scholarly journals Nanosized Cu-SSZ-13 and Its Application in NH3-SCR

Catalysts ◽  
2020 ◽  
Vol 10 (5) ◽  
pp. 506 ◽  
Author(s):  
Ana Palčić ◽  
Paolo Cleto Bruzzese ◽  
Kamila Pyra ◽  
Marko Bertmer ◽  
Kinga Góra-Marek ◽  
...  

Nanosized SSZ-13 was synthesized hydrothermally by applying N,N,N-trimethyl-1-adamantammonium hydroxide (TMAdaOH) as a structure-directing agent. In the next step, the quantity of TMAdaOH in the initial synthesis mixture of SSZ-13 was reduced by half. Furthermore, we varied the sodium hydroxide concentration. After ion-exchange with copper ions (Cu2+ and Cu+), the Cu-SSZ-13 catalysts were characterized to explore their framework composition (XRD, solid-state NMR, ICP-OES), texture (N2-sorption, SEM) and acid/redox properties (FT-IR, TPR-H2, DR UV-Vis, EPR). Finally, the materials were tested in the selective catalytic reduction of NOx with ammonia (NH3-SCR). The main difference between the Cu-SSZ-13 catalysts was the number of Cu2+ in the double six-membered ring (6MRs). Such copper species contribute to a high NH3-SCR activity. Nevertheless, all materials show comparable activity in NH3-SCR up to 350 °C. Above 350 °C, NO conversion decreased for Cu-SSZ-13(2–4) due to side reaction of NH3 oxidation.

Catalysts ◽  
2021 ◽  
Vol 11 (8) ◽  
pp. 979
Author(s):  
Zexiang Chen ◽  
Meiqing Shen ◽  
Chen Wang ◽  
Jianqiang Wang ◽  
Jun Wang ◽  
...  

To improve the alkali metal resistance of commercial catalyst Cu/SSZ-13 for ammonia selective catalytic reduction (NH3-SCR) reaction, a simple method to synthesize Cu/SSZ-13 with a core–shell like structure was developed. Compared with smaller-sized counterparts, Cu/SSZ-13 with a crystal size of 2.3 μm exhibited excellent resistance to Na poisoning. To reveal the influence of the crystal size on Cu/SSZ-13, physical structure characterization (XRD, BET, SEM, NMR) and chemical acidic distribution (H2-TPR, UV-Vis, Diethylamine-TPD, pyridine-DRIFTs, EDS) were investigated. It was found that the larger the crystal size of the molecular sieve, the more Cu is distributed in the crystal core, and the less likely it was to be replaced by Na to generate CuO. Therefore, a 2.3 μm sized Cu/SSZ-13 well-controlled the reactivity of the side reaction NH3 oxidation and the generation of N2O. The result was helpful to guide the extension of the service life of Cu/SSZ-13.


2019 ◽  
Vol 2019 ◽  
pp. 1-9 ◽  
Author(s):  
Zhuo Yao ◽  
Dianli Qu ◽  
Yuxiang Guo ◽  
Yujing Yang ◽  
Hong Huang

Novel catalysts with high activity for the selective catalytic reduction of NO with NH3 (NH3-SCR) at low temperatures are highly demanded. In this study, mixed-node metal-organic frameworks (MOFs), e.g. Mn@CuBTC with controlled Mn composition in Cu3(BTC)2, were fabricated using postsynthetic exchange method and their structural characteristics and catalytic performances for NH3-SCR reaction were assessed. A series of analyses in terms of structure, surface morphology, texture, and chemical state determined that Mn ions were successfully incorporated into the Cu3(BTC)2 crystal lattice as well as adsorbed on the walls of nanopores in the framework. The pore sizes can be finely tuned in the presence of Mn ions in the cages, which significantly suppressed water adsorption. The NH3-SCR activity of Mn@CuBTC exhibited nearly 100% NOx conversion rate in the temperature range (230–260°C). The superior NH3-SCR performance is attributed to the proper pore sizes, reduced water content, and the synergistic effect between manganese and copper ions in the MOF structure, which enhanced NH3 bound to the active Lewis sites.


2018 ◽  
Vol 148 (4) ◽  
pp. 1228-1235 ◽  
Author(s):  
Rui Wu ◽  
Ningqiang Zhang ◽  
Xiaojun Liu ◽  
Lingcong Li ◽  
Liyun Song ◽  
...  

Abstract Heteropolyacids and their salts have been effectively used in selective catalytic reduction because of the Keggin structure and extraordinarily strong acidity. Catalysts with and without the Keggin structure were synthesized to further investigate the effects of heteropolyoxometallate on low temperature NH3–SCR. XRD, BET, Raman, H2–TPR, NH3–TPD, FT-IR, and SO2–TPD techniques were used to characterize the physicochemical characteristics of the catalysts. Results indicate that catalysts with the Keggin structure had more surface Brönsted and Lewis acid sites, and these catalysts had significantly improved performances in the SCR reaction and in SO2 poisoning resistance. Graphical Abstract


Materials ◽  
2018 ◽  
Vol 11 (8) ◽  
pp. 1307 ◽  
Author(s):  
Yaping Zhang ◽  
Xiupeng Yue ◽  
Tianjiao Huang ◽  
Kai Shen ◽  
Bin Lu

