Effect of citric acid complexation on the structure and NH3-SCR performance of CuCe/ZSM-5 catalysts

IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Zhi-Hao Wei, Xu-Long Li, Shu-Feng Wu, Xiao-Tong Feng, Jun-Qiang Liu, Xing-Yu Liu, Zhang Zhang
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引用次数: 0

Abstract

Citric acid-assisted CuCe/ZSM-5 catalysts with different Ce loadings were prepared by an incipient wetness impregnation method and evaluated for the selective catalytic reduction of NOx with NH3 (NH3-SCR). Among the prepared catalysts, the sample containing 1.5 wt% Ce exhibited the highest NO conversion over a broad temperature window, while citric acid modification further enhanced the low-temperature catalytic activity. Characterization results revealed that Ce incorporation regulated the textural properties and the distribution of active species while preserving the ZSM-5 framework. XPS, UV–vis DRS, and H2-TPR analyses indicate the coexistence of Cu2⁺/Cu⁺ and Ce4⁺/Ce3⁺ species and support a strong redox interaction between Cu and Ce, which contributes to the enhanced redox capability of the catalysts. Meanwhile, NH3-TPD and NO-TPD results confirmed that Ce addition and citric acid modification enhanced NH3 adsorption and NO activation, thereby promoting the NH3-SCR reaction. Moreover, the optimized catalyst exhibited excellent resistance to H2O and SO2 poisoning and maintained stable catalytic performance during a 120 h continuous stability test. The superior catalytic performance is mainly attributed to the synergistic interaction between Cu and Ce species together with the dispersion regulation induced by citric acid, which contributes to enhanced redox properties, suitable surface acidity, and improved accessibility of active sites.

柠檬酸络合对CuCe/ZSM-5催化剂结构及NH3-SCR性能的影响
采用初湿浸渍法制备了不同Ce载量的柠檬酸辅助CuCe/ZSM-5催化剂,并对NH3选择性催化还原NOx的性能进行了评价。在所制备的催化剂中,含有1.5 wt% Ce的样品在宽温度窗内的NO转化率最高,而柠檬酸改性进一步提高了低温催化活性。表征结果表明,Ce的掺入调节了ZSM-5的结构性质和活性物质的分布,同时保持了ZSM-5的骨架结构。XPS、UV-vis DRS和H2-TPR分析表明Cu2 + /Cu +和Ce4 + /Ce3 +共存,Cu和Ce之间存在强的氧化还原相互作用,这有助于增强催化剂的氧化还原能力。同时,NH3- tpd和NO- tpd结果证实,Ce的加入和柠檬酸改性增强了NH3的吸附和NO的活化,从而促进了NH3- scr反应。此外,优化后的催化剂具有优异的抗H2O和SO2中毒性能,并在120 h的连续稳定性测试中保持稳定的催化性能。优异的催化性能主要是由于Cu和Ce之间的协同作用以及柠檬酸诱导的分散调节,从而增强了氧化还原性能,适宜的表面酸度,提高了活性位点的可及性。
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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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