scholarly journals Influence of Impurity Dissolution on Surface Properties and NH3-SCR Catalytic Activity of Rare Earth Concentrate

Minerals ◽  
2019 ◽  
Vol 9 (4) ◽  
pp. 246
Author(s):  
Zhang ◽  
Zhu ◽  
Zhang ◽  
Li ◽  
Luo ◽  
...  
Keyword(s):  
Rare Earth ◽  
Active Sites ◽  
Catalytic Effect ◽  
Catalytic Reduction ◽  
Weak Acid ◽  
Active Components ◽  
Catalyst Sample ◽  
Nh3 Scr ◽  
O2 Concentration ◽  
Alkali Leaching

Impurity removal and modification of rare earth concentrate powder were conducted by roasting weak acid-weak alkali leaching to obtain the active components of denitrification catalysts. NH3 selective catalytic reduction catalyst samples were prepared by mixing and kneading with pseudo-γ-Al2O3 boehmite as carrier. The results showed that the Ce7O12 content in the active component samples increased and dispersed more evenly. The grain size of the samples was refined, the specific surface area increased, and the active sites exposed more. Ce coexists in the form of Ce3+ and Ce4+. Fe coexists in the form of Fe3+ and Fe2+, but Fe3+ is abundant. Some Ce, La, Nd, Pr, Fe, Mn, and other components formed solid melts during preparation, which increased the synergistic catalytic effect. The denitrification efficiency of the catalyst sample was 92.8% under the conditions of reaction temperature 400 °C, NO content was 600 ppm, NH3/NO ratio was 1.5, and O2 concentration was 4%.

scholarly journals Prepare a catalyst consist of rare earth minerals to denitrate via NH3-SCR

2020 ◽  
Vol 9 (1) ◽  
pp. 191-202
Author(s):  
Jian Wang ◽  
Chao Zhu ◽  
Baowei Li ◽  
Zhijun Gong ◽  
Zhaolei Meng ◽  
...  
Keyword(s):  
Rare Earth ◽  
Active Sites ◽  
Nh3 Scr ◽  
Composite Oxides ◽  
Rare Earth Minerals ◽  
Denitrification Activity ◽  
Denitrification Reactor ◽  
Surface Active ◽  
Rare Earth Tailings ◽  
Treatment Step

AbstractTo research the roles of rare earth minerals in denitrification via the NH3-SCR, a mixture was made by certain ratio of rare earth concentrates and rare earth tailings, then treated by microwave roasting, and acids and bases to form a denitrification catalyst. The mineral phase structure and surface morphology of the catalyst were characterized by XRD, BET, SEM and EDS. The surface properties of the catalyst were tested by TPD and XPS methods, and the denitrification activity of the catalyst was evaluated in a denitrification reactor. The results showed that the denitrification efficiency increased up to 82% with complete processing. XRD, BET, SEM, and EDS spectrum analysis stated that the treated minerals contained cerium oxides and Fe−Ce composite oxides. The surface of the modified minerals became rough and porous, the surface area increased, and the surface-active sites were exposed. The results of NH3-TPD and NO-TPD showed that the catalyst surface could gradually adsorb more NH3 and NO after each step. XPS analysis indicated that there were more Ce3+, Fe2+, and lattice oxygen in rare earth minerals catalyst after each treatment step.

scholarly journals The Role of SO3 Poisoning in CU/SSZ-13 NH3-SCR Catalysts

Catalysts ◽  
2019 ◽  
Vol 9 (9) ◽  
pp. 741 ◽  
Author(s):  
Wang ◽  
Hou ◽  
Yan ◽  
Zhang ◽  
Wang ◽  
...  
Keyword(s):  
Copper Sulfate ◽  
Active Sites ◽  
Catalytic Reduction ◽  
Copper Ions ◽  
Acid Resistance ◽  
Temperature Program Reduction ◽  
Copper Species ◽  
Nh3 Scr ◽  
Scr Catalysts

