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通过一锅溶胶-凝胶法制备介孔Mn-Ce-Ti-O气凝胶用于NH3选择性催化还原NO

Preparation of Mesoporous Mn-Ce-Ti-O Aerogels by a One-Pot Sol-Gel Method for Selective Catalytic Reduction of NO with NH.

作者信息

Wei Yabin, Jin Shuangling, Zhang Rui, Li Weifeng, Wang Jiangcan, Yang Shuo, Wang He, Yang Minghe, Liu Yan, Qiao Wenming, Ling Licheng, Jin Minglin

机构信息

School of Materials Science and Engineering, Shanghai Institute of Technology, Shanghai 201418, China.

State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.

出版信息

Materials (Basel). 2020 Jan 19;13(2):475. doi: 10.3390/ma13020475.

DOI:10.3390/ma13020475
PMID:31963836
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7013643/
Abstract

Novel Mn-Ce-Ti-O composite aerogels with large mesopore size were prepared via a one-pot sol-gel method by using propylene oxide as a network gel inducer and ethyl acetoacetate as a complexing agent. The effect of calcination temperature (400, 500, 600, and 700 °C) on the NH-selective catalytic reduction (SCR) performance of the obtained Mn-Ce-Ti-O composite aerogels was investigated. The results show that the Mn-Ce-Ti-O catalyst calcined at 600 °C exhibits the highest NH-SCR activity and lowest apparent activation energy due to its most abundant Lewis acid sites and best reducibility. The NO conversion of the MCTO-600 catalyst maintains 100% at 200 °C in the presence of 100 ppm SO, showing the superior resistance to SO poisoning as compared with the MnO-CeO-TiO catalysts reported the literature. This should be mainly attributed to its large mesopore sizes with an average pore size of 32 nm and abundant Lewis acid sites. The former fact facilitates the decomposition of NHHSO, and the latter fact reduces vapor pressure of NH. The NH-SCR process on the MCTO-600 catalyst follows both the Eley-Rideal (E-R) mechanism and the Langmuir-Hinshelwood (L-H) mechanism.

摘要

通过一锅溶胶 - 凝胶法，以环氧丙烷作为网络凝胶诱导剂、乙酰乙酸乙酯作为络合剂，制备了具有大介孔尺寸的新型Mn - Ce - Ti - O复合气凝胶。研究了煅烧温度（400、500、600和700℃）对所得Mn - Ce - Ti - O复合气凝胶的NH₃选择性催化还原（SCR）性能的影响。结果表明，在600℃煅烧的Mn - Ce - Ti - O催化剂表现出最高的NH₃ - SCR活性和最低的表观活化能，这归因于其最丰富的Lewis酸位点和最佳的还原性。在100 ppm SO₂存在下，MCTO - 600催化剂在200℃时的NO转化率保持100%，与文献报道的MnO - CeO₂ - TiO₂催化剂相比，显示出优异的抗SO₂中毒性能。这主要归因于其平均孔径为32 nm的大介孔尺寸和丰富的Lewis酸位点。前者有利于NH₄HSO₄的分解，后者降低了NH₃的蒸气压。MCTO - 600催化剂上的NH₃ - SCR过程遵循Eley - Rideal（E - R）机理和Langmuir - Hinshelwood（L - H）机理。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0860/7013643/28f60e7755b1/materials-13-00475-g012.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0860/7013643/98707f14432d/materials-13-00475-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0860/7013643/2fd51291b80f/materials-13-00475-g007a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0860/7013643/023fd2cf10e2/materials-13-00475-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0860/7013643/db209e549f8a/materials-13-00475-g009.jpg
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