Excellent selective catalytic reduction of NOx by NH3 over Cu/SAPO-34 with hierarchical pore structure

Li, Rui; Wang, Peiqiang; Ma, Shibo; Yuan, Fang; Li, Zhibin; Zhu, Yujun

doi:10.1016/j.cej.2019.122376

Cited by 57 publications

(32 citation statements)

References 72 publications

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“…Figure shows the XRD patterns of pure SAPO‐34 and 0.15Cu/SAPO‐34. Obviously, both SAPO‐34 and 0.15Cu/SAPO‐34 present the diffraction peaks at 2θ of about 9.5, 14.0, 16.1, 17.8, 20.7, 25.0 and 30.7 °, belonging to the CHA topological structure, which indicates that the introduction of Cu ions has no effect on the formation of CHA topological structure for 0.15Cu/SAPO‐34. However, the crystallinity of 0.15Cu/SAPO‐34 is observed an obvious decrease compared with the SAPO‐34.…”

Section: Resultsmentioning

confidence: 99%

“…[18a] The negative band at 1200 cm À 1 can be assigned to nitrite which is generated by NO + O 2 adsorbed on the surface of 0.15Cu/SAPO-34. [12] While the bands between 1500 and 1700 cm À 1 are quite complicated, most of the bands cannot stable existence on the catalyst surface. But the intensity of the band at 1624 cm À 1 increases with the extension of contact time with NO + O 2 , belonging to the adsorbed NO 2 species formed by the reaction NO and O 2 .…”

Section: Resultsmentioning

confidence: 99%

“…As displayed in Figure A, NO+O 2 adsorbed on the surface of 0.15Cu/SAPO‐34 can engender many kinds of nitrate species, such as monodentate nitrate, bridged nitrate, bidentate nitrate, etc . The negative band at 1200 cm −1 can be assigned to nitrite which is generated by NO+O 2 adsorbed on the surface of 0.15Cu/SAPO‐34 . While the bands between 1500 and 1700 cm −1 are quite complicated, most of the bands cannot stable existence on the catalyst surface.…”

Section: Resultsmentioning

confidence: 99%

“…In order to further increase mass transfer and shorten the reactant transport path, the hierarchical pore structure was introduced into the zeolite catalyst. [12] Liu et al prepared a kind of Cu/SAPO-34 with meso-microporous with Cu-TEPA and DIEPA as the co-OSDA by the one-pot route, the synthetized Cu/SAPO-34 showed an excellent NH 3 -SCR performance in the operating temperature window of 150-425°C, but the hydrothermal stability was not discussed. [13] In addition to Cu-TEPA, there are many copper complexes suitable for one-step method as the copper source, but some conditions need to be met, for example, the complex molecule is easily available, the size of the complex molecule cannot exceed the size of the CHA cage, [8] and need stably exist in the synthetic sol, etc.…”

Section: Introductionmentioning

confidence: 99%

“…In order to further increase mass transfer and shorten the reactant transport path, the hierarchical pore structure was introduced into the zeolite catalyst . Liu et al.…”

Section: Introductionmentioning

confidence: 99%

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One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

Wang

et al. 2020

ChemCatChem

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It is still a serious challenge to develop a simple synthesized method of SAPO-34 sieve modified by Cu with high NH 3-SCR performance. The Cu/SAPO-34 samples with hierarchical structure were synthesized for the first time using cupric citrate as copper source by one-pot hydrothermal method which showed excellent NH 3-SCR performance for NO removal. Among them, the 0.15Cu/SAPO-34 catalyst with a Cu/Al ratio of 0.15 exhibited the widest temperature operating window (160-500°C) and better hydrothermal stability. The physicochemical properties of 0.15Cu/SAPO-34 was measured to understand the impacts of the Cu species on the NH 3-SCR of NO activity by various characterization methods including XRD, NH 3-TPD, N 2 adsorption-desorption, XPS, EPR, UV-vis, NH 3-oxidation, NMR and in situ DRIFTS. The results reveal that the good activity is assigned to the isolated Cu species located at the site (I) in SAPO-34, and the coexistence of surface Cu 2 + and Cu + species with almost equal amounts. In addition, 0.15Cu/SAPO-34 also possesses suitable acidic sites which are conducive to catalytic activity. The results of in situ DRIFTS suggest that the NH 3-SCR reaction follows Eley-Rideal mechanism over 0.15Cu/SAPO-34.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