To reveal the role of SO3 poisoning in Cu/SSZ-13 NH3-SCR catalysts, fresh and sulfated Cu/SSZ-13 catalysts were prepared in the presence or absence of SO3 flux. The deactivation mechanism is probed by the changes of structural, copper species, and selective catalytic reduction (SCR) activity. The variations concentrate on the changes of copper species as the Chabazite (CHA) framework of Cu/SSZ-13 catalysts could keep intact at high ratios of SO3/SOx. The thermal gravimetric analyzer (TGA) results reveal that the copper sulfate formed during sulfation and the amounts of sulfate species increased with an increase in the SO3/SOx ratio. In contrast to the changing trend of copper sulfate, temperature program reduction (H2-TPR), and electron paramagnetic resonance (EPR) results manifest that, since the number of active copper ions declines with an increase of the SO3/SOx ratio, the active sites transform to these inactive species during sulfation. Due to the combination of NH3-SCR activity and the kinetic tests, it is shown that the decreased number of active sites is responsible for the declined SCR activity at low temperature. As Cu/SSZ-13 catalysts show excellent acid-resistance ability, our study reveals that the Cu/SSZ-13 catalyst is a good candidate for NOx elimination, especially when SO3 exists.

scholarly journals Copper-Iron Bimetal Ion-Exchanged SAPO-34 for NH3-SCR of NOx

Catalysts ◽  
2020 ◽  
Vol 10 (3) ◽  
pp. 321 ◽  
Author(s):  
Tuan Doan ◽  
Phong Dam ◽  
Khang Nguyen ◽  
Thanh Huyen Vuong ◽  
Minh Thang Le ◽  
...  
Keyword(s):  
Active Sites ◽  
Catalytic Reduction ◽  
Catalytic Performance ◽  
Physical Structure ◽  
Acid Sites ◽  
Tetraethylammonium Hydroxide ◽  
Nh3 Scr ◽  
Nox Conversion ◽  
Temperature Window ◽  
Scr Of Nox

SAPO-34 was prepared with a mixture of three templates containing triethylamine, tetraethylammonium hydroxide, and morpholine, which leads to unique properties for support and production cost reduction. Meanwhile, Cu/SAPO-34, Fe/SAPO-34, and Cu-Fe/SAPO-34 were prepared through the ion-exchanged method in aqueous solution and used for selective catalytic reduction (SCR) of NOx with NH3. The physical structure and original crystal of SAPO-34 are maintained in the catalysts. Cu-Fe/SAPO-34 catalysts exhibit high NOx conversion in a broad temperature window, even in the presence of H2O. The physicochemical properties of synthesized samples were further characterized by various methods, including XRD, FE-SEM, EDS, N2 adsorption-desorption isotherms, UV-Vis-DRS spectroscopy, NH3-TPD, H2-TPR, and EPR. The best catalyst, 3Cu-1Fe/SAPO-34 exhibited high NOx conversion (> 90%) in a wide temperature window of 250–600 °C, even in the presence of H2O. In comparison with mono-metallic samples, the 3Cu-1Fe/SAPO-34 catalyst had more isolated Cu2+ ions and additional oligomeric Fe3+ active sites, which mainly contributed to the higher capacity of NH3 and NOx adsorption by the enhancement of the number of acid sites as well as its greater reducibility. Therefore, this synergistic effect between iron and copper in the 3Cu-1Fe/SAPO-34 catalyst prompted higher catalytic performance in more extensive temperature as well as hydrothermal stability after iron incorporation.

scholarly journals Strikingly Distinctive NH3-SCR Behavior over Cu-SSZ-13 in the Presence of NO2

2021 ◽  
Author(s):  
Yulong Shan ◽  
Guangzhi He ◽  
Jinpeng Du ◽  
Yu Sun ◽  
Zhongqi Liu ◽  
...  
Keyword(s):  
Active Sites ◽  
Density Functional ◽  
Catalytic Reduction ◽  
Acid Sites ◽  
Zeolite Catalysts ◽  
Nh3 Scr ◽  
Highly Active ◽  
Small Pore ◽  
Standard Scr ◽  
Catalyst Systems

