scholarly journals Effect of Stannic Species Modification on the Acidity of Silicalite-1 and Its Enhancement in Transforming Ethylenediamine to Heterocyclic Amines

Catalysts ◽  
2020 ◽  
Vol 10 (2) ◽  
pp. 211
Author(s):  
Yongxin Zhang ◽  
Long Lin ◽  
Xiaoming Zheng ◽  
Chunyan Liu ◽  
Quanren Zhu ◽  
...  

In this study, a series of SnO2 modified zeolite catalysts (Snx-S-1; x is the weight percentage of Sn) were prepared with SnCl2 and a defective Silicalite-1 (S-1) zeolite via facile deposition–precipitation method. It was found that the stannic species modified all-silica zeolite catalysts were active for the intermolecular condensation of ethylenediamine (EDA) to 1, 2-Diazabicyclo [2, 2, 2] octane (TEDA) and piperazine (PIP). The best catalyst Sn6-S-1 (6 wt.% Sn loading) showed 86% EDA conversion and 93% total selectivity to TEDA and PIP. By contrast, the defective S-1 zeolite parent showed only approximately 9% EDA conversion under the same conditions. With the help of catalyst characterization techniques including hydroxyl vibration and pyridine adsorption FT-IR spectroscopy (transmission mode), the enhancement of the catalytic activity of the SnO2 modified zeolite catalysts (Snx-S-1) was mainly attributed to the formation of mild Lewis acid sites in the siliceous zeolite. Both the hydroxyl nests of the defective S-1 zeolite and the dispersed SnO2 clusters should be the important factors for the formation of mild Lewis acid sites on the modified zeolite. Based on the catalytic performance of the modified zeolite in the conversion of EDA to PIP and TEDA, it is inferred that the mildly acidified defective S-1 zeolite by the SnO2 deposition modification might become a very active and durable catalyst for reactions involving strongly alkaline reactants and products.

RSC Advances ◽  
2017 ◽  
Vol 7 (39) ◽  
pp. 24177-24187 ◽  
Author(s):  
Haidi Xu ◽  
Mengmeng Sun ◽  
Shuang Liu ◽  
Yuanshan Li ◽  
Jianli Wang ◽  
...  

The calcined temperature of the carrier obviously affected SCR activity of catalysts, WO3/Ce0.68Zr0.32O2-500 showed the best low-temperature NH3-SCR activity due to its more Lewis acid sites and stronger redox property.


2017 ◽  
Vol 7 (23) ◽  
pp. 5482-5494 ◽  
Author(s):  
Francisco G. Cirujano

Comparative review of the catalytic performance of isolated tetravalent metals as Lewis acid sites in zeolite and MOF materials.


2000 ◽  
Vol 104 (17) ◽  
pp. 4122-4129 ◽  
Author(s):  
Wenmin Zhang ◽  
Panagiotis G. Smirniotis ◽  
M. Gangoda ◽  
Rathindra N. Bose

2018 ◽  
Vol 43 (1) ◽  
pp. 21-29 ◽  
Author(s):  
Yali Du ◽  
Yalin Feng ◽  
Chunlei Zou ◽  
Xu Wu ◽  
Wei Huang

The nitrate form of Ni–Al layered double hydroxide (denoted as Ni–Al–NO3-LDH) and the corresponding carbonate form (denoted as Ni–Al–CO3-LDH) were tunably fabricated by the hexamethylenetetramine hydrolysis method. A catalytic behaviour investigation proved Ni–Al–CO3-LDH to be an ineffective catalyst, while for Ni–Al–NO3-LDH excellent catalytic activity and reusability were obtained, in the acetalisation of furfural to furfural diethyl acetal. Characterisation and analysis revealed that the appearance of Lewis acid sites in Ni–Al–NO3-LDH was responsible for its excellent catalytic performance. The acquired kinetic parameters confirmed that this reaction was a first-order process and the apparent activation energy was 36.28 kJ mol−1, which is in reasonable agreement with the theoretical result of 38.57 kJ mol−1. Additionally, apart from the typical Brønsted acid catalytic mechanism, a possible Lewis acid catalytic mechanism was probed theoretically.