“…In order to further increase mass transfer and shorten the reactant transport path, the hierarchical pore structure was introduced into the zeolite catalyst . Liu et al.…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

Wang

et al. 2020

ChemCatChem

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Synthesis and Applications of SAPO‐34 Molecular Sieves

Cheng

et al. 2021

Chemistry A European J

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Silicoaluminophosphate zeolite (SAPO‐34) has been attracting increasing attention due to its excellent form selection and controllability in the chemical industry, as well as being one of the best industrial catalysts for methanol‐to‐olefin (MTO) reaction conversion. However, as a microporous molecular sieve, SAPO‐34 easily generates carbon deposition and rapidly becomes inactivated. Therefore, it is necessary to reduce the crystal size of the zeolite or to introduce secondary macropores into the zeolite crystal to form a hierarchical structure in order to improve the catalytic effect. In this review, the synthesis methods of conventional SAPO‐34 molecular sieves, hierarchical SAPO‐34 molecular sieves and nanosized SAPO‐34 molecular sieves are introduced, and the properties of the synthesized SAPO‐34 molecular sieves are described, including the phase, morphology, pore structure, acid source, and catalytic performance, in particular with respect to the synthesis of hierarchical SAPO‐34 molecular sieves. We hope that the review can provide guidance to the preparation of the SAPO‐34 catalysts, and stimulate the future development of high‐performance hierarchical SAPO‐34 catalysts to meet the growing demands of the material and chemical industries.

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One‐pot facile synthesis of Cu‐SAPO‐34 via addition of tetraethylenepentamine and its enhanced catalytic activity in selective catalytic reduction of NO_x with NH₃

Cao

Chen

Dong

et al. 2022

J of Chemical Tech & Biotech

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BACKGROUND A series of Cu‐SAPO‐34 samples were prepared with different copper sources and addition of tetraethylenepentamine (TEPA) by a one‐pot method, which were applied for selective catalytic reduction of NOx with ammonia (NH3‐SCR). RESULTS Various measurements were carried out to investigate the effect of TEPA addition and copper sources used on sample properties. The results indicated that Cu‐SAPO‐34 obtained with the addition of TEPA using copper citrate (Cu‐SAPO‐34‐TC) displayed over 90% NOx conversion at 150–500 °C and excellent H2O and SO2 resistance in NH3‐SCR. This is because the addition of TEPA can control the formation of isolated Cu2+ species located at the junction of D6R in CHA cage, Site (I), which is regarded as a more easily approachable site to adsorbates (NH3 and NO) than others, thus leading to the excellent NH3‐SCR performance. Further study demonstrated that the Cu‐SAPO‐34‐TC catalyst shows much wider temperature window and more hydrothermal stability due to a greater amount of surface isolated Cu2+, fewer Si islands and more Al(IV) species. CONCLUSIONS The excellent activity of the Cu‐SAPO‐34‐TC catalyst can be attributed to the addition of TEPA, which is beneficial for controlling the isolated Cu2+ at Site (I) as well as inhibiting the aggregation of CuO species. Various characterizations also confirm that more surface Cu2+ can be produced using copper citrate as copper source. © 2022 Society of Chemical Industry (SCI).

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Excellent selective catalytic reduction of NOx by NH3 over Cu/SAPO-34 with hierarchical pore structure

Cited by 57 publications

References 72 publications

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

Synthesis and Applications of SAPO‐34 Molecular Sieves

One‐pot facile synthesis of Cu‐SAPO‐34 via addition of tetraethylenepentamine and its enhanced catalytic activity in selective catalytic reduction of NO_x with NH₃

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Excellent selective catalytic reduction of NOx by NH3 over Cu/SAPO-34 with hierarchical pore structure

Cited by 57 publications

References 72 publications

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH3‐SCR of NO performance

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH3‐SCR of NO performance

Synthesis and Applications of SAPO‐34 Molecular Sieves

One‐pot facile synthesis of Cu‐SAPO‐34 via addition of tetraethylenepentamine and its enhanced catalytic activity in selective catalytic reduction of NOx with NH3

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One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

One‐pot synthesis of Cu/SAPO‐34 with hierarchical pore using cupric citrate as a copper source for excellent NH₃‐SCR of NO performance

One‐pot facile synthesis of Cu‐SAPO‐34 via addition of tetraethylenepentamine and its enhanced catalytic activity in selective catalytic reduction of NO_x with NH₃