پاورپوینت بهبود گزینش پذیری واکنش تبدیل متانول به الفین (مهندسی شیمی)

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وو سمدم رعص وحص In the name of God Improved methanol-to-olefin reaction selectivity and catalyst Ife by CeO? coating of Yerrerite zeolite 

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paypasiaaasd@) Index . Introduction . Zeolites . Reaction MTO . Analyses and Results . Conclusions . Reference 2 3 4 5 6 

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paypasiaaasd@) Introduction The methanol-to-olefin (MTO) or methanol-to- hydrocarbon (MTH) reaction is of importance in both fundamental research and industrial applications because of the increasing demand for lower olefins, such as ethylene, propylene, and butenes, from alternative carbon sources instead of from thermal cracking of naphtha. => INEOS MTO => ‏ء‎ ‎> | MTP tugri => ‏فاد‎ 5۸۶04 

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paypasiaaasd@) Zeolites Fl » MFS » CHA, MTT, TON, *MRE > EUO > SZR,FER. FI, EUO, *MRE, MFS, TON, MTT, and FER zeolites, consisting of 10MR, mainly produce C4+ hydrocarbons. >MFI, EUO, *MRE, and MFS zeolites also produced aromatic compounds, which can lead to significant deterioration of the catalytic performance. *Ca-MFI zeolite impregnated with 35 wt% CeO2 showed five times higher catalytic activity than that of unmodified Ca- MFI zeolite in the dimethylether-to-olefin reaction at 773 K because the CeO2-coated surface strongly inhibited coke formation at the portals. 

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0 . .Agommercial FER zeolite with ۶ ۵ Si02/AI203 molar ratio of 20 «“was obtained from Zeolyst International (CP914C). Cerium nitrate hexahydrate (Yakuri, 98%) was impregnated into FER zeolite using an incipient wetness method by varying the amount of the impregnation material within the range of 10e30 wt%. The ceriacoated FER catalysts (denoted as Ce(x)-FER (x % 10, 20, and 30)) were obtained by drying و ‎eT‏ 0و2 3 1 ِ & 

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وه سصعميعص يحض MTO Reaction 

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paypasiaaiasd@) Analyses and Results (0 م2 Fig. 1, XRD paternsof HOt FER cts with erent 0 adn "A (bce 10} Ce a0) RK, (4) Ce FEK fe) GOs The ed and an ener phase, especie (or mere hs gute gen the eater lev othe we 

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paypasiaaasd@) Analyses and Results Teal pry ata andthe pice ie ata cn eyo te coated ER cas ‏کار‎ Cebaing amount wt?’ ‏اما رها‎ Forel c) ها ‎Miu Extra Tol‏ لما ‎TNO |s15) 8 1 1 ۳ ol‏ = 0 19 ۳ 3 17 30 : 0 "1 ‎Ww 3 mat‏ 29 ماللا نك ‎a 1B 10"‏ قلا 0 2۳00 ‎G(R‏ ‎i ۳ oo‏ 146 1 تلع 117 نم الا 1 ‎gh EK ays‏ شاه سس ویو ‎peas wig terse = here Othe mean sie of tallies om), 8‏ ۱ هه اه ارو ‎ste yang ste il whale max FY che dines‏ رای ولا ‎they ange ‎ ‎ ‎ 

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هچ ممم يعض حصن * Analyses and Results 

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paypasiaaiasd@) Analyses and Results ‘elaive pressure (P/F) ‘Quantity adsorbed (em?/eSTP) Fig 5 atin epi ‏ه مها‎ 77 ٩ ‏وراه اج مه یمتا‎ ۱ Ce 20}ER (0) CeO) FER. am (Ce The open and closed sya sepieiea’ the dezepton al alsin bach reper is Fig shows the N2 rption-desorption otherms at 77 K for CeO2- ated FER catalysts. Increasing the CeO2 loading resulted in a decrease of the amount of N2 adsorbed at low P/PO, but a significant increase of the amount of N2 adsorbed at high P/PO. This finding suggested the formation of macroporous CeO2, which would increase the pore volume at high P/PO. 

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paypasiaaiasd@) Analyses and Results conversion (%) 0 0ت عد ص م و ‎‘Time (min}‏ Fe Metin coven at 63K a 12° WHS ver Ce cite FER 2p whet C0, ales 9) 7 ue (10-2, (a) 20, a ‏يل‎ This Fig. shows the MTO conversion as a function of action time. The catalytic activity over the parent FER catalyst decreased dramatically with the time on stream owing to coke formation. Such deactivation is often observed for zeolites with low Si/Al ratios. the MTO conversion increased dramatically with selective CeO2 coating of the catalyst, even at 10 wt%. 

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جسمسیسوصن Analyses and Results @ 0 © @ 

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وج مه رعصوحص pra ‏صم‎ Analyses and Results 7 1 300 400 500 600 700 00 900 1000 1100 1200 1300 ‘Temperature (K) Fa Temagrine mala ae nd 202 co FER ca The coke deposited on the parent FER catalyst as removed readily in the temperature range of 700-900 K, ascribed to the presence of 8.3 wt% heavy coke, as shown in this Fig. > All the weight change was observed in the low-temperature region below 500 K for CeO2 coated FER catalyst. 

