scholarly journals A Facile Strategy to Prepare Shaped ZSM-5 Catalysts with Enhanced Para-Xylene Selectivity and Stability for Toluene Methylation: The Effect of In Situ Modification by Attapulgite

Molecules ◽  
2019 ◽  
Vol 24 (19) ◽  
pp. 3462 ◽  
Author(s):  
Yiren Wang ◽  
Yang Chang ◽  
Min Liu ◽  
Anfeng Zhang ◽  
Xinwen Guo
Keyword(s):  
Physical Adsorption ◽  
Catalytic Performance ◽  
Acid Sites ◽  
General Strategy ◽  
X Ray Diffraction ◽  
In Situ Modification ◽  
Para Xylene ◽  
Toluene Methylation ◽  
Temperature Programmed

A general strategy for preparing shaped toluene methylation catalysts with enhanced para-selectivity and stability is developed by extruding ZSM-5 zeolite with attapulgite as a binder. The novel attapulgite/ZSM-5 extrudate exhibited significantly higher para-selectivity and stability in comparison to the conventional alumina-bound ZSM-5 extrudate. The catalyst samples have been characterized by in situ X-ray diffraction, scanning electron microscope (SEM), NH3 temperature programmed desorption (TPD), thermogravimetric analysis (TGA) as well as n-hexane/cyclohexane physical adsorption. The enhanced catalytic performance of attapulgite/ZSM-5 extrudate is correlated with the in-situ modification of acid sites in the catalyst by mobile alkaline species, which is introduced via extrusion with attapulgite. Moreover, a higher para-selectivity was obtained over attapulgite-bound modified ZSM-5 extrudate. Such facile and universal strategy of extruding ZSM-5 catalysts with attapulgite as binder could pave a way for preparation of shaped zeolite-base catalyst with enhanced catalytic performance.

scholarly journals A Facile Strategy to Prepare Shaped ZSM-5 Catalyst with Enhanced para-Xylene Selectivity and Stability for Toluene Methylation

2017 ◽  
Author(s):  
Yiren Wang ◽  
Yang Chang ◽  
Min Liu ◽  
Anfeng Zhang ◽  
Chunshan Song ◽  
...  
Keyword(s):  
Physical Adsorption ◽  
Catalytic Performance ◽  
Acid Sites ◽  
The Novel ◽  
In Situ Xrd ◽  
Para Xylene ◽  
Toluene Methylation ◽  
Temperature Programmed ◽  
Catalytic Performances

This work describes the catalytic performances of attapulgite/ZSM-5 extrudate in comparison to conventional alumina-bound ZSM-5 extrudate in toluene methylation. The novel attapulgite/ZSM-5 extrudate is prepared by using natural clay attapulgite as binder which introduces mobile alkaline species and macropores to the extrudate. In contrast to alumina-bound extrudate, this novel extrudate shows significantly higher para-selectivity and stability. By using characterization techniques, including in-situ XRD, SEM, NH3 temperature programmed desorption (TPD), thermogravimetric analysis and n-hexane/cyclohexane physical adsorption, the catalytic performance improvement of attapulgite/ZSM-5 extrudate is correlated with the neutralization of Brønsted acid sites by mobile alkaline species during calcination and reaction process. Moreover, a higher para-selectivity was obtained over attapulgite-bound modified ZSM-5 extrudate. The strategy of extruding ZSM-5 catalysts with attapulgite as binder is facile and universal. Such method paves a new way for preparation of shaped toluene methylation catalyst with enhanced para-selectivity and stability.

scholarly journals Fabrication of the Hierarchical HZSM-5 Membrane with Tunable Mesoporosity for Catalytic Cracking of n-Dodecane

Catalysts ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 155 ◽  
Author(s):  
Zhenheng Diao ◽  
Lushi Cheng ◽  
Xu Hou ◽  
Di Rong ◽  
Yanli Lu ◽  
...  
Keyword(s):  
Catalytic Cracking ◽  
Inductively Coupled Plasma ◽  
Catalytic Performance ◽  
X Ray Diffraction ◽  
Inductively Coupled ◽  
Swelling Agent ◽  
Ft Ir ◽  
Temperature Programmed ◽  
Adsorption Desorption

