scholarly journals Synthesis of Dimethyl Carbonate from CO2 and Methanol over Zr-Based Catalysts with Different Chemical Environments

Catalysts ◽  
2021 ◽  
Vol 11 (6) ◽  
pp. 710
Author(s):  
Linmeng Huo ◽  
Tian Wang ◽  
Keng Xuan ◽  
Lei Li ◽  
Yanfeng Pu ◽  
...  

The adsorption and activation of both CO2 and methanol are mainly affected by the distance of the Lewis acid site, Zr4+, and Lewis base, Zr4+/O2−, of the Zr-based catalysts. In this paper, Zr-incorporated SBA-15 (Zr-SBA-15) and Zr-grafted SBA-15 (Zr/SBA-15) catalysts were prepared with different Zr environments, and were analyzed with N2 adsorption–desorption isotherms, X-ray diffraction, UV-vis spectra, and XPS. It was proposed that Zr-SBA-15 catalyst with Si-O-Zr-OH and Zr-O-Si-OH structure exhibited non-adjacent sites between Zr4+ and Zr4+/O2−, while Zr/SBA-15 catalyst with Zr-O-Zr-OH structure showed neighboring sites between Zr4+ and Zr4+/O2−. Furthermore, the Zr/SBA-15 catalyst exhibited good catalytic activity, while no DMC was detected over the Zr-SBA-15 catalyst at the same reaction conditions. For combined in situ infrared and catalytic performance, it was indicated that the methanol and CO2 could be activated to form DMC, only when the Zr4+ and Zr4+/O2− sites existed and were adjacent to each other in the Zr-O-Zr-OH of Zr/SBA-15 catalyst.

2020 ◽  
Vol 4 (4) ◽  
pp. 1-3
Author(s):  
Liu L

The mesoporous ZSM-5 zeolite containing MoCoP/Al2O3 catalyst (C12-ZSM5) with the mixture of Al2O3 and mesoporous ZSM- 5 zeolite as carrier was synthesized. The catalytic performance of C12-ZSM5 catalyst was evaluated by the hydrodesulfurization (HDS) of different diesel feedstock. The carriers and catalysts were characterized by N2 adsorption-desorption, pyridine-FTIR, X-ray diffraction (XRD) and CO in-situ FTIR (CO-FTIR) techniques. Results showed that mesoporous ZSM-5 can improve the acidity of the catalyst and increase the number of MoCoS active phases. The C12-ZSM5 catalyst had low HDS and HDN activity, because the acidic sites of mesoporous ZSM-5 were easily occupied by nitrogen compounds. The HDS activity of C12-ZSM5 catalyst was fully exploited by using graded packing technology, the sulfur content of product oil was 5.9 ng/μL. The relative HDS activity of C12-ZSM5 catalyst is 1.47 times that of FHUDS-8 catalyst.


2018 ◽  
Author(s):  
Laura Abad Galán ◽  
Alexandre N. Sobolev ◽  
Eli Zysman-Colman ◽  
Mark Ogden ◽  
Massimiliano Massi

<i>β</i>-Triketonates have been recently used as chelating ligands for lanthanoid ions, presenting unique structures varying from polynuclear assemblies to polymers. In an effort to overcome low solubility of the complexes of tribenzoylmethane, four <i>β</i>-triketones with higher lipophilicity were synthesised. Complexation reactions were performed for each of these molecules using different alkaline bases in alcoholic media. X-ray diffraction studies suggested that the ligands were undergoing decomposition under the reaction conditions. This is proposed to be caused by <i>in situ</i>retro-Claisen condensation reactions, consistent with two examples that have been reported previously. The lability of the lanthanoid cations in the presence of a varying set of potential ligands gave rise to structures where one, two, or three of the molecules involved in the retro-Claisen condensationreaction were linked to the lanthanoid centres. These results, along with measurements of ligand decomposition in the presence of base alone, suggest that using solvents of lower polarity will mimimise the impact of the retro-Claisen condensation in these complexes. <br>


2019 ◽  
Vol 44 (1) ◽  
pp. 37-44 ◽  
Author(s):  
Yunwu Yu ◽  
Lianjie Liang ◽  
Changwei Xu ◽  
Yubo Dai ◽  
Wenhao Pan ◽  
...  

