic catalysts. Traditional monolithic catalysts were prepared by coating and impregnating the ceramic carrier, which led to uneven distribution of active components, low utilization rate, and even deactivation, thereby reducing the performance of monolithic catalysts. In this study, a MnO₂ monolithic catalyst (MnO₂/NF-IS) was prepared in situ by the redox reaction between nickel foam and KMnO₄. The catalytic performance of the as-obtained catalysts for toluene oxidation was investigated. Besides, the catalysts were characterized by XRD, SEM, TEM, H₂-TPR, O₂-TPD, and XPS, and the degradation pathway of toluene oxidation was investigated. It has been shown that MnO₂/NF-IS had a special structure of porous nanosheet arrays and abundant oxygen vacancies, delivering the best performance for toluene oxidation (T₉₀=248 ℃), which was better than that of powder MnO₂ (T₉₀=271 ℃) as well as the integrated MnO₂/NF-WC (T₉₀=293 ℃) prepared by the coating method. Therefore, a new strategy for the synthesis of MnO₂ monolithic catalysts was provided in this study.
- MnO₂ /
- nickel foam /
- VOCs /
- catalytic oxidation /
- nanoarray /
- monolithic catalyst

HTML全文

参考文献(15)

[1]	GUO Y L, WEN M C, LI G Y, et al. Recent advances in VOC elimination by catalytic oxidation technology onto various nanoparticles catalysts: a critical review[J]. Applied Catalysis B: Environmental, 2021, 281: 119447.
[2]	POSCHL U, SHIRAIWA M. Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene[J]. Chem Rev, 2015, 115(10): 4440-4475.
[3]	KONG J J, YANG T, RUI Z B, et al. Perovskite-based photocatalysts for organic contaminants removal: current status and future perspectives[J]. Catalysis Today, 2019, 327: 47-63.
[4]	SŁOMIŃSKA M, KRÓL S, NAMIEŚNIK J. Removal of BTEX compounds from waste gases; destruction and recovery techniques[J]. Critical Reviews in Environmental Science and Technology, 2013, 43(14): 1417-1445.
[5]	王小强, 杨宁, 徐力, 等. 铁锰基整体式催化剂催化燃烧甲苯和氯苯的性能[J]. 中国环境科学, 2022: 1-12.
[6]	ZHANG Q, WU D F. Mechanical stability of monolithic catalysts: the influence mechanism of primer on the washcoat adhesion to the metallic substrates[J]. ChemistrySelect, 2019, 4(11): 3214-3221.
[7]	LU X X, TANG W X, LI M L, et al. Mass transport in nanoarray monolithic catalysts: an experimental-theory study[J]. Chemical Engineering Journal, 2021, 405: 126906.
[8]	JIANG X D, XU W C, LAI S F, et al. Integral structured Co-Mn composite oxides grown on interconnected Ni foam for catalytic toluene oxidation[J]. RSC Advances, 2019, 9(12): 6533-6541.
[9]	ZHANG Q, MO S P, CHEN B X, et al. Hierarchical Co₃O₄ nanostructures in-situ grown on 3D nickel foam towards toluene oxidation[J]. Molecular Catalysis, 2018, 454: 12-20.
[10]	ZHANG X D, LV X T, BI F K, et al. Highly efficient Mn₂O₃ catalysts derived from Mn-MOFs for toluene oxidation: the influence of MOFs precursors[J]. Molecular Catalysis, 2020, 482: 110701.
[11]	YANG W H, SU Z A, XU Z H, et al. Comparative study of α-, β-, γ-and δ-MnO₂ on toluene oxidation: oxygen vacancies and reaction intermediates[J]. Applied Catalysis B: Environmental, 2020, 260: 118150.
[12]	YANG W H, PENG Y, WANG Y, et al. Controllable redox-induced in-situ growth of MnO₂ over Mn₂O₃ for toluene oxidation: active heterostructure interfaces[J]. Applied Catalysis B: Environmental, 2020, 278: 119279.
[13]	MO S P, ZHANG Q, REN Q M, et al. Leaf-like Co-ZIF-L derivatives embedded on Co₂AlO₄/Ni foam from hydrotalcites as monolithic catalysts for toluene abatement[J]. J Hazard Mater, 2019, 364: 571-580.
[14]	WANG J, YOSHIDA A, WANG P F, et al. Catalytic oxidation of volatile organic compound over cerium modified cobalt-based mixed oxide catalysts synthesized by electrodeposition method[J]. Applied Catalysis B: Environmental, 2020, 271: 118941.
[15]	吴宇昊, 张健, 龙超. MCM-41孔径对负载MnO_<em>x催化氧化甲苯性能的影响[J]. 环境科学学报, 2022, 42(3): 1-10. ZHAO Q, ZHENG Y F, SONG C F, et al. Novel monolithic catalysts derived from in-situ decoration of Co₃O₄ and hierarchical Co₃O₄@MnO_<em>x on Ni foam for VOC oxidation[J]. Applied Catalysis B: Environmental, 2020, 265: 118552.[16] ZHAO Y X, CHANG C, TENG F, et al. Defect-engineered ultrathin δ-MnO₂ nanosheet arrays as bifunctional electrodes for efficient overall water splitting[J]. Advanced Energy Materials, 2017, 7(18): 1700005. [17] MO S P, ZHANG Q, LI J Q, et al. Highly efficient mesoporous MnO₂ catalysts for the total toluene oxidation: oxygen-vacancy defect engineering and involved intermediates using in situ DRIFTS[J]. Applied Catalysis B: Environmental, 2020, 264: 110701. [18] ZHENG Y F, LIU Q L, SHAN C P, et al. Defective ultrafine MnO_<em>x nanoparticles confined within a carbon matrix for low-temperature oxidation of volatile organic compounds[J]. Environ Sci Technol, 2021, 55(8): 5403-5411. [19] SU Z, YANG W H, WANG C Z, et al. Roles of oxygen vacancies in the bulk and surface of CeO₂ for toluene catalytic combustion[J]. Environ Sci Technol, 2020, 54(19): 12684-12692. [20] LIAO H Y, GUO X Z, HOU Y, et al. Construction of defect-rich Ni-Fe-doped K_0.23 MnO₂ cubic nanoflowers via etching prussian blue analogue for efficient overall water splitting[J]. Small, 2020, 16(10): 1905223. [21] ZHAO Y F, ZHANG J Q, WU W J, et al. Cobalt-doped MnO₂ ultrathin nanosheets with abundant oxygen vacancies supported on functionalized carbon nanofibers for efficient oxygen evolution[J]. Nano Energy, 2018, 54: 129-137. [22] SONG L L, DUAN Y P, HE G H, et al. Enhanced thermal stability and dielectric performance of δ-MnO₂ by Ni²⁺ doping[J]. Journal of Materials Science: Materials in Electronics, 2019, 30(16): 15362-15370. [23]