Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts

Razdan, Neil K.; Kumar, Anurag; Bhan, Aditya

doi:10.1016/j.jcat.2019.03.016

Title: Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoC_x/H-ZSM-5 catalysts

Abstract

Addition of Zr metal absorbent to MoC_x/H-ZSM-5 in the form of staged-bed, stratified-bed, and interpellet physical mixtures effectively scavenges H₂ from catalyst proximity, enhancing maximum single-pass benzene + naphthalene yield during methane dehydroaromatization (DHA) reactions to 14-16% compared to 8% in formulations without zirconium. The coupling of spatially-distinct catalytic and absorptive functions is achieved by dispersive/diffusive transport which conveys H₂ to staged Zr both co- and counter-current to bulk advection, thereby suppressing axial H₂ partial pressure profiles along the catalyst bed and enhancing net aromatization rates. We evince hitherto unreported significance of dispersive hydrogen transport during methane DHA by measurement of Péclet number, Pe = 1.32, in H₂ tracer studies with step-change or impulse input to inert catalyst proxies. Kinetic limits to methane pyrolysis are quantified by Damköhler number, Da, for synthesis of benzene, Da_B = 0.15, and naphthalene, Da_N = 0.03, determined from kinetic studies which rigorously account for reversibility of DHA reactions. Here, detailed reaction-transport models synthesize interplay of kinetic, diffusive, and convective length-scales captured by Péclet and Damköhler number to predict influence of catalyst-absorbent proximity and process flow-conditions on aromatization rates. Systematic control of catalyst bed-length, L, or linear flow velocity, u, predictably alters Pe and Damore »« less

Authors:

Razdan, Neil K. ^[1]; Kumar, Anurag ^[1];

^[1]

University of Minnesota, Twin Cities, Minneapolis, MN (United States)

Publication Date:: Wed Mar 27 00:00:00 EDT 2019

Research Org.:: Univ. of Minnesota, Minneapolis, MN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

OSTI Identifier:: 1658226

Grant/Contract Number:: SC0019028

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Catalysis

Additional Journal Information:: Journal Volume: 372; Related Information: https://doi.org/10.1016/j.jcat.2019.03.016; Journal ID: ISSN 0021-9517

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 03 NATURAL GAS; Methane conversion; Non-oxidative; Polyfunctional catalysis; Reversibility; Molybdenum carbide

Citation Formats


                    Razdan, Neil K., Kumar, Anurag, and Bhan, Aditya. Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts.  United States: N. p., 2019. 
Web.  doi:10.1016/j.jcat.2019.03.016.

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                    Razdan, Neil K., Kumar, Anurag, & Bhan, Aditya. Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts.  United States.  https://doi.org/10.1016/j.jcat.2019.03.016

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                    Razdan, Neil K., Kumar, Anurag, and Bhan, Aditya. Wed .  
"Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts".  United States.  https://doi.org/10.1016/j.jcat.2019.03.016.  https://www.osti.gov/servlets/purl/1658226.

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@article{osti_1658226,

  title        = {Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts},

  author       = {Razdan, Neil K. and Kumar, Anurag and Bhan, Aditya},

  abstractNote = {Addition of Zr metal absorbent to MoCx/H-ZSM-5 in the form of staged-bed, stratified-bed, and interpellet physical mixtures effectively scavenges H2 from catalyst proximity, enhancing maximum single-pass benzene + naphthalene yield during methane dehydroaromatization (DHA) reactions to 14-16% compared to 8% in formulations without zirconium. The coupling of spatially-distinct catalytic and absorptive functions is achieved by dispersive/diffusive transport which conveys H2 to staged Zr both co- and counter-current to bulk advection, thereby suppressing axial H2 partial pressure profiles along the catalyst bed and enhancing net aromatization rates. We evince hitherto unreported significance of dispersive hydrogen transport during methane DHA by measurement of Péclet number, Pe = 1.32, in H2 tracer studies with step-change or impulse input to inert catalyst proxies. Kinetic limits to methane pyrolysis are quantified by Damköhler number, Da, for synthesis of benzene, DaB = 0.15, and naphthalene, DaN = 0.03, determined from kinetic studies which rigorously account for reversibility of DHA reactions. Here, detailed reaction-transport models synthesize interplay of kinetic, diffusive, and convective length-scales captured by Péclet and Damköhler number to predict influence of catalyst-absorbent proximity and process flow-conditions on aromatization rates. Systematic control of catalyst bed-length, L, or linear flow velocity, u, predictably alters Pe and Da to effect improvements in methane conversion with and without Zr metal, corroborating results from simulation of the reaction-transport model.},