ChemCatChem ◽  
2014 ◽  
Vol 6 (10) ◽  
pp. 2970-2975 ◽  
Author(s):  
Zichun Wang ◽  
Yijiao Jiang ◽  
Michael Hunger ◽  
Alfons Baiker ◽  
Jun Huang

1996 ◽  
Vol 50 (10) ◽  
pp. 1319-1324 ◽  
Author(s):  
Stephen A. Bagshaw ◽  
Ralph P. Cooney

Adsorption interactions of the bidentate molecules 2,2'-bipyridine and 4,4'-bipyridine with the surfaces of different alumina-pillar interlayered clays have been investigated by FT-IR spectroscopy. These interactions were examined in an attempt to establish a spectroscopic method for the determination of interpillar distances in the galleries of pillared clays. 2,2'-Bipyridine adsorbs in a bidentate C2 v, interaction to single Lewis acid sites on the surfaces of individual pillars and not to adjacent pillars, indicating that the distances between binding sites on adjacent pillars are too great to be successfully probed by this molecule. 4,4'-Bipyridine maintains the D2 h symmetry of the free molecule through interaction with Lewis acid sites on two adjacent pillars simultaneously via both ends of the molecule, thereby exhibiting possible utility as a probe of the interpillar distance. Surface-adsorbed monoprotonated 2,2'-bipyridinium cations are formed through interaction with Brönsted acid sites on the pillared clay surfaces. The IR spectrum of the surface-adsorbed protonated species suggests C2/i transoid symmetry and is presented for the first time.


Catalysts ◽  
2021 ◽  
Vol 11 (8) ◽  
pp. 962
Author(s):  
Xun Wang ◽  
Yongkang Lv ◽  
Shanhui Zhu ◽  
Xuefeng Wang ◽  
Cunbao Deng

Regulating the acid property of zeolite is an effective strategy to improve dehydration of intermediate alcohol, which is the rate-determining step in hydrodeoxygenation of lignin-based phenolic compounds. Herein, a commercial Hβ (SiO2/Al2O3 = 25) was modified by phosphoric acid, and evaluated in the catalytic performance of guaiacol to cyclohexane, combined with Ni/SiO2 prepared by the ammonia evaporation hydrothermal (AEH) method. Incorporating a small amount of phosphorus had little impact on the morphology, texture properties of Hβ, but led to dramatic variations in acid property, including the amount of acid sites and the ratio of Brønsted acid sites to Lewis acid sites, as confirmed by NH3-TPD, Py-IR, FT-IR and 27Al MAS NMR. Phosphorus modification on Hβ could effectively balance competitive adsorption of guaiacol on Lewis acid sites and intermediate alcohol dehydration on Brønsted acid sites, and then enhanced the catalytic performance of guaiacol hydrodeoxygenation to cyclohexane. By comparison, Hβ containing 2 wt.% phosphorus reached the highest activity and cyclohexane selectivity.


2018 ◽  
Vol 9 (31) ◽  
pp. 6470-6479 ◽  
Author(s):  
Yueying Chu ◽  
Xianfeng Yi ◽  
Chengbin Li ◽  
Xianyong Sun ◽  
Anmin Zheng

The Lewis acid site combined with a Brønsted acid site in zeolite catalysts facilitates first C–C bond formation in the initiation step of the MTO reaction.


2020 ◽  
Vol 44 (42) ◽  
pp. 18319-18325
Author(s):  
Zheng Wang ◽  
Qianjie Xie ◽  
Yajun Wang ◽  
Yu Shu ◽  
Cong Li ◽  
...  

Ni-based MOFs with Lewis acid sites was developed for CO2 fixation with epoxides into cyclic carbonates, and a comparative study shows that the density and accessibility of the Lewis acid sites in the MOFs greatly influence the catalytic performance.


Sign in / Sign up

Export Citation Format

Share Document