Hierarchical HZSM-5 membranes were prepared on the inner wall of stainless steel tubes, using amphiphilic organosilane (TPOAC) and mesitylene (TMB) as a meso-porogen and a swelling agent, respectively. The mesoporosity of the HZSM-5 membranes were tailored via formulating the TPOAC/Tetraethylorthosilicate (TPOAC/TEOS) ratio and TMB/TPOAC ratio, in synthesis gel, and the prepared membranes were systematically characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), N2 adsorption–desorption, N2 permeation, inductively coupled plasma (ICP), in situ fourier transform infrared (FT-IR), ammonia temperature-programmed desorption (NH3-TPD), etc. It was found that the increase of the TPOAC/TEOS ratio promoted a specific surface area and diffusivity of the HZSM-5 membranes, as well as decreased acidity; the increase of the TMB/TPOAC ratios led to an enlargement of the mesopore size and diffusivity of the membranes, but with constant acid properties. The catalytic performance of the prepared HZSM-5 membranes was tested using the catalytic cracking of supercritical n-dodecane (500 °C, 4 MPa) as a model reaction. The hierarchical membrane with the TPOAC/TEOS ratio of 0.1 and TMB/TPOAC ratio of 2, exhibited superior catalytic performances with the highest activity of up to 13% improvement and the lowest deactivation rate (nearly a half), compared with the microporous HZSM-5 membrane, due to the benefits of suitable acidity, together with enhanced diffusivity of n-dodecane and cracking products.

Influence of Final Nitriding Temperature on the Preparation and the Catalytic Performance of CoMoNx/CNTs for Ammonia Decomposition

2012 ◽  
Vol 557-559 ◽  
pp. 1514-1517
Author(s):  
Zhao Hui Zhao ◽  
Han Bo Zou ◽  
Wei Ming Lin
Keyword(s):  
Physical Adsorption ◽  
Catalyst Activity ◽  
Catalytic Performance ◽  
Ammonia Decomposition ◽  
Molybdenum Nitride ◽  
Nitriding Temperature ◽  
X Ray Diffraction ◽  
Cobalt Molybdenum Nitride ◽  
Temperature Programmed ◽  
Temperature Programmed Reaction

A series of cobalt-molybdenum nitride catalysts were prepared using Co-Mo oxide precursors via temperature-programmed reaction in N2-H2 mixed gases. The catalysts were characterized by N2 physical adsorption, X-ray diffraction, temperature-programmed desorption of H2. Their catalytic performance was evaluated in the model reaction of ammonia decomposition. The influence of the final nitriding temperatures on the surface properties and the catalytic perfomance of CoMoNx/CNTs were described. The catalyst nitrided at 650°C shows the best catalytic performance. The results indicated that a suitable final nitriding temperature contributes directly to the formation of nitrides and favor the catalyst activity.

Effects of SiO2/Al2O3 Ratio on Physicochemical Properties and Catalytic Performance of the Non-Templated ZSM-5 Zeolite

2011 ◽  
Vol 197-198 ◽  
pp. 992-995
Author(s):  
Wei Qiao Liu ◽  
Wei Ning Lei ◽  
Tong Ming Shang ◽  
Zhi Gang Mou ◽  
Heng Qiang Wang ◽  
...  
Keyword(s):  
Catalytic Properties ◽  
Temperature Programmed Desorption ◽  
Catalytic Performance ◽  
Acid Sites ◽  
X Ray Diffraction ◽  
Lewis Acid Sites ◽  
X Ray ◽  
Transmission Electron ◽  
Ft Ir ◽  
Temperature Programmed

The ZSM-5 zeolites of various SiO2/Al2O3ratios were synthesized without using any template agent. X-ray diffraction (XRD), transmission electron microscope (TEM), temperature- programmed desorption of ammonia (NH3-TPD) and Fourier transform infrared spectroscopy (FT-IR) techniques were employed to analyze the natures of the as-synthesized zeolite. The results show that the as-synthesized non-templated ZSM-5 zeolite is very pure. Meanwhile, Lewis acid sites and Bronsted acid sites are all presented in the as-synthesized non-templated HZSM-5 zeolite. The number of acid sites decreases almost linearly with the increasing of SiO2/Al2O3ratio of the zeolite. In addition, the reaction of propylene oligomerization was carried out over the as-synthesized non-templated HZSM-5 zeolite to evaluate the catalytic properties. The results show that the catalytic activity of propylene oligomerization decreases with the increasing of SiO2/Al2O3ratio.

scholarly journals Influence of Sulfur-Containing Sodium Salt Poisoned V2O5–WO3/TiO2 Catalysts on SO2–SO3 Conversion and NO Removal

Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 541 ◽  
Author(s):  
Haiping Xiao ◽  
Chaozong Dou ◽  
Hao Shi ◽  
Jinlin Ge ◽  
Li Cai
Keyword(s):  
Photoelectron Spectroscopy ◽  
No Reduction ◽  
Catalytic Performance ◽  
Acid Sites ◽  
Impregnation Method ◽  
So2 Oxidation ◽  
Sodium Salts ◽  
X Ray ◽  
Temperature Programmed ◽  
Physical Features