  doi          = {10.1016/j.jcat.2019.03.016},

  journal      = {Journal of Catalysis},

  number       = ,

  volume       = 372,

  place        = {United States},

  year         = {Wed Mar 27 00:00:00 EDT 2019},

  month        = {Wed Mar 27 00:00:00 EDT 2019}

}

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Works referencing / citing this record:

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis
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Kang, Jincan; He, Shun; Zhou, Wei
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Similar Records

Title: Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts

Abstract

Citation Formats

Catalytic conversion of methane to more useful chemicals and fuels: a challenge for the 21st century journal, December 2000

Understanding and exploiting C–H bond activation journal, May 2002

Coke accumulation and deactivation behavior of microzeolite-based Mo/HZSM-5 in the non-oxidative methane aromatization under cyclic CH 4 -H 2 feed switch mode journal, January 2017

On the deactivation of Mo/HZSM-5 in the methane dehydroaromatization reaction journal, October 2015

Aromatization of Methane over Supported and Unsupported Mo-Based Catalysts journal, January 1997

Direct Conversion of Methane to Value-Added Chemicals over Heterogeneous Catalysts: Challenges and Prospects journal, March 2017

Dehydrogenation and aromatization of methane under non-oxidizing conditions journal, January 1993

The influence of molybdenum loading on activity of ZSM-5 zeolite in dehydroaromatization of methane journal, August 2015

Methane dehydroaromatization over Mo/HZSM-5 catalysts: The reactivity of MoCx species formed from MoOx associated and non-associated with Brönsted acid sites journal, October 2005

Characterization of a Mo/ZSM-5 Catalyst for the Conversion of Methane to Benzene journal, July 1997

Conversion of Methane to Benzene over Transition Metal Ion ZSM-5 Zeolites journal, April 1998

Stable Mo/HZSM-5 methane dehydroaromatization catalysts optimized for high-temperature calcination-regeneration journal, February 2017

CH4 dehydroaromatization on Mo/H–ZSM-5: 1. Effects of co-processing H2 and CH3COOH journal, October 2013

Raman and X-Ray Absorption Studies of Mo Species in Mo/H-ZSM5 Catalysts for Non-Oxidative CH4 Reactions journal, April 2000

Stability, structure, and oxidation state of Mo/H-ZSM-5 catalysts during reactions of CH4 and CH4–CO2 mixtures journal, February 2005

Isothermal activation of Mo 2 O 5 2+ –ZSM-5 precursors during methane reactions: effects of reaction products on structural evolution and catalytic properties journal, January 2005

Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts journal, November 2018

Dehydro-oligomerization of Methane to Ethylene and Aromatics over Molybdenum/HZSM-5 Catalyst journal, November 1995

Structure and Density of Mo and Acid Sites in Mo-Exchanged H-ZSM5 Catalysts for Nonoxidative Methane Conversion journal, July 1999

Reaction-transport simulations of non-oxidative methane conversion with continuous hydrogen removal — homogeneous–heterogeneous reaction pathways journal, March 2001

A Relation Between Permeability and size Distribution of Pores journal, March 1958

The Diffusion of Gases Through Porous Media journal, March 1959

Measurement of mutual diffusion coefficients of gases by the Taylor method: Measurements on H2-Air,H2-N2, and H2-O2 systems journal, April 2002

Diffusion by Continuous Movements journal, January 1922

Voidage profiles in packed beds of spheres journal, January 1986

The kinetics of hydrogen desorption from and adsorption on zirconium hydride journal, February 2010

Continuous flow systems journal, February 1953

Co-processing CH4 and oxygenates on Mo/H-ZSM-5: 2. CH4–CO2 and CH4–HCOOH mixtures journal, January 2013