TiO2-ZrO2 (Ti-Zr) carrier was prepared by a co-precipitation method and 1 wt. % V2O5 and 0.2 CeO2 (the Mole ratio of Ce to Ti-Zr) was impregnated to obtain the V2O5-CeO2/TiO2-ZrO2 catalyst for the selective catalytic reduction of NOx by NH3. The transient activity tests and the in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) analyses were employed to explore the NH3-SCR (selective catalytic reduction) mechanism systematically, and by designing various conditions of single or mixing feeding gas and pre-treatment ways, a possible pathway of NOx reduction was proposed. It was found that NH3 exhibited a competitive advantage over NO in its adsorption on the catalyst surface, and could form an active intermediate substance of -NH2. More acid sites and intermediate reaction species (-NH2), at lower temperatures, significantly promoted the SCR activity of the V2O5-0.2CeO2/TiO2-ZrO2 catalyst. The presence of O2 could promote the conversion of NO to NO2, while NO2 was easier to reduce. The co-existence of NH3 and O2 resulted in the NH3 adsorption strength being lower, as compared to tests without O2, since O2 could occupy a part of the active site. Due to CeO2’s excellent oxygen storage-release capacity, NH3 adsorption was weakened, in comparison to the 1 wt. % V2O5-0.2CeO2/TiO2-ZrO2 catalyst. If NOx were to be pre-adsorbed in the catalyst, the formation of nitrate and nitro species would be difficult to desorb, which would greatly hinder the SCR reaction. All the findings concluded that NH3-SCR worked mainly through the Eley-Rideal (E-R) mechanism.


2006 ◽  
Vol 113 (1-2) ◽  
pp. 87-93 ◽  
Author(s):  
F. Romero Sarria ◽  
O. Marie ◽  
P. Bazin ◽  
J. Saussey ◽  
J. Lesage ◽  
...  

2018 ◽  
Vol 8 (4) ◽  
pp. 1028-1038 ◽  
Author(s):  
Ramon Oord ◽  
Joel E. Schmidt ◽  
Bert M. Weckhuysen

Using in situ FT-IR and operando UV-vis-NIR DRS, performed on a series of different Cu–ion-exchanged SSZ-13 zeolites, both a mono-nuclear site or a dimeric copper active site are consistent for methane-to-methanol activation.


Catalysts ◽  
2021 ◽  
Vol 11 (7) ◽  
pp. 796
Author(s):  
Huawang Zhao ◽  
Lei Han ◽  
Yujie Wang ◽  
Jiandong Zheng

Platinum’s (Pt) poisoning effect on Cu-SSZ-13 and its regeneration were investigated. The Pt enhanced the parallel reactions, such as NH3 oxidation and NO oxidation reactions, which decreased the deNOx activities. In the temperature range below 330 °C, the deactivation of Cu-SSZ-13 by Pt poisoning was primarily caused by the overconsumption of NH3, due to the enhanced NH3-selective oxidation reaction, while the formation of NOx in NH3 oxidation and NO oxidation into NO2 further aggravated the degradation when the temperature was above 460 °C. The non-selective NH3 oxidation and non-selective NOx catalytic reduction reactions resulted in increased N2O formation over Pt-doped samples. The transformation of Pt0 into PtOx after hydrothermal aging recovered the deNOx activities of the Pt-poisoned samples.


Catalysts ◽  
2019 ◽  
Vol 9 (11) ◽  
pp. 929 ◽  
Author(s):  
Auvray ◽  
Mihai ◽  
Lundberg ◽  
Olsson

Lean nitric oxide (NOx)-trap (LNT) and selective catalytic reduction (SCR) are efficient systems for the abatement of NOx. The combination of LNT and SCR catalysts improves overall NOx removal, but there is a risk that the SCR catalyst will be exposed to high temperatures and rich exhaust during the LNTs sulfur regeneration. Therefore, the effect of exposure to various rich conditions and temperatures on the subsequent SCR activity of a Cu-exchanged chabazite catalyst was studied. CO, H2, C3H6, and the combination of CO + H2 were used to simulate rich conditions. Aging was performed at 800 °C, 700 °C, and, in the case of CO, 600 °C, in a plug-flow reactor. Investigation of the nature of Cu sites was performed with NH3-temperature-programed desorption (TPD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) of probe molecules (NH3 and NO). The combination of CO and H2 was especially detrimental to SCR activity and to NH3 oxidation. Rich aging with low reductant concentrations resulted in a significantly larger deactivation compared to lean conditions. Aging in CO at 800 °C caused SCR deactivation but promoted high-temperature NH3 oxidation. Rich conditions greatly enhanced the loss of Brønsted and Lewis acid sites at 800 °C, indicating dealumination and Cu migration. However, at 700 °C, mainly Brønsted sites disappeared during aging. DRIFT spectroscopy analysis revealed that CO aging modified the Cu2+/CuOH+ ratio in favor of the monovalent CuOH+ species, as opposed to lean aging. To summarize, we propose that the reason for the increased deactivation observed for mild rich conditions is the transformation of the Cu species from Z2Cu to ZCuOH, possibly in combination with the formation of Cu clusters.


Author(s):  
Dang Van Long ◽  
Le Thanh Son ◽  
Pham Dinh Trong

Abstract: Since NOx emission requirements from stationary and mobile sources are more strictly regulated in the United States, Europe, and other countries; researchers have conducted many studies to improve the performance of selective catalytic reduction (SCR) catalysts to meet more and more stringent emission standards. Herein, we reported the synthesis of small pore zeolite (Cu)-SSZ-13 using N,N,N-dimethylethylcyclohexylammonium as the structure directing agent. The catalytic activity of the fresh and hydrothermal aged copper exchanged supported on SSZ-13 catalyst was investigated in the SCR of NOx using NH3 as a reductant. Cu-SSZ-13 possessing a high SCR performance (NOx conversion reached approximately 100% at 250oC), and high hydrothermal stability in combination with an easy synthesis route is considered to be a potential catalyst for SCR application. Keywords: Zeolite, SSZ-13, synthesis, SCR, NOx.


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