A combined experimental and modeling study of Microwave-assisted methane dehydroaromatization process

Bai, Xinwei; Muley, Pranjali D.; Musho, Terence; Abdelsayed, Victor; Robinson, Brandon; Caiola, Ashley; Shekhawat, Dushyant; Jiang, Changle; Hu, Jianli

doi:10.1016/j.cej.2021.134445

Title: A combined experimental and modeling study of Microwave-assisted methane dehydroaromatization process

Journal Article · 03 January 2022 · Chemical Engineering Journal

DOI: https://doi.org/10.1016/j.cej.2021.134445 · OSTI ID:1888743

Bai, Xinwei ^[1]; Muley, Pranjali D. ^[2]; Musho, Terence ^[1]; Abdelsayed, Victor ^[2]; Robinson, Brandon ^[1