树莓状 MnOx/Cu-SSZ-13 催化剂:同时去除烟尘和氮氧化物的简便制备、催化性能和反应机理

IF 6.7 1区 工程技术 Q2 ENERGY & FUELS
Fuel Pub Date : 2024-11-25 DOI:10.1016/j.fuel.2024.133862
Lanyi Wang , Mengxia You , Xinyu Chen , Shengran Zhou , Dong Li , Di Yu , Chunlei Zhang , Siyu Gao , Xuehua Yu , Bing Liu , Xiaoqiang Fan , Chengyang Yin , Zhen Zhao
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引用次数: 0

摘要

采用蒸汽辅助法和浸渍法合成了具有树莓状形状的 n%MnOx/Cu-SSZ-13 催化剂。结果表明,40%MnOx/Cu-SSZ-13 催化剂的催化活性最好,烟尘燃烧的 Tm 温度最低(455 ℃),NO 转化的温度窗口最宽(144-417 ℃)(90%),N2 选择性最高(96%)。由于催化剂具有丰富的活性氧物种、充足的酸性位点、优异的氧化还原特性、高比例的表面 Mn4+以及独特的覆盆子状结构,因此所获得的催化剂能够在柴油车尾气排放温度范围内高效消除氮氧化物和烟尘。此外,还根据密度泛函理论(DFT)计算和原位漫反射红外傅里叶变换光谱(DRIFTs)的结果,阐明了参与去除烟尘和氮氧化物的活性位点及反应机理。结果表明,Mn2O3 是烟尘氧化的活性相,而 Cu-SSZ-13 则是 NH3 选择性催化还原(NH3-SCR)活性相的最佳选择。Mn2O3 的存在促进了 Cu-SSZ-13 上 NO 的还原。此外,40%MnOx/Cu-SSZ-13 催化剂在低温 NH3-SCR 中遵循 E-R 机制,在高温烟尘燃烧中遵循 NO2 辅助机制和活性氧机制。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Raspberry-like shape MnOx/Cu-SSZ-13 catalysts: Facile preparation, catalytic performance and reaction mechanism for the simultaneous removal of soot and NOx

Raspberry-like shape MnOx/Cu-SSZ-13 catalysts: Facile preparation, catalytic performance and reaction mechanism for the simultaneous removal of soot and NOx
n%MnOx/Cu-SSZ-13 catalysts with raspberry-like shapes were synthesized using the steam-assisted method and incipient impregnation methods. The catalytic activities of as-prepared catalysts were also tested for the simultaneous removal of soot and nitrogen oxides (NOx), and the 40 %MnOx/Cu-SSZ-13 catalyst exhibited the best catalytic performance with the lowest Tm temperature (455 °C) for soot combustion, the widest temperature window (144–417 °C) for NO conversion (>90 %), and the highest N2 selectivity (96 %). The obtained catalyst achieves the efficient elimination of NOx and soot in the temperature range of diesel vehicle exhaust emissions because of its rich active oxygen species, sufficient acidic sites, excellent redox properties, high proportion of surface Mn4+, and unique raspberry-like structure. Moreover, the active sites involved in the removal of soot and NOx and reaction mechanism were also elucidated according to the results of density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs). The results shows that Mn2O3 is the active phase for soot oxidation, while Cu-SSZ-13 is the best choice of active phase for NH3 selective catalytic reduction (NH3-SCR). And the existence of Mn2O3 promotes the reduction of NO on Cu-SSZ-13. Additionally, the 40 %MnOx/Cu-SSZ-13 catalyst followed the E-R mechanism in NH3-SCR at low temperatures as well as NO2-assisted mechanism and the active oxygen mechanism in soot combustion at high temperatures.
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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