Abstract Commercial Cu-exchanged small-pore SSZ-13 (Cu-SSZ-13) zeolite catalysts are highly active for the selective catalytic reduction (SCR) of NOx with NH3, but distinct from other catalyst systems, their activity is unexpectedly inhibited in the presence of NO2. Here, we combined kinetic experiments, in-situ/operando X-ray absorption spectroscopy, and density functional theory (DFT) calculations to obtain direct evidence that under reaction conditions, strong oxidation by NO2 forces Cu ions to exist mainly as fixed framework Cu2+ species (fw-Cu2+), which impede the formation of dynamic binuclear Cu+ species that serve as the main active sites for the standard SCR (SSCR) reaction. As a result, the SSCR reaction is significantly inhibited by NO2 in the zeolite system, and the NO2-involved SCR reaction occurs with an energy barrier higher than that of the SSCR reaction on dynamic binuclear sites. Moreover, the NO2-involved SCR reaction tends to occur at the Brønsted acid sites (BAS) rather than the fw-Cu2+ sites. This work clearly explains the strikingly distinctive selective catalytic behavior in the zeolite system.

scholarly journals Theoretical and Spectroscopic Evidence of the Dynamic Nature of Copper Active Sites in Cu-CHA Catalysts under Selective Catalytic Reduction (NH3–SCR–NOx) Conditions

2020 ◽  
Vol 11 (23) ◽  
pp. 10060-10066
Author(s):  
Reisel Millan ◽  
Pieter Cnudde ◽  
Alexander E. J. Hoffman ◽  
Christian W. Lopes ◽  
Patricia Concepción ◽  
...  
Keyword(s):  
Selective Catalytic Reduction ◽  
Active Sites ◽  
Catalytic Reduction ◽  
Dynamic Nature ◽  
Spectroscopic Evidence ◽  
Nh3 Scr

scholarly journals A Review of Low Temperature NH3-SCR for Removal of NOx

Catalysts ◽  
2019 ◽  
Vol 9 (4) ◽  
pp. 349 ◽  
Author(s):  
Devaiah Damma ◽  
Padmanabha Ettireddy ◽  
Benjaram Reddy ◽  
Panagiotis Smirniotis
Keyword(s):  
Low Temperature ◽  
Transition Metal ◽  
Transition Metal Oxides ◽  
Active Sites ◽  
Catalytic Reduction ◽  
Operating Conditions ◽  
Advanced Materials ◽  
Research Progress ◽  
Nh3 Scr ◽  
Mixed Transition

The importance of the low-temperature selective catalytic reduction (LT-SCR) of NOx by NH3 is increasing due to the recent severe pollution regulations being imposed around the world. Supported and mixed transition metal oxides have been widely investigated for LT-SCR technology. However, these catalytic materials have some drawbacks, especially in terms of catalyst poisoning by H2O or/and SO2. Hence, the development of catalysts for the LT-SCR process is still under active investigation throughout seeking better performance. Extensive research efforts have been made to develop new advanced materials for this technology. This article critically reviews the recent research progress on supported transition and mixed transition metal oxide catalysts for the LT-SCR reaction. The review covered the description of the influence of operating conditions and promoters on the LT-SCR performance. The reaction mechanism, reaction intermediates, and active sites are also discussed in detail using isotopic labelling and in situ FT-IR studies.

scholarly journals Promoting Effect of Mn on In Situ Synthesized Cu-SSZ-13 for NH3-SCR

Catalysts ◽  
2020 ◽  
Vol 10 (12) ◽  
pp. 1375
Author(s):  
Jinpeng Du ◽  
Jingyi Wang ◽  
Xiaoyan Shi ◽  
Yulong Shan ◽  
Yan Zhang ◽  
...  
Keyword(s):  
Low Temperature ◽  
Active Sites ◽  
Catalytic Reduction ◽  
Acid Sites ◽  
Promoting Effect ◽  
Nh3 Scr ◽  
Temperature Programmed ◽  
Diffuse Reflectance Infrared ◽  
Redox Ability

