Toward rational design of a novel hierarchical porous Cu-SSZ-13 catalyst with boosted low-temperature NOx reduction performance

被引:39
作者
Peng, Cheng [1 ]
Yan, Ran [1 ]
Mi, Yangyang [1 ]
Li, Gang [1 ]
Zheng, Yuling [1 ]
Luo, Yiwei [1 ]
Liang, Jian [1 ]
Liu, Wenming [1 ]
Li, Zhenguo [2 ]
Wu, Daishe [1 ]
Wang, Xiang [1 ]
Peng, Honggen [1 ]
机构
[1] Nanchang Univ, Coll Chem, Key Lab Poyang Lake Environm & Resource Utilizat, Minist Educ,Sch Resources Environm & Chem Engn, 999 Xuefu Rd, Nanchang 330031, Jiangxi, Peoples R China
[2] China Automot Technol & Res Ctr, Natl Engn Lab Mobile Source Emiss Control Technol, Tianjin 300300, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
Nitrogen oxide; Reduction of NOx; Hierarchical porous Cu-SSZ-13; Hydrothermal stability; SO2; resistance; NH3-SCR; NH3; SSZ-13; OXIDE; SCR; REACTIVITY; MECHANISM; OXIDATION; ZEOLITE; AMMONIA;
D O I
10.1016/j.jcat.2021.07.024
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nitrogen oxide (NOx), one of the main air pollutants exhausted from diesel vehicles, is harmful to the environment and human health and has been selectively catalytically reduced to N-2 by Cu-exchanged zeolites with chabazite structures (CHA, Cu-SSZ-13). Unfortunately, the conventional Cu-SSZ-13 catalyst still has disadvantages in real applications, such as diffusion limits and micropore blocking due to formation of ammonium sulfates, especially at low reaction temperatures. Here, a highly crystalline hierarchical porous Cu-SSZ-13 zeolite (termed Cu-SSZ-13-HP) with enriched mesopores was rationally designed and prepared via a dual-template method for the first time. The novel Cu-SSZ-13-HP catalyst displayed boosted low-temperature activity (temperature of 70% conversion below 150 degrees C) and broadened active temperature window (between 175 and 500 degrees C, NOx conversion above 90%) compared with conventional Cu-SSZ-13 with only micropores. Importantly, Cu-SSZ-13-HP also exhibited superior hydrothermal stability and enhanced sulfur dioxide (SO2) tolerance, even when exposed to 100 ppm of SO2 for 4 h. The in situ diffuse reflectance infrared Fourier transform spectroscopy revealed that the NH3 selective catalytic reduction reaction might conform to the Langmuir-Hinshelwood mechanism in which ammonia (NH3) and NOx were activated by the acid and redox sites, respectively. The Cu-SSZ-13-HP catalyst developed by the dual-template strategy might be a good candidate for low-temperature reduction of NOx exhaust from diesel vehicles. (C) 2021 Elsevier Inc. All rights reserved.
引用
收藏
页码:309 / 320
页数:12
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