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One-pot synthesis, characterization and ammonia-selective catalytic reduction performance of MnSAPO-18 molecular sieves

分子筛 催化作用 结晶度 选择性催化还原 氮氧化物 水热合成 空间速度 结晶 氧化还原 化学 无机化学 一锅法合成 选择性 热液循环 化学工程 有机化学 材料科学 燃烧 结晶学 工程类
作者
Chunhuo Zhou,Xiang Tu,Xuehui Jia,Zhiyong Zhong,Guorong Ni,Zunkang Zhao,Jingxian Li,Hong Huang,Changwei Zou,Bichun Huang,Chenglong Yu
出处
期刊:Journal of Cleaner Production [Elsevier BV]
卷期号:336: 130163-130163 被引量:9
标识
DOI:10.1016/j.jclepro.2021.130163
摘要

A one-pot synthetic method was used to prepare novel MnSAPO-18 catalysts with high crystallinity that were employed to efficiently scrub NO x in the flue-gas denitration reaction. In the controllable synthesis of MnSAPO-18, the effect of Mn content, organic amine templates, Mn precursors as well as hydrothermal crystallization time on the SCR performance of the resulting MnSAPO-18 catalysts and the structure-activity relationship of these samples was also investigated. The optimum combination of these variables in the hydrothermal synthesis process appeared to be using N,N-Diisopropylethylamine as the organic templates, manganese acetate as the Mn precursor, a crystallization time of 24 h and Mn content of n(MnO)/n(Al 2 O 3 ) = 0.2 in the synthesis gel. The optimum Mn 0.2 SAPO-18-2 catalyst exhibited nearly 95% NO x conversion and 90% N 2 selectivity in temperature range of 275–375 °C with a space velocity of 37,500 h −1 . In the low-cost seed-assisted, one-pot synthesis of Mn 0.2 SAPO-18-1.0DIPEA-Seed, it was found that this sample had almost comparable activity as the Mn 0.2 SAPO-18-2 in the traditional one-pot method. These novel catalysts were characterized using the H 2 -TPR, NH 3 -TPD, XRD, FESEM, DR UV–Vis and ESR analysis. The results of these characterizations showed that the optimum SCR performance of Mn 0.2 SAPO-18-2 was closely related to its abundant high valence framework manganese, suitable surface acidity and high redox capability. Thus, Mn 0.2 SAPO-18-2 was shown to be a promising catalyst for NH 3 -SCR removal of NO x and this fabrication technique appeared to be potentially valuable for application in industry. • MnSAPO-18 molecular sieves were synthesized by one-pot synthesis method. • The preparation and properties of MnSAPO-18 molecular sieves are outlined. • Mn 0.2 SAPO-18-2 and Mn 0.2 SAPO-18-1.0DIPEA-Seed samples exhibited high SCR activity. • Mn species in the Mn 0.2 SAPO-18 catalyst was mainly in the form of Mn 4+ .
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