Catalytic Compatibility of Methanol with Petroleum Naphtha in Mixed Feeds Used in the Thermal-Catalytic/Steam-Cracking (TCSC) Process for the Production of Propylene and Ethylene

Yan, Haitao; Mao, R. Le Van

doi:10.1007/s10562-011-0734-8

Cited by 7 publications

(2 citation statements)

References 30 publications

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“…These synergies lead to a higher yield of C 2 –C 4 olefins in the joint transformation than theoretically expected by summing the yields of the individual reactions. , Yan and Le Van Mao have also reported a higher yield of ethylene and propylene in the thermal-catalytic steam cracking of methanol/naphtha …”

Section: Introductionmentioning

confidence: 81%

“…16,17 Yan and Le Van Mao have also reported a higher yield of ethylene and propylene in the thermal-catalytic steam cracking of methanol/naphtha. 26 Given the rapid deactivation of the catalyst, a further step toward the viability of the joint transformation of methanol and n-butane requires both a catalyst that can be regenerated and the knowledge of its reactivation kinetics, which will allow studying alternative reaction−regeneration systems. This paper addresses the reactivation of an HZSM-5 zeolite catalyst for which the process kinetics at zero time on stream and deactivation have already been determined.…”

Section: Introductionmentioning

confidence: 99%

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Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles

Aguayo

Gayubo

Ateka

et al. 2012

Ind. Eng. Chem. Res.

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The joint transformation of methanol and n-butane has been studied under energy-neutral conditions (methanol/n-butane molar ratio of 3/1) on an HZSM-5 zeolite catalyst in order to determine the reactivation kinetics and optimize the process conditions for maximizing the light olefin production rate. The methodology for determining the reactivation kinetics combines the kinetic models for the main reaction and deactivation (determined in previous studies), as well as the experimental reactivation results obtained for a reaction step (at 500 and 550 °C) subsequent to regeneration by coke combustion with air (at 550 °C, up to 120 min). By simulation of the operation in reaction–regeneration cycles, an optimum average olefin production rate of 22 mol/(gcatalyst h) is obtained for a reaction temperature of 500 °C, space time of 0.37 gcatalyst h mol–1, time on stream of 40 min, and partial reactivation by coke combustion for 15 min.

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Section: Introductionmentioning

confidence: 81%

Section: Introductionmentioning

confidence: 99%

Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles

Aguayo

Gayubo

Ateka

et al. 2012

Ind. Eng. Chem. Res.

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Alkane Activation Initiated by Hydride Transfer: Co‐conversion of Propane and Methanol over H‐ZSM‐5 Zeolite

Liu

et al. 2015

Angewandte Chemie

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Co-conversion of alkane with another reactant over zeolite catalysts has emerged as an ew approach to the longstanding challenge of alkane transformation. With the aid of solid-state NMR spectroscopya nd GC-MS analysis,i tw as found that the co-conversion of propane and methanol can be readily initiated by hydride transfer at temperatures of ! 449 K over the acidic zeoliteH-ZSM-5. The formation of 13 C-labeled methane and singly 13 C-labeled n-butanes in selective labeling experiments provided the first evidence for the initial hydride transfer from propane to surface methoxy intermediates.T he results not only providenew insight into carbocation chemistry of solid acids,b ut also shed light on the low-temperature transformation of alkanes for industrial applications.Alkanes are the main components in natural gas and crude oil. Thec onversion of abundant but inert alkanes into highvalue-added products has been al ong-standing challenge to chemists. [1] Thed irect transformation of alkanes [2] suffers from the inertness of C À H/C À Cb onds and unfavorable thermodynamics which result in high reaction temperature, low product yield/selectivity,and unrealistic cost for industrial applications.Alternatively,the co-conversion of alkanes with reactive hydrocarbons [3] or oxygenates [4] over zeolites has recently been explored to overcome these limitations.M ethanol is ak ey platform chemical produced from various sources and can be readily converted over acidic zeolites through the industrial process. [5] Many efforts have accordingly been attempted to use methanol as the co-reactant [6] for coupling with methane, [6a] ethane, [6b] C 3 -C 4 alkanes, [6c] nbutane, [6d] n-hexane, [6e] and petroleum naphtha. [6f] However, the development of robust catalytic systems for efficient activation and further conversion of alkanes is severely hindered by the lack of mechanistic understanding.I nt his regard, solid-state NMR spectroscopy has been applied as ap owerful tool for monitoring the mechanistic events on heterogeneous catalysts. [7] In addition, GC-MS analysis on the distribution of either 13 Cor 2 Hlabels in the reaction products may offer the complementary information on many mechanistic details.T hrough solid-state magic-angle-spinning (MAS) NMR spectroscopy and GC-MS analysis,w ef ound herein, that upon addition of methanol, the C À Hb ond activation of propane was initiated by hydride transfer to surface methoxy species over zeolite H-ZSM-5 (Scheme 1). Initiated by hydride transfer, even at temperature as low as 449 K, the co-conversion of propane and methanol can be further achieved by secondary reactions,s uch as propene methylation (Scheme 2). This work not only details the longpursued evidence for hydride transfer over zeolite catalysts, but also offers insightful information on practical utilization of alkanes through the co-conversion strategy.To obtain unambiguous evidence for the initial hydride transfer, we chose 13 C-labeled methanol and nonlabeled propane (as the model compound of inert alkane) for ...

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Alkane Activation Initiated by Hydride Transfer: Co‐conversion of Propane and Methanol over H‐ZSM‐5 Zeolite

Liu

et al. 2015

Angew Chem Int Ed

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Co-conversion of alkane with another reactant over zeolite catalysts has emerged as a new approach to the long-standing challenge of alkane transformation. With the aid of solid-state NMR spectroscopy and GC-MS analysis, it was found that the co-conversion of propane and methanol can be readily initiated by hydride transfer at temperatures of ≥449 K over the acidic zeolite H-ZSM-5. The formation of (13)C-labeled methane and singly (13)C-labeled n-butanes in selective labeling experiments provided the first evidence for the initial hydride transfer from propane to surface methoxy intermediates. The results not only provide new insight into carbocation chemistry of solid acids, but also shed light on the low-temperature transformation of alkanes for industrial applications.

show abstract

Catalytic Compatibility of Methanol with Petroleum Naphtha in Mixed Feeds Used in the Thermal-Catalytic/Steam-Cracking (TCSC) Process for the Production of Propylene and Ethylene

Cited by 7 publications

References 30 publications

Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles

Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles

Alkane Activation Initiated by Hydride Transfer: Co‐conversion of Propane and Methanol over H‐ZSM‐5 Zeolite

Alkane Activation Initiated by Hydride Transfer: Co‐conversion of Propane and Methanol over H‐ZSM‐5 Zeolite

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