Abstract:Mordenite (H-MOR) catalysts were synthesized by a hydrothermal method, and silver-modified mordenite (Ag-MOR) catalysts were prepared by ion exchange with AgNO3 at different concentrations. The performance of these catalysts in the carbonylation of dimethyl ether (DME) to methyl acetate (MA) was also evaluated. The catalysts were characterized by Ar adsorption/desorption, XRD, ICP-AES, SEM, HRTEM, 27Al NMR, H2-TPR, NH3-TPD, Py-IR, and CO-TPD. According to the characterization results, Ag ion exchange sites wer… Show more
“…To further investigate the interaction of H 3 PO 4 with Ag NPs, we characterized Ag + /MCM-48 (unreduced) and Ag + / MCM-48-H 3 PO 4 (unreduced) by H 2 -TPR (Figure 4f). The TPR profile of Ag + /MCM-48 (unreduced) demonstrates reduction in peak maxima at temperatures close to 80 and 280 °C, attributed to the reduction of Ag x O y and some positive valence silver in MCM-48 pores, 9,36 respectively. The addition of H 3 PO 4 leads to the shift of TPR peak to the higher temperature up to 155 °C, indicated that there may be a strong coordination between the loaded phosphoric acid and Ag ions, and it is consistent with the XPS and 31 P SSNMR results above.…”
Supported silver nanoparticle (Ag NP) catalysts usually have high reactivity for organic oxidation reactions; however, catalyst deactivation caused by the migration, aggregation, and oxidation of Ag NPs during catalytic reactions pose significant challenges in their practical applications. Herein, mesoporous MCM-48 was employed as a carrier to covalently graft phosphoric acid and Ag NPs on its surface, affording supported Ag NP catalyst Ag/MCM-48-H 3 PO 4 . A variety of spectral characterizations reveal that there is an electron-donating effect of the grafted phosphoric acid moieties on the MCM-48 surface toward Ag NPs, which induce a higher Ag 0 /Ag + ratio in comparison to Ag/MCM-48 without H 3 PO 4 modification. Consequently, Ag/MCM-48-H 3 PO 4 exhibits better activity than Ag/MCM-48 for the selective oxidation of ethylene glycol in a fixed-bed reactor under more energyefficient reaction conditions. In addition, Ag/MCM-48-H 3 PO 4 can also prevent the migration, aggregation, and oxidation of reactive Ag NP species in the reaction process due to the coordination and molecular fence effect generated by MCM-48 surface phosphoric acid functionalization, thus exhibiting higher stability than Ag/MCM-48.
“…To further investigate the interaction of H 3 PO 4 with Ag NPs, we characterized Ag + /MCM-48 (unreduced) and Ag + / MCM-48-H 3 PO 4 (unreduced) by H 2 -TPR (Figure 4f). The TPR profile of Ag + /MCM-48 (unreduced) demonstrates reduction in peak maxima at temperatures close to 80 and 280 °C, attributed to the reduction of Ag x O y and some positive valence silver in MCM-48 pores, 9,36 respectively. The addition of H 3 PO 4 leads to the shift of TPR peak to the higher temperature up to 155 °C, indicated that there may be a strong coordination between the loaded phosphoric acid and Ag ions, and it is consistent with the XPS and 31 P SSNMR results above.…”
Supported silver nanoparticle (Ag NP) catalysts usually have high reactivity for organic oxidation reactions; however, catalyst deactivation caused by the migration, aggregation, and oxidation of Ag NPs during catalytic reactions pose significant challenges in their practical applications. Herein, mesoporous MCM-48 was employed as a carrier to covalently graft phosphoric acid and Ag NPs on its surface, affording supported Ag NP catalyst Ag/MCM-48-H 3 PO 4 . A variety of spectral characterizations reveal that there is an electron-donating effect of the grafted phosphoric acid moieties on the MCM-48 surface toward Ag NPs, which induce a higher Ag 0 /Ag + ratio in comparison to Ag/MCM-48 without H 3 PO 4 modification. Consequently, Ag/MCM-48-H 3 PO 4 exhibits better activity than Ag/MCM-48 for the selective oxidation of ethylene glycol in a fixed-bed reactor under more energyefficient reaction conditions. In addition, Ag/MCM-48-H 3 PO 4 can also prevent the migration, aggregation, and oxidation of reactive Ag NP species in the reaction process due to the coordination and molecular fence effect generated by MCM-48 surface phosphoric acid functionalization, thus exhibiting higher stability than Ag/MCM-48.
“…In heterogeneous catalysis using supported zeolite catalysts, active site concentration, feed diffusion, and site accessibility play vital roles . Incorporation of metallic nanoparticles onto the channels and cavities of zeolite materials − has a critical effect on their catalytic properties and stability. Inoue et al reported in 1995 the effect of silver-exchanged zeolites on the methanol to aromatics conversion .…”
Aromatics are one of the most highly demanded hydrocarbon raw materials for the chemical industry. In the present study, efforts are made to understand the promotional effect of silver together with gallium on ZSM-5 zeolite as a catalyst for the reforming reaction of realistic, full range commercial naphtha feed in a fixed bed reactor at atmospheric pressure and 550 °C temperature. The dual metal system showed a synergic effect to enhance the aromatic selectivity and liquid yield and decrease the off-gas formation. The catalyst samples are prepared by desilication followed by co-impregnation of silver and gallium on to ZSM-5, characterized by X-ray diffraction, N 2 adsorption, NH 3 desorption, pyridine-FTIR, temperature-programmed reduction, and analysis of morphology. It is observed from reduction studies that upon incorporation of silver and gallium, catalyst properties like proton abstraction, reducibility, Lewis and Bronsted acidities, etc. are favorably modified. These results are discussed in detail, and an attempt is made to correlate them with the catalytic reaction results obtained.
“…Various metallic species, such as ions, clusters and nanoparticles, deposited on the surface or implanted into zeolites and other microporous, mesoporous and nanoporous matrices, are of great interest for the development of nanostructured materials for diverse applications in areas such as catalysis [1][2][3][4][5][6][7], water purification [8][9][10][11][12], general medicine [13,14], synthesis of antimicrobial and antifungal materials [15][16][17] and in a number of otherareas [18][19][20][21][22][23]. The development of packing materials containing zeolites modified with silver, copper and zinc ions and metal nanoparticles, which have antimicrobial and fungicidal properties is reviewed in [15,20,23].…”
Long-term changes in nanoparticles of copper-silver bimetallic systems on natural clinoptilolite obtained by ion exchange of Cu2+ and Ag+, and then reduced at different temperatures, have been studied. Even after storage under ambient conditions, XRD and UV-Vis diffuse reflectance spectra indicate the presence of nanospecies of reduced copper and silver. Scanning Electron Microscopy of aged bimetallic samples, reduced at the highest temperature (450oC) and the primary samples for their preparation, also aged, showed the presence of silver nanoparticles with a size of about 100 nm. They are formed in the initial ion-exchanged sample (without reduction) due to the degradation of Ag+ ions. The nanoparticles in the reduced sample are larger; in both samples they are evenly distributed over the surface. The presence of silver affects the stability and the mechanism of decomposition/oxidation of reduced copper nanospecies, and this stability is higher in bimetallic systems. The decomposition pattern of recently reduced species includes the formation of smaller nanoparticles and few-atomic clusters. This can occur, preceding the complete oxidation of Cu to ions. Quasi-colloidal silver, which is present in fresh bimetallic samples reduced at lower temperatures, transforms after aging into Ag8 clusters, which indicates the stability of these nanospecies on natural clinoptilolite.
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