The effect of Mn impregnation on the NH3-SCR (selective catalytic reduction of NOx by NH3) activity of in situ synthesized Cu-SSZ-13 was investigated in this work. It was found that Mn addition could efficiently improve the low-temperature activity of Cu-SSZ-13. The optimal amount of Mn was 5 wt.%, and NOx conversion was improved by more than 20% over a temperature range of 120 °C to 150 °C. SEM (scanning electron microscopy), XRD (X-ray diffraction), N2 adsorption-desorption, H2-TPR (temperature programmed reduction of H2), NH3-TPD (temperature programmed desorption of NH3) and in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) experiments were conducted to investigate the changes in the zeolite structure, active sites, acid sites and reaction mechanism. The impregnated MnOx species caused a decline in the crystallinity of Cu-SSZ-13 but markedly improved the redox ability. Nitrate and nitrite species were observed in the Mn-modified Cu-SSZ-13, and the formation of these species was thought to cause the observed increase in low-temperature NH3-SCR activity. The results show that the addition of Mn is a promising method for promoting the low-temperature catalytic activity of Cu-SSZ-13.

scholarly journals Hybrid Cu-Fe/ZSM-5 Catalyst Prepared by Liquid Ion-Exchange for NOx Removal by NH3-SCR Process

2021 ◽  
Vol 2021 ◽  
pp. 1-15
Author(s):  
Tuan Doan ◽  
Anh Dang ◽  
Dat Nguyen ◽  
Thanh Huyen Vuong ◽  
Minh Thang Le ◽  
...  
Keyword(s):  
Ion Exchange ◽  
Active Sites ◽  
Flow Reactor ◽  
Catalytic Reduction ◽  
Fixed Bed ◽  
Chemical Properties ◽  
Resonance Method ◽  
Exchange Method ◽  
Characterization Methods ◽  
Nh3 Scr

A series of Cu/ZSM-5, Fe/ZSM-5, and Cu-Fe/ZSM-5 catalysts (Si/Al in ZSM-5 = 25) were prepared by different metal loadings using the liquid ion-exchange method. Several characterization methods were conducted to explore the effects of metals on the physical and chemical properties of catalysts. Meanwhile, the electron paramagnetic resonance method is also used to assess the copper and/or iron elements’ coordination and valence state at intersections or in channels of ZSM-5. The metal-loading effects of all catalysts on the catalytic activities were studied for the removal of NOx in a fixed-bed flow reactor using selective catalytic reduction with ammonia (NH3-SCR). The results showed that the iron’s addition could markedly broaden the operation temperature range of the Cu/ZSM-5 catalyst for NH3-SCR between 200 and 550°C due to the presence of more isolated Cu2+ ions as well as additional oligomeric Fe3+ active sites and FexOy oligomeric species. This paper gives a facile and straightforward way to synthesize the practical-promising catalyst applied in NH3-SCR technology to control NOx emissions.

The synergistic effects between Ce and Cu in CuyCe1−yW5Ox catalysts for enhanced NH3-SCR of NOx and SO2 tolerance

2019 ◽  
Vol 9 (3) ◽  
pp. 718-730 ◽  
Author(s):  
Jian-Wen Shi ◽  
Yao Wang ◽  
Ruibin Duan ◽  
Chen Gao ◽  
Baorui Wang ◽  
...  
Keyword(s):  
Metal Oxides ◽  
Selective Catalytic Reduction ◽  
Low Temperatures ◽  
Catalytic Reduction ◽  
Synergistic Effects ◽  
Reduction Of No ◽  
Nh3 Scr ◽  
So2 Tolerance ◽  
Scr Of Nox

Non-manganese-based metal oxides are promising catalysts for the NH3-SCR (selective catalytic reduction) of NOx at low temperatures.

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