Methane aromatisation based upon elementary steps: Kinetic and catalyst descriptors journal, December 2012

The Effects of Silanation of External Acid Sites on the Structure and Catalytic Behavior of Mo/H–ZSM5 journal, February 2002

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis journal, February 2020

One-pass selective conversion of syngas to para -xylene journal, January 2017

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis journal, February 2020

Title: Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoC_x/H-ZSM-5 catalysts

Catalytic conversion of methane to more useful chemicals and fuels: a challenge for the 21st century
journal, December 2000

Understanding and exploiting C–H bond activation
journal, May 2002

Coke accumulation and deactivation behavior of microzeolite-based Mo/HZSM-5 in the non-oxidative methane aromatization under cyclic CH 4 -H 2 feed switch mode
journal, January 2017

On the deactivation of Mo/HZSM-5 in the methane dehydroaromatization reaction
journal, October 2015

Aromatization of Methane over Supported and Unsupported Mo-Based Catalysts
journal, January 1997

Direct Conversion of Methane to Value-Added Chemicals over Heterogeneous Catalysts: Challenges and Prospects
journal, March 2017

Dehydrogenation and aromatization of methane under non-oxidizing conditions
journal, January 1993

The influence of molybdenum loading on activity of ZSM-5 zeolite in dehydroaromatization of methane
journal, August 2015

Methane dehydroaromatization over Mo/HZSM-5 catalysts: The reactivity of MoCx species formed from MoOx associated and non-associated with Brönsted acid sites
journal, October 2005

Characterization of a Mo/ZSM-5 Catalyst for the Conversion of Methane to Benzene
journal, July 1997

Conversion of Methane to Benzene over Transition Metal Ion ZSM-5 Zeolites
journal, April 1998

Stable Mo/HZSM-5 methane dehydroaromatization catalysts optimized for high-temperature calcination-regeneration
journal, February 2017

CH4 dehydroaromatization on Mo/H–ZSM-5: 1. Effects of co-processing H2 and CH3COOH
journal, October 2013

Raman and X-Ray Absorption Studies of Mo Species in Mo/H-ZSM5 Catalysts for Non-Oxidative CH4 Reactions
journal, April 2000

Stability, structure, and oxidation state of Mo/H-ZSM-5 catalysts during reactions of CH4 and CH4–CO2 mixtures
journal, February 2005

Isothermal activation of Mo ₂ O ₅ ²⁺ –ZSM-5 precursors during methane reactions: effects of reaction products on structural evolution and catalytic properties
journal, January 2005

Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts
journal, November 2018

Dehydro-oligomerization of Methane to Ethylene and Aromatics over Molybdenum/HZSM-5 Catalyst
journal, November 1995

Structure and Density of Mo and Acid Sites in Mo-Exchanged H-ZSM5 Catalysts for Nonoxidative Methane Conversion
journal, July 1999

Reaction-transport simulations of non-oxidative methane conversion with continuous hydrogen removal — homogeneous–heterogeneous reaction pathways
journal, March 2001

A Relation Between Permeability and size Distribution of Pores
journal, March 1958

The Diffusion of Gases Through Porous Media
journal, March 1959

Measurement of mutual diffusion coefficients of gases by the Taylor method: Measurements on H2-Air,H2-N2, and H2-O2 systems
journal, April 2002

Diffusion by Continuous Movements
journal, January 1922

Voidage profiles in packed beds of spheres
journal, January 1986

The kinetics of hydrogen desorption from and adsorption on zirconium hydride
journal, February 2010

Continuous flow systems
journal, February 1953

Co-processing CH4 and oxygenates on Mo/H-ZSM-5: 2. CH4–CO2 and CH4–HCOOH mixtures
journal, January 2013

Methane aromatisation based upon elementary steps: Kinetic and catalyst descriptors
journal, December 2012

The Effects of Silanation of External Acid Sites on the Structure and Catalytic Behavior of Mo/H–ZSM5
journal, February 2002

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis
journal, February 2020

One-pass selective conversion of syngas to para -xylene
journal, January 2017

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis
journal, February 2020