A series of ceria promoted Ni2P catalysts were prepared and evaluated in dibenzothiophene hydrodesulfurization steam. These catalysts were characterized by X-ray diffraction, N2 adsorption–desorption, CO chemisorptions, and X-ray photoelectron spectroscopy. The results showed that the addition of ceria into the bulk Ni2P catalyst was conducive to the formation of the Ni2P phase and contributed to a higher surface area, leading to a better dispersion and smaller crystallite size of Ni2P particles. The CexNi2P catalysts showed higher dibenzothiophene hydrodesulfurization activity than Ni2P catalyst and the Ce0.09Ni2P catalyst showed the highest dibenzothiophene hydrodesulfurization activity. The Ce0.09Ni2P catalyst showed a dibenzothiophene hydrodesulfurization conversion of 94.5% at the reaction conditions of 320°C, 4.0 MPa, a H2/oil ratio of 500 (V/V), and a weight hourly space velocity of 8.0 h−1. The dibenzothiophene was mainly transformed through desulfurization pathway.


Catalysts ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 155 ◽  
Author(s):  
Zhenheng Diao ◽  
Lushi Cheng ◽  
Xu Hou ◽  
Di Rong ◽  
Yanli Lu ◽  
...  

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.


Nanomaterials ◽  
2020 ◽  
Vol 10 (9) ◽  
pp. 1643 ◽  
Author(s):  
Oleg A. Usoltsev ◽  
Anna Yu. Pnevskaya ◽  
Elizaveta G. Kamyshova ◽  
Andrei A. Tereshchenko ◽  
Alina A. Skorynina ◽  
...  

Adsorption of ethylene on palladium, a key step in various catalytic reactions, may result in a variety of surface-adsorbed species and formation of palladium carbides, especially under industrially relevant pressures and temperatures. Therefore, the application of both surface and bulk sensitive techniques under reaction conditions is important for a comprehensive understanding of ethylene interaction with Pd-catalyst. In this work, we apply in situ X-ray absorption spectroscopy, X-ray diffraction and infrared spectroscopy to follow the evolution of the bulk and surface structure of an industrial catalysts consisting of 2.6 nm supported palladium nanoparticles upon exposure to ethylene under atmospheric pressure at 50 °C. Experimental results were complemented by ab initio simulations of atomic structure, X-ray absorption spectra and vibrational spectra. The adsorbed ethylene was shown to dehydrogenate to C2H3, C2H2 and C2H species, and to finally decompose to palladium carbide. Thus, this study reveals the evolution pathway of ethylene on industrial Pd-catalyst under atmospheric pressure at moderate temperatures, and provides a conceptual framework for the experimental and theoretical investigation of palladium-based systems, in which both surface and bulk structures exhibit a dynamic nature under reaction conditions.


2013 ◽  
Vol 634-638 ◽  
pp. 696-700
Author(s):  
Lin Jiu Xiao ◽  
Peng Li ◽  
Yong Gang Sheng

A series of Ti(SO4)2/γ-Al2O3 catalysts were prepared by impregnation method and the catalytic performance of these catalysts in 1-butene oligomerization was investigated. The heat treatment temperature played great influences on the catalytic performance of these catalysts in the oligomerization. 90.1 wt.% conversion of 1-butene and 92.2 wt.% selectivity of dimers were obtained on Ti(SO4)2/γ-Al2O3(450) catalyst at 80 °C, 1.0 Mpa and LHSV=0.6 h−1. The heat treatment temperature determined the crystallinity of TiOSO4 and specific surface area of these catalysts, which affected the catalytic performance of these catalysts in 1-butene oligomerization. In addition, the physicochemical properties of these catalysts were comparatively characterized by powder X-ray diffraction (XRD), N2 isothermal adsorption-desorption techniques.


