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Using renewable green hydrogen and carbon dioxide (CO2) to produce methanol is one of the fundamental ways to reduce CO2 emissions in the future, and research and development related to catalysts for efficient and stable methanol synthesis is one of the key factors in determining the entire synthesis process. Metal nanoparticles stabilized on a support are frequently employed to catalyze the methanol synthesis reaction. Metal-support interactions (MSIs) in these supported catalysts can play a significant role in catalysis. Tuning the MSI is an effective strategy to modulate the activity, selectivity, and stability of heterogeneous catalysts. Numerous studies have been conducted on this topic; however, a systematic understanding of the role of various strengths of MSI is lacking. Herein, three Cu/ZnO-SiO2 catalysts with different strengths of MSI, namely, normal precipitation Cu/ZnO-SiO2 (Nor-CZS), co-precipitation Cu/ZnO-SiO2 (Co-CZS), and reverse precipitation Cu/ZnO-SiO2 (Re-CZS), were successfully prepared to determine the role of such interactions in the hydrogenation of CO2 to methanol. The results of temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) characterization illustrated that the MSI of the catalysts was considerably affected by the precipitation sequence. Fourier transform infrared reflection spectroscopy (FT-IR) results indicated that the Cu species existed as CuO in all cases and that copper phyllosilicate was absent (except for strong Cu-SiO2 interaction). Transmission electron microscopy (TEM), X-ray diffraction (XRD), and N2O chemical titration results revealed that strong interactions between the Cu and Zn species would promote the dispersion of Cu species, thereby leading to a higher CO2 conversion rate and improved catalytic stability. As expected, the Re-CZS catalyst exhibited the highest activity with 12.4% CO2 conversion, followed by the Co-CZS catalyst (12.1%), and the Nor-CZS catalyst (9.8%). After the same reaction time, the normalized CO2 conversion of the three catalysts decreased in the following order: Re-CZS (75%) > Co-CZS (70%) > Nor-CZS (65%). Notably, the methanol selectivity of the Re-CZS catalyst was found to level off after a prolonged period, in contrast to that of Co-CZS and Nor-CZS. Investigation of the structural evolution of the catalyst with time on stream revealed that the high methanol selectivity of the catalyst was caused by the reconstruction of the catalyst, which was induced by the strong MSI between the Cu and Zn species, and the migration of ZnO onto Cu species, which caused an enlargement of the Cu/ZnO interface. This work offers an alternative strategy for the rational and optimized design of efficient catalysts. 相似文献
23.
环丙基甲基酮是合成环丙氟哌酸类广谱抗菌药物和抗艾滋特效药依法韦仑的重要中间体,在医药、化工及农林等领域均有广泛应用。环丙基甲基酮的合成方法大致分为4类,分别以酮类、酯类、醇类及呋喃有机物为原料,在一定条件下生成环丙基甲基酮粗品,经萃取及精馏得到环丙基甲基酮纯品。本文综述了环丙基甲基酮的合成研究进展。 相似文献
24.
Qingde Zhang Yisheng Tan Caihong Yang Yizhuo Han Jun Shamoto Noritatsu Tsubaki 《天然气化学杂志》2007,16(3):322-325
The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40(40%)/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40(40%)/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40(40%)/SiO2. 相似文献
25.
C.L. Liu X.Y. Wang Z.M. Wang S.S. Li C.T. Xin H.F. Wang B. Li L. Jiang 《Journal of Radioanalytical and Nuclear Chemistry》2001,250(3):587-591
The migration of 99Tc in a weak loess aquifer was investigated in-situ with undisturbed aquifer medium columns. The columns were obtained horizontally at a depth of 3236 m in an Underground Research Facility (URF). Quartz containing 3H (HTO) and 99Tc (in the form of 99TcO4
-) was introduced into one end of the columns and the columns were covered tightly. Aquifer water was introduced into the columns directly from an experimental shaft in the UFR. Effluents from the columns were collected and the activity of 3H and 99Tc were determined with a liquid scintillation analyzer. The breakthrough curves of 3H and 99Tc indicate that 99Tc migrates a little faster than that 3H does in the aquifer. 相似文献
26.