A series of poisoned catalysts with various forms and contents of sodium salts (Na2SO4 and Na2S2O7) were prepared using the wet impregnation method. The influence of sodium salts poisoned catalysts on SO2 oxidation and NO reduction was investigated. The chemical and physical features of the catalysts were characterized via NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). The results showed that sodium salts poisoned catalysts led to a decrease in the denitration efficiency. The 3.6% Na2SO4 poisoned catalyst was the most severely deactivated with denitration efficiency of only 50.97% at 350 °C. The introduction of SO42− and S2O72− created new Brønsted acid sites, which facilitated the adsorption of NH3 and NO reduction. The sodium salts poisoned catalysts significantly increased the conversion of SO2–SO3. 3.6%Na2S2O7 poisoned catalyst had the strongest effect on SO2 oxidation and the catalyst achieved a maximum SO2–SO3-conversion of 1.44% at 410 °C. Characterization results showed sodium salts poisoned catalysts consumed the active ingredient and lowered the V4+/V5+ ratio, which suppressed catalytic performance. However, they increased the content of chemically adsorbed oxygen and the strength of V5+=O bonds, which promoted SO2 oxidation.

In-situ FTIR to unravel the bifunctional nature of aromatics hydrogenation synergy on zeolite / metal catalysts

2022 ◽  
Author(s):  
Nuno Batalha ◽  
Jean-Dominique Comparot ◽  
Anthony Le Valant ◽  
Ludovic Pinard
Keyword(s):  
Catalytic Performance ◽  
Acid Sites ◽  
Metal Catalysts ◽  
In Situ Ftir

Acid sites, in particular Brønsted sites, are often reported to enhance the catalytic performance of metal catalysts, like platinum, in hydrogenation. The significant boost in catalytic performance suggests a bifunctional...

scholarly journals Effect of Zirconia Polymorph on Vapor-Phase Ketonization of Propionic Acid

Catalysts ◽  
2019 ◽  
Vol 9 (9) ◽  
pp. 768 ◽  
Author(s):  
Shuang Ding ◽  
Jiankang Zhao ◽  
Qiang Yu
Keyword(s):  
Propionic Acid ◽  
Vapor Phase ◽  
Surface Concentration ◽  
X Ray Diffraction ◽  
In Situ Drifts ◽  
X Ray ◽  
Surface Intermediates ◽  
Temperature Programmed ◽  
Diffuse Reflectance Infrared

Vapor-phase ketonization of propionic acid derived from biomass was studied at 300–375 °C over ZrO2 with different zirconia polymorph. The tetragonal ZrO2 (t-ZrO2) are more active than monoclinic ZrO2 (m-ZrO2). The results of characterizations from X-ray diffraction (XRD) and Raman suggest m-ZrO2 and t-ZrO2 are synthesized by the solvothermal method. NH3 and CO2 temperature-programmed desorption (NH3-TPD and CO2-TPD) measurements show that there were more medium-strength Lewis acid base sites with lower coordination exposed on m-ZrO2 relative to t-ZrO2, increasing the adsorption strength of propionic acid. The in situ DRIFTS (Diffuse reflectance infrared Fourier transform spectroscopy) of adsorbed propionic acid under ketonization reaction reveal that as the most abundant surface intermediates, the monodentate propionates are more active than bidentate propionates. In comparison with m-ZrO2, the t-ZrO2 surface favors monodentate adsorption over bidentate adsorption. Additionally, the adsorption strength of monodentate propionate is weaker on t-ZrO2. These differences in adsorption configuration and adsorption strength of propionic acid are affected by the zirconia structure. The higher surface concentration and weaker adsorption strength of monodentate propionates contribute to the higher ketonization rate in the steady state.

scholarly journals Generalized Methodology for Inserting Metal Heteroatoms into the Layered Zeolite Precursor RUB-36 by Interlayer Expansion

Crystals ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 530 ◽  
Author(s):  
Chaoqun Bian ◽  
Xiao Wang ◽  
Lan Yu ◽  
Fen Zhang ◽  
Jie Zhang ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Catalytic Performance ◽  
X Ray Diffraction ◽  
Zeolite Sample ◽  
X Ray ◽  
Inductively Coupled ◽  
Temperature Programmed ◽  
First Time ◽  
N2 Sorption