2010 ◽  
Vol 93-94 ◽  
pp. 22-26 ◽  
Author(s):  
Surachai Artkla ◽  
Won Yong Choi ◽  
Jatuporn Wittayakun

This work compared properties and catalytic performance of two hybrid photocatalysts, TiO2/RH-MCM-41 and TiO2/TEOS-MCM-41 prepared by loading nanoparticles of TiO2 (10 wt.%) on MCM-41 synthesized with rice husk silica and tetraethyl orthosilicate respectively. The supports and catalysts were characterized by X-ray diffraction, N2 adsorption-desorption, transmission electron microscopy and zeta potential. The photocatalytic activities of the TiO2/RH-MCM-41 and TiO2/TEOS-MCM-41 for the degradation of tetramethylammonium (TMA) in aqueous slurry were similar with a complete conversion after irradiation time of 90 min at pH 7.


MRS Bulletin ◽  
2007 ◽  
Vol 32 (12) ◽  
pp. 1038-1043 ◽  
Author(s):  
John Evans ◽  
Anna Puig-Molina ◽  
Moniek Tromp

AbstractX-ray absorption fine structure (XAFS) spectroscopy probes the structure and electronic properties of metal centers. Because it can be applied to noncrystalline materials, it is a key technique for probing nanoparticulate materials, such as colloidal and heterogeneous metal catalysts. The high brilliance of modern synchrotron radiation x-ray sources facilitates in situ studies, which provide direct structure–function relationships with both spatial and time resolution; this is especially effective when applied in combination with complementary techniques such as x-ray diffraction, mass spectrometry, and optical or vibrational spectroscopies. Tracking the particle formation of platinum-group metal catalysts, their behavior under reaction conditions, and the distribution of sites within a catalyst bed shows that this approach is essential for understanding the chemistry of these nanoparticles. Rather than behave as monolithic entities, nanoparticulate catalysts undergo rapid structural transformations induced by the gas environment and reaction conditions, and their lifetimes as catalysts depend on the reversibility of these changes.


2021 ◽  
Vol 21 (12) ◽  
pp. 6082-6087
Author(s):  
Chih-Wei Tang ◽  
Hsiang-Yu Shih ◽  
Ruei-Ci Wu ◽  
Chih-Chia Wang ◽  
Chen-Bin Wang

The increase of harmful carbon monoxide (CO) caused by incomplete combustion can affect human health even lead to suffocation. Therefore reducing the CO discharged by vehicles or factories is urgent to improve the air quality. The spinel cobalt (II, III) oxide (Co3O4) is an active catalyst for CO abatement. In this study, we tried to fabricate dispersing Co3O4 via the dispersion-precipitation method with acetic acid, formic acid, and oxalic acid as the chelating dispersants. Then, the asprepared samples were calcined at 300 ºC for 4 h to obtain active catalysts, and assigned as Co(A), Co(F) and Co(O) respectively, the amount of the dispersants used are labeled as I (0.12 mole), II (0.03 mole) and III (0.01 mole). For comparison, another CoAP sample was prepared via alkaliinduced precipitation and calcined at 300 ºC. All samples were characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), scanning electron microscope (SEM), and nitrogen adsorption/desorption system, and the catalytic activity focused on the CO oxidation. The influence of chelating dispersant on the performance of abatement of CO was pursued in this study. Apparently, the results showed that the chelating dispersant can influence the catalytic activity of CO abatement. An optimized ratio of dispersant can improve the performance, while excess dispersant lessens the surface area and catalytic performance. The series of Co(O) samples can easily donate the active oxygen since the labile Co–O bonding and indicated the preferential performance than both Co(A) and Co(F) samples. The nanorod Co(O)-II showed preferential for CO oxidation, T50 and T90 approached 96 and 127 ºC, respectively. Also, the favorable durability of Co(O)-II sample maintains 95% conversion still for 50 h at 130 ºC and does not emerge deactivation.


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