The interaction of cyclodextrins with meso- Tetrakis (4-N-trimethylaminobenzyl) porphyrin (TAPP) in 0.1 mol l(-1) phosphate buffer (pH 7.0, 20 degrees C) has been studied by polarography. The TAPP can form the 1:1 inclusion complex with Sulfobutylether-beta-cyclodextrin (SBE-beta-CD) and1:2 inclusion complexes with other four cyclodextrins. A new expression, which is used to calculate the inclusion constant for1:2 inclusion complex by polarography, has been educed and testified firstly in this paper. Furthermore, the inclusion abilities of different kinds of cyclodextrins are compared. The result shows the inclusion ability of anionic cyclodextrin SBE-beta-CD with cationic porphyrin TAPP is very strong. It suggests that the charge attraction between CDs and TAPP plays an important role in the inclusion procedure except for the hydrophobic effect. The inclusion formation of anionic cyclodextrins with drugs can increase released rate of drugs at high pH; therefore, the suparmolecular data for the controlled release of the drugs that owned the similar properties as hematoporphyrin have been offered by polarography in this paper. 相似文献
27.
J. M. Wang R. Ballad P. Grimaldi W. Lei 《Journal of Radioanalytical and Nuclear Chemistry》1983,76(1):105-108
A manganese dioxide coprecipitation procedure is utilized to replace a time-consuming evaporation step for the extraction
of thorium, uranium and cerium from freshwater samples. The average recovery for 20-liter samples is greater than 95% for234Th and144Ce. The data indicate that the manganese dioxide coprecipitation process does not affect the recovery of thorium and uranium
during our routine analytical procedure. 相似文献
28.
29.
A study of carboxylic-modified mesoporous silica in controlled delivery for drug famotidine 总被引:2,自引:0,他引:2
A series of pure silica MSU and carboxylic-modified MSU materials were prepared. The formation of mesoporous silica materials with terminal carboxylic groups on pore surface was performed by the acid-catalyzed hydrolysis of cyano to carboxylic. Then their potential applications in controlled drug delivery carriers were investigated. Drug famotidine was selected as a model molecule out of the consideration of the terminal amino groups in its molecule. The adsorption experiments show significant adsorption of famotidine on the carboxylic-modified MSU materials. And, the functionalization level of carboxylic groups has been found to be the key factor affecting the adsorption capacities of the modified MSU materials for famotidine. Subsequently, three kinds of release fluids, including simulated gastric medium, simulated intestinal medium, and simulated body fluid, were used to test the famotidine release rate from the carboxylic-modified MSU material. Obvious delayed effect has been observed for the famotidine release from the carboxylic-modified mesoporous silica material under the in vitro assays. 相似文献
30.
《Spectrochimica Acta Part B: Atomic Spectroscopy》2005,60(7-8):905-914
In this work, an aluminum laser plasma produced in ambient air at atmospheric pressure by laser pulses at a fluence of 10 J/cm2 is characterized by time- and space-resolved measurements of electron density and temperature. Varying the laser pulse duration from 6 ns to 80 fs and the laser wavelength from ultraviolet to infrared only slightly influences the plasma properties. The temperature exhibits a slight decrease both at the plasma edge and close to the target surface. The electron density is found to be spatially homogeneous in the ablation plume during the first microsecond. Finally, the plasma expansion is in good agreement with the Sedov's model during the first 500 ns and it becomes subsonic, with respect to the velocity of sound in air, typically 1 μs after the plasma creation. The physical interpretation of the experimental results is also discussed to the light of a one-dimensional fluid model which provides a good qualitative agreement with measurements. 相似文献