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一种用于低温选择性催化还原NO的高固含量高性能Mn/TiO催化剂。

A High-Performance Mn/TiO Catalyst with a High Solid Content for Selective Catalytic Reduction of NO at Low-Temperatures.

作者信息

Yang Lei, Wang Zhen, Xu Bing, Hu Jie, Pan Dehua, Fan Guozhi, Zhang Lei, Zhou Ziyang

机构信息

Hubei Provincial Engineering Technology Research Center of Agricultural and Sideline Resources, Chemical Engineering and Utilization, School of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China.

出版信息

Molecules. 2024 Jul 24;29(15):3467. doi: 10.3390/molecules29153467.

DOI:10.3390/molecules29153467
PMID:39124872
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11313882/
Abstract

Mn/TiO catalysts with varying solid contents were innovatively prepared by the sol-gel method and were used for selective catalytic reduction of NO at low temperatures using NH (NH-SCR) as the reducing agent. Surprisingly, it was found that as the solid content of the sol increased, the catalytic activity of the developed Mn/TiO catalyst gradually increased, showing excellent catalytic performance. Notably, the Mn/TiO (50%) catalyst demonstrates outstanding denitration performance, achieving a 96% NO conversion rate at 100 °C under a volume hourly space velocity (VHSV) of 24,000 h, while maintaining high N selectivity and stability. It was discovered that as the solid content increased, the catalyst's specific surface area (SSA), surface Mn concentration, chemisorbed oxygen, chemisorption of NH, and catalytic reducibility all improved, thereby enhancing the catalytic efficiency of NH-SCR in degrading NO. Moreover, NH at the Lewis acidic sites and NH at the Bronsted acidic sites of the catalyst were capable of reacting with NO. Conversely, NO and NO adsorbed on the catalyst, along with bidentate and monodentate nitrates, were unable to react with NH at low temperatures. Consequently, the developed catalyst's low-temperature catalytic reaction mechanism aligns with the E-R mechanism.

摘要

通过溶胶-凝胶法创新性地制备了具有不同固体含量的Mn/TiO催化剂,并将其用于以NH₃(NH₃-SCR)作为还原剂的低温选择性催化还原NO。令人惊讶的是,发现随着溶胶固体含量的增加,所制备的Mn/TiO催化剂的催化活性逐渐提高,表现出优异的催化性能。值得注意的是,Mn/TiO(50%)催化剂展现出出色的脱硝性能,在体积空速(VHSV)为24,000 h⁻¹的条件下,于100℃时实现了96%的NO转化率,同时保持了高N₂选择性和稳定性。研究发现,随着固体含量的增加,催化剂的比表面积(SSA)、表面Mn浓度、化学吸附氧、NH₃的化学吸附以及催化还原能力均得到改善,从而提高了NH₃-SCR降解NO的催化效率。此外,催化剂Lewis酸性位点上的NH₃和Bronsted酸性位点上的NH₃能够与NO反应。相反,吸附在催化剂上的NO和NO₂以及双齿和单齿硝酸盐在低温下无法与NH₃反应。因此,所制备催化剂的低温催化反应机理符合E-R机理。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/0cb1636f7db9/molecules-29-03467-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/07122da7854f/molecules-29-03467-g001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/c4c6f474b208/molecules-29-03467-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/f01f24968e2f/molecules-29-03467-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/edacdcf555d1/molecules-29-03467-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/2dbbed3c4403/molecules-29-03467-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/99313f44d040/molecules-29-03467-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/6a99226bec99/molecules-29-03467-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/0cb1636f7db9/molecules-29-03467-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/07122da7854f/molecules-29-03467-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/05c42954ea07/molecules-29-03467-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/c4c6f474b208/molecules-29-03467-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/f01f24968e2f/molecules-29-03467-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/edacdcf555d1/molecules-29-03467-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/2dbbed3c4403/molecules-29-03467-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/99313f44d040/molecules-29-03467-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/6a99226bec99/molecules-29-03467-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/210f/11313882/0cb1636f7db9/molecules-29-03467-g009.jpg

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