一锅原位合成具有高效NH3-SCR催化性能和耐H2O/SO2性能的Ti/Cu-SSZ-13催化剂

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Catalysis Surveys from Asia Pub Date : 2022-09-29 DOI:10.1007/s10563-022-09374-8
Jie Wan, Jiawei Chen, Yijun Shi, Yiyan Wang, Yanjun Liu, Jin Zhang, Gongde Wu, Renxian Zhou
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引用次数: 1

摘要

采用原位一锅法制备了一系列可变钛含量Ti/Cu-SSZ-13分子筛催化剂。对所得催化剂的NH3-SCR催化性能进行了系统评价。结果表明,Ti含量合适的Ti/Cu-SSZ-13(目前的研究为Ti0.81/Cu2.15-SSZ-13)具有高效的催化活性,其工作温度窗宽从140°C扩大到540°C, N2选择性接近100%,对水蒸气和SO2具有良好的耐受性,可以作为NH3-SCR应用的候选材料。进一步的结构/物理化学表征表明,所制备的Ti/Cu-SSZ-13催化剂具有良好结晶的特征恰辉石(CHA)结构。分离Cu2+和单体Ti4+被认为是主要的活性物质,前者主要参与低温SCR反应,而后者则有利于提高高温SCR活性。Ti过掺杂会导致沸石结构部分破坏,占据Cu2+阳离子位点,形成表面聚集的TiOx,从而导致NH3-SCR性能不理想。此外,水热老化过程中形成的CuOx团块和SO2预处理过程中形成的硫酸盐堵塞表面活性位点被认为是耐受性试验中活性下降的原因。
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In-situ One-Pot Synthesis of Ti/Cu-SSZ-13 Catalysts with Highly Efficient NH3-SCR Catalytic Performance as Well as Superior H2O/SO2 Tolerability

Series of Ti/Cu-SSZ-13 zeolite catalysts with variable Ti content were prepared via convenient in-situ one-pot synthesizing strategy. Systematic evaluations of the NH3-SCR catalytic performance over the obtained catalysts were conducted. Results show that Ti/Cu-SSZ-13 with appropriate Ti content (in the current work Ti0.81/Cu2.15-SSZ-13) could serve as capable candidate for NH3-SCR application, as it exhibits highly efficient catalytic activity with expanded operation temperature window width from 140 to 540 °C, nearly 100% N2 selectivity, as well as superior tolerability against water vapor and SO2. Further structural/physicochemical characterizations demonstrate that the obtained Ti/Cu-SSZ-13 catalysts possess well-crystallized characteristic chabazite (CHA) structure. Isolated Cu2+ and monomeric Ti4+ are recognized as the primary active species, as the former mainly contributes to SCR reaction at low temperatures, while the latter are conducive for improving the high temperature SCR activity. Ti over doping would result in partial destruction of the zeolite structure, occupation of Cu2+ cation sites and formation of surface aggregated TiOx, thus leading to unsatisfactory NH3-SCR performances. Moreover, formation of agglomerated CuOx species during hydrothermal ageing and blockage of surface active sites by sulfate species formed during SO2 pretreatment are considered responsible for activity deterioration in the tolerability tests.

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来源期刊
Catalysis Surveys from Asia
Catalysis Surveys from Asia 化学-物理化学
CiteScore
4.80
自引率
0.00%
发文量
29
审稿时长
>12 weeks
期刊介绍: Early dissemination of important findings from Asia which may lead to new concepts in catalyst design is the main aim of this journal. Rapid, invited, short reviews and perspectives from academia and industry will constitute the major part of Catalysis Surveys from Asia . Surveys of recent progress and activities in catalytic science and technology and related areas in Asia will be covered regularly as well. We would appreciate critical comments from colleagues throughout the world about articles in Catalysis Surveys from Asia . If requested and thought appropriate, the comments will be included in the journal. We will be very happy if this journal stimulates global communication between scientists and engineers in the world of catalysis.
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