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paypasiaaasd@) Analyses and Results Product yields for the MTO reaction at 673 K and 1.2 h”* WHSV over CeO,-coated Ce (30) FER 96 30 35 54 18 241 612 00 04 ۳۳۳ 997 32 HFER Ce (I0}FER Ce 999 34 54 72 17 264 357 02 01 83.8 225 5.0 51 13 206 293 14 13.2 FER catalysts, MeOH conversion (%) Product Yield (3) Methane Ethylene Propylene 8 ‏اب‎ ‎G=+6= ‎Aromatics ‎MeQH + DME 

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paypasiaaasd@) Conclusions In the present work, selective coating of CeO2 on FER zeolite was shown to mask acid sites on the external surface of the eolite, thereby inhibiting heavy coke formation. It was confirmed that that the 2 coating did not cause pore blockage, while acid sites on the external surface were masked effectively. Y Interestingly, the product distribution for MTO conversion over the CeO2 coated FER catalyst supported a reaction mechanism based on the olefin cycle, with high product yields of C4/C4* to C6/C6* (90%) and negligible formation of aromatics, which are associated with heavy coke deposition. 

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paypasiaaasd@) Reference Park, S. J. et al. (2018) ‘Improved methanol- to-olefin reaction selectivity and catalyst life by CeO2 coating of ferrierite zeolite’, Microporous and Mesoporous Materials. Elsevier Ltd, 256, pp. 155-164. doi: 10.1016/j.micromeso.2017.08.003. 

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© Thanks for your attention i i Maryam Nasseri June 2019 

@projectsonline1 In the name of God Improved methanol-to-olefin reaction selectivity and catalyst life by CeO2 coating of ferrierite zeolite 1 Index Introduction Zeolites Reaction MTO Analyses and Results Conclusions Reference @projectsonline1 1. 2. 3. 4. 5. 6. 2 Introduction INEOS MTO SAPO-34 MTP Lugri High-silica ZSM-5 @projectsonline1 The methanol-to-olefin (MTO) or methanol-tohydrocarbon (MTH) reaction is of importance in both fundamental research and industrial applications because of the increasing demand for lower olefins, such as ethylene, propylene, and butenes, from alternative carbon sources instead of from thermal cracking of naphtha. MTO 3 Zeolites @projectsonline1 MFI » MFS » CHA, MTT, TON, *MRE > EUO > SZR,FER. MFI, EUO, *MRE, MFS, TON, MTT, and FER zeolites, consisting of 10MR, mainly produce C4+ hydrocarbons. MFI, EUO, *MRE, and MFS zeolites also produced aromatic compounds, which can lead to significant deterioration of the catalytic performance. Ca-MFI zeolite impregnated with 35 wt% CeO2 showed five times higher catalytic activity than that of unmodified CaMFI zeolite in the dimethylether-to-olefin reaction at 773 K because the CeO2-coated surface strongly inhibited coke formation at the portals. 4 MTO Reaction • Catalyst preparation @projectsonline1 A commercial FER zeolite with a SiO2/Al2O3 molar ratio of 20 was obtained from Zeolyst International (CP914C). Cerium nitrate hexahydrate (Yakuri, 98%) was impregnated into FER zeolite using an incipient wetness method by varying the amount of the impregnation material within the range of 10e30 wt%. The ceriacoated FER catalysts (denoted as Ce(x)-FER (x ¼ 10, 20, and 30)) were obtained by drying 5 MTO Reaction @projectsonline1 6 Analyses and Results @projectsonline1 7 Analyses and Results @projectsonline1 8 Analyses and Results @projectsonline1 9 Analyses and Results @projectsonline1 This Fig shows the N2 adsorption-desorption isotherms at 77 K for CeO2coated FER catalysts. Increasing the CeO2 loading resulted in a decrease of the amount of N2 adsorbed at low P/P0, but a significant increase of the amount of N2 adsorbed at high P/P0. This finding suggested the formation of macroporous CeO2, which would increase the pore volume at high P/P0. 10 Analyses and Results @projectsonline1  This Fig. shows the MTO conversion as a function of reaction time. The catalytic activity over the parent FER catalyst decreased dramatically with the time on stream owing to coke formation. Such deactivation is often observed for zeolites with low Si/Al ratios.  the MTO conversion increased dramatically with selective CeO2 coating of the catalyst, even at 10 wt%. 11 Analyses and Results @projectsonline1 12 Analyses and Results @projectsonline1  The coke deposited on the parent FER catalyst was removed readily in the temperature range of 700-900 K, ascribed to the presence of 8.3 wt% heavy coke, as shown in this Fig.  All the weight change was observed in the low-temperature region below 500 K for CeO2 coated FER catalyst. 13 Analyses and Results @projectsonline1 14 Conclusions @projectsonline1  In the present work, selective coating of CeO2 on FER zeolite was shown to mask acid sites on the external surface of the zeolite, thereby inhibiting heavy coke formation.  It was confirmed that that the CeO2 coating did not cause pore blockage, while acid sites on the external surface were masked effectively.  Interestingly, the product distribution for MTO conversion over the CeO2 coated FER catalyst supported a reaction mechanism based on the olefin cycle, with high product yields of C4/C4+ to C6/C6+ (90%) and negligible formation of aromatics, which are associated with heavy coke deposition. 15 Reference @projectsonline1 Park, S. J. et al. (2018) ‘Improved methanolto-olefin reaction selectivity and catalyst life by CeO2 coating of ferrierite zeolite’, Microporous and Mesoporous Materials. Elsevier Ltd, 256, pp. 155–164. doi: 10.1016/j.micromeso.2017.08.003. 16 Maryam Nasseri June 2019 17 @projectsonline1 Thanks for your attention