Construction of mesoporous amorphous Smα-MnTiOx with high deNOx performance and sulfur Tolerance: Insight into the synergistic Sulfur-Resistant effect between Manganese-Samarium species

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-08-14 Epub Date: 2025-02-10 DOI:10.1016/j.seppur.2025.132030
Xuewu Hou , Jitong Wang , Cheng Ma , Wenming Qiao , Licheng Ling
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Abstract

Low-temperature SCR denitrification technology requires catalysts with both NOx oxidation and NH3 adsorption capabilities. However, most catalysts, such as MnOx and MnO2/TiO2, with the problems of narrow activity temperature windows and low sulfur resistance. Herein, the mesoporous amorphous oxide catalysts Smα-MnTiOx are successfully synthesized by a solvothermal method. The catalyst displays excellent low-temperature activity and sulfur tolerance, with a denitrification conversion of over 90 % within the range of 160°C to 350°C. Furthermore, the denitrification conversion wasis maintained at more than 98 % for 8 h at 250°C and 50 ppm SO2 atmosphere. The reducibility capacity and surface acidity of Smα-MnTiOx catalysts are improve by the doping of Sm, thus facilitating the adsorption and activation of NH3 and O2, which is beneficial for the improvement of catalytic activity. The in-situ DRIFTS shows the abundant chemisorbed oxygen on the surface of Smα-MnTiOx favors NO2 generation, and the doping of Sm extended the temperature range of NO2 (50–250 ℃),which promotes the reaction towards the Fast-SCR reaction pathway at low temperatures. The combined effect of E-R mechanism and Fast-SCR reaction successfully broaden the denitration temperature window of Smα-MnTiOx catalysts. Furthermore, the interaction between Mn and Sm species effectively inhibits the electron transfer from Mn to SO2, which reduces the generation of metal sulfate and protects the active sites of the catalyst. This study provides new ideas for the improvement of denitrification catalysts with sulfur tolerance, water resistance and upper and lower catalytic activity.

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具有高脱氧性能和耐硫性能的介孔无定形Smα-MnTiOx的构建:锰-钐协同抗硫效应的洞察
低温SCR脱硝技术要求催化剂同时具备NOx氧化和NH3吸附能力。然而,大多数催化剂,如MnOx和MnO2/TiO2,存在活性温度窗窄、耐硫性低等问题。本文采用溶剂热法成功合成了介孔非晶氧化物催化剂Smα-MnTiOx。该催化剂表现出优异的低温活性和耐硫性能,在160℃~ 350℃范围内,脱硝转化率达90% %以上。此外,在250°C和50 ppm SO2气氛下,脱硝转化率保持在98 %以上,持续8 h。Sm的掺杂提高了Smα- mntiox催化剂的还原性和表面酸度,有利于NH3和O2的吸附和活化,有利于催化活性的提高。原位漂移表明,Smα- mntiox表面丰富的化学吸附氧有利于NO2的生成,Sm的掺杂延长了NO2的温度范围(50-250℃),促进了反应在低温下向快速scr反应途径发展。E-R机制和Fast-SCR反应的共同作用成功地拓宽了Smα-MnTiOx催化剂的脱硝温度窗。此外,Mn和Sm之间的相互作用有效地抑制了Mn向SO2的电子转移,从而减少了金属硫酸盐的生成,保护了催化剂的活性位点。该研究为改进具有耐硫、耐水和上下催化活性的脱硝催化剂提供了新的思路。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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