Ultra-low temperature selective catalytic reduction of NOx into N2 by micron spherical CeMnOx in high-humidity atmospheres containing SO2

Xixi Chen, Peng Gao, Ling Huang, Yongji Hu, Jianhai Wang, Zonghang Liu, Yuesong Shen
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Abstract

The solvothermal synthesis of optimized micron-sized spherical CeMnO-350 yields remarkable results in ultra-low temperature NH-SCR of NO, with over 91 % NO conversion achieved between 59 and 255 ℃. Notably, under 5 vol% HO and 50 ppm SO, the CeMnO maintains NO conversion >99 % at 127 ℃ for extended periods, surpassing current ultra-low temperature deNO standards. This superior performance is attributed to the material's unique characteristics: the regular and porous surface morphology enhances exposure to active sites, particularly MnO(112) facets crucial for ultra-low temperature deNO, while the rough and loose surface and high MnO(222) exposure mitigate water vapor and SO poisoning. Furthermore, the thermal storage effect of the MnO/MnO system within CeMnO facilitates rapid thermal dissipation and ammonium sulfite decomposition. This process is further augmented by the pores, which aid in the confinement of deNO reaction heat and facilitate the flushing of flowing flue gas, thereby impeding the formation of ammonium bisulfate.
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在含有二氧化硫的高湿度大气中,微米球形氧化锰通过超低温选择性催化将氮氧化物还原为 N2
溶热合成优化的微米级球形 CeMnO-350 在超低温 NH-SCR 脱硝方面取得了显著效果,在 59 至 255 ℃ 之间实现了超过 91% 的氮氧化物转化率。值得注意的是,在 5 vol% HO 和 50 ppm SO 的条件下,CeMnO 在 127 ℃ 时的氮氧化物转化率长期保持在 99% 以上,超过了目前的超低温脱硝标准。这种优异的性能归功于材料的独特特性:规则多孔的表面形态增强了活性位点的暴露,尤其是对超低温脱硝至关重要的 MnO(112) 面,而粗糙松散的表面和高 MnO(222) 暴露则减轻了水蒸气和 SO 的毒害。此外,CeMnO 中 MnO/MnO 系统的蓄热效应有助于快速散热和亚硫酸铵分解。孔隙进一步加强了这一过程,有助于封闭脱硝反应热,并促进流动烟气的冲洗,从而阻碍硫酸氢铵的形成。
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