One-pot synthesis, characterization and ammonia-selective catalytic reduction performance of MnSAPO-18 molecular sieves
One-pot synthesis, characterization and ammonia-selective catalytic reduction performance of MnSAPO-18 molecular sieves
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MnSAPO-18分子筛的一锅法合成、表征及氨选择性催化还原性能
DOI：
10.1016/j.jclepro.2021.130163
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发表时间：
2021-12
影响因子：
11.1
通讯作者：
Chenglong Yu
中科院分区：
文献类型：
--
作者：
Chunhuo Zhou;Xiang Tu;Xuehui Jia;Zhiyong Zhong;Guorong Ni;Zunkang Zhao;Jingxian Li;Hong Huang;Changwei Zou;Bichun Huang;Chenglong Yu
采用一锅法制备了高结晶度的MnSAPO-18催化剂，并将其用于烟气脱硫反应中的NO脱除。在MnSAPO-18的可控合成过程中，考察了Mn含量、有机胺模板剂、Mn前驱体以及水热晶化时间对MnSAPO-18催化剂SCR性能的影响，并对样品的结构与活性关系进行了研究。在水热合成过程中，这些变量的最佳组合似乎是使用N，N-二异丙基乙胺作为有机模板剂，醋酸锰作为Mn的前体，晶化时间为24 h，在合成凝胶中Mn含量为n（MnO）/n（Al 2 O3）= 0.2。最佳的Mn0.2SAPO-18-2催化剂在275-375 °C的温度范围内表现出接近95%的NOx转化率和90%的N2选择性，空速为37，500 h-1。在低成本晶种辅助的一锅法合成Mn 0.2SAPO-18-1. 0 DIPEA-Seed中，发现该样品具有与传统一锅法中的Mn 0.2SAPO-18-2几乎相当的活性。采用H_2-TPR、NH_3-TPD、XRD、FESEM、DR UV-Vis和ESR等手段对催化剂进行了表征。结果表明，Mn 0. 2SAPO-18-2的最佳SCR性能与其丰富的高价骨架锰、适宜的表面酸性和高的氧化还原能力密切相关。因此，Mn0.2SAPO-18-2是一种很有前途的NH3-SCR脱硝催化剂，该制备技术具有潜在的工业应用价值。
A one-pot synthetic method was used to prepare novel MnSAPO-18 catalysts with high crystallinity that were employed to efficiently scrub NOxin 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(Al2O3) = 0.2 in the synthesis gel. The optimum Mn0.2SAPO-18-2 catalyst exhibited nearly 95% NOxconversion and 90% N2selectivity 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 Mn0.2SAPO-18-1.0DIPEA-Seed, it was found that this sample had almost comparable activity as the Mn0.2SAPO-18-2 in the traditional one-pot method. These novel catalysts were characterized using the H2-TPR, NH3-TPD, XRD, FESEM, DR UV–Vis and ESR analysis. The results of these characterizations showed that the optimum SCR performance of Mn0.2SAPO-18-2 was closely related to its abundant high valence framework manganese, suitable surface acidity and high redox capability. Thus, Mn0.2SAPO-18-2 was shown to be a promising catalyst for NH3-SCR removal of NOxand this fabrication technique appeared to be potentially valuable for application in industry.
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