Mn1-yNiyOx的制备及其催化燃烧甲苯性能的研究

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摘要通过水热共沉淀法制备了Mn₁_-yNi_yO_x复合氧化物催化剂(y=0.1~0.5),考察掺杂Ni对Mn基氧化物在甲苯燃烧中的影响,在获得最优锰镍比例后,对其热稳定性与耐久性进行测试,然后通过XRD、N₂吸脱附、SEM、H₂-TPR以及XPS对其物理结构和氧化还原性能进行表征.结果表明,Mn和Ni在甲苯吸附和活化中产生相互作用,生成更多的Mn⁴⁺以及表面吸附氧,提供大量的反应活性位点,增强了催化氧化性能.Mn_0.8Ni_0.2O_x在甲苯催化燃烧中表现出的催化性能最好,其热稳定性与耐久性也表现优异,与MnO_x在甲苯催化燃烧中相比,其T₅₀、T₉₀分别下降12和11 ℃,在238℃即可将甲苯完全氧化,并且碳平衡值约为99%,无二次污染产生,该研究成果可为挥发性有机化合物(VOCs)催化燃烧提供更好的方式和材料.

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	周媛媛
	刘晗
	邓琳
	吴功德
	万杰
	王晓丽
	胡纯政
	于先坤
	杨晓军

关键词 ：甲苯, 锰镍催化剂, 催化氧化, 热稳定性

Abstract：Series of dual meta oxides Mn_1-yNi_yO_x (y=0.1~0.5) catalysts were prepared by hydrothermal co-precipitation to investigate the effect of nickel doping on manganese-based oxides for toluene catalytic combustion reaction. Manganese to nickel ratio was optimized and the corresponding thermal stability as well as durability performances were also evaluated. The physical structure and redox performance of the obtained catalysts were characterized through XRD, N₂ adsorption/desorption, SEM, H₂-TPR and XPS. Results revealed that strong interaction exists between Mn and Ni, which results in the generation of more high valent Mn⁴⁺ and surface adsorbed oxygen species, thus providing more reactive sites and enhancing the catalytic oxidation performance. Mn_0.8Ni_0.2O_x proposed the best toluene removal efficiency in the catalytic combustion, as well as excellent thermal stability and durability. Compared with MnO_x, its T₅₀ and T₉₀ were reduced by 12 and 11℃, respectively, demonstrating complete toluene elimination at 238℃, and the carbon balance was about 99% without secondary pollution. This work provides promising materials with practical potentials for the catalytic combustion of volatile organic compounds (VOCs) as well as new insights regarding catalyst design principles.

Key words： toluene Mn-Ni catalysts catalytic oxidation thermal stability

收稿日期: 2021-09-18

PACS:

X701.7

基金资助:国家自然科学基金资助项目(22076023);安徽省重点研发计划项目(202104g01020006);江苏省重点研发计划项目(BE2018718);江苏省基础研究计划(自然科学基金)项目(BK20201037);江苏省高等学校自然科学研究面上项目(20KJB610005);南京工程学院引进人才科研启动基金资助项目(YKJ2019111)

通讯作者: 邓琳,副教授,dlwhu@163.com;吴功德,教授,wugongde@njit.edu.cn E-mail: dlwhu@163.com;wugongde@njit.edu.cn

作者简介: 周媛媛(1997-),女,江苏南京人,东南大学硕士研究生,主要从事VOCs催化材料研究.发表论文2篇.

引用本文:

周媛媛, 刘晗, 邓琳, 吴功德, 万杰, 王晓丽, 胡纯政, 于先坤, 杨晓军. Mn_1-yNi_yO_x的制备及其催化燃烧甲苯性能的研究[J]. 中国环境科学, 2022, 42(4): 1601-1609. ZHOU Yuan-yuan, LIU Han, DENG Lin, WU Gong-de, WAN Jie, WANG Xiao-li, HU Chun-zheng, YU Xian-kun, YANG Xiao-jun. Synthesis of Mn₁_-yNi_yO_x catalyst and its high efficient performance for toluene catalytic combustion. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(4): 1601-1609.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2022/V42/I4/1601

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