The incorporation of metal heteroatoms into zeolites is an effective modification strategy for enhancing their catalytic performance. Herein, for the first time we report a generalized methodology for inserting metal heteroatoms (such as Sn, Fe, Zn, and Co) into the layered zeolite precursor RUB-36 via interlayer expansion by using the corresponding metal acetylacetate salt. Through this generalized methodology, Sn-JHP-1, Fe-JHP-1, Zn-JHP-1 and Co-JHP-1 zeolites could be successfully prepared by the reaction of RUB-36 and corresponding metal acetylacetate salt at 180 °C for 24 h in the presence of HCl solution. As a typical example, Sn-JHP-1 and calcined Sn-JHP-1 (Sn-JHP-2) zeolite is well characterized by the X-ray diffraction (XRD), diffuse reflectance ultraviolet-visible (UV-Vis), inductively coupled plasma (ICP), N2 sorption, temperature-programmed-desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS) techniques, which confirm the expansion of adjacent interlayers and thus the incorporation of isolated Sn sites within the zeolite structure. Notably, the obtained Sn-JHP-2 zeolite sample shows enhanced catalytic performance in the conversion of glucose to levulinic acid (LA) reaction.

scholarly journals “PdO vs. PtO”—The Influence of PGM Oxide Promotion of Co3O4 Spinel on Direct NO Decomposition Activity

Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 62 ◽  
Author(s):  
Gunugunuri K. Reddy ◽  
Torin C. Peck ◽  
Charles A. Roberts
Keyword(s):  
Photoelectron Spectroscopy ◽  
No Decomposition ◽  
Single Element ◽  
X Ray Diffraction ◽  
X Ray ◽  
Promotional Effect ◽  
Ft Ir ◽  
Temperature Programmed ◽  
Thermal Stability Of

Direct decomposition of NO into N2 and O2 (2NO→N2 + O2) is recognized as the “ideal” reaction for NOx removal because it needs no reductant. It was reported that the spinel Co3O4 is one of the most active single-element oxide catalysts for NO decomposition at higher reaction temperatures, however, activity remains low below 650 °C. The present study aims to investigate new promoters for Co3O4, specifically PdO vs. PtO. Interestingly, the PdO promoter effect on Co3O4 was much greater than the PtO effect, yielding a 4 times higher activity for direct NO decomposition at 650 °C. Also, Co3O4 catalysts with the PdO promoter exhibit higher selectivity to N2 compared to PtO/Co3O4 catalysts. Several characterization measurements, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature programmed reduction (H2-TPR), and in situ FT-IR, were performed to understand the effect of PdO vs. PtO on the properties of Co3O4. Structural and surface analysis measurements show that impregnation of PdO on Co3O4 leads to a greater ease of reduction of the catalysts and an increased thermal stability of surface adsorbed NOx species, which contribute to promotion of direct NO decomposition activity. In contrast, rather than remaining solely as a surface species, PtO enters the Co3O4 structure, and it promotes neither redox properties nor NO adsorption properties of Co3O4, resulting in a diminished promotional effect compared to PdO.

scholarly journals In-Exchanged CHA Zeolites for Selective Dehydrogenation of Ethane: Characterization and Effect of Zeolite Framework Type

Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 807
Author(s):  
Zen Maeno ◽  
Xiaopeng Wu ◽  
Shunsaku Yasumura ◽  
Takashi Toyao ◽  
Yasuharu Kanda ◽  
...  
Keyword(s):  
Active Sites ◽  
Temperature Programmed Desorption ◽  
X Ray Diffraction ◽  
Zeolite Framework ◽  
X Ray ◽  
Catalytic Activities ◽  
Ethane Dehydrogenation ◽  
Temperature Programmed

In this study, the characterization of In-exchanged CHA zeolite (In-CHA (SiO2/Al2O3 = 22.3)) was conducted by in-situ X-ray diffraction (XRD) and ammonia temperature-programmed desorption (NH3-TPD). We also prepared other In-exchanged zeolites with different zeolite structures (In-MFI (SiO2/Al2O3 = 22.3), In-MOR (SiO2/Al2O3 = 20), and In-BEA (SiO2/Al2O3 = 25)) and different SiO2/Al2O3 ratios (In-CHA(Al-rich) (SiO2/Al2O3 = 13.7)). Their catalytic activities in nonoxidative ethane dehydrogenation were compared. Among the tested catalysts, In-CHA(Al-rich) provided the highest conversion. From kinetic experiments and in-situ Fourier transform infrared (FTIR) spectroscopy, [InH2]+ ions are formed regardless of SiO2/Al2O3 ratio, serving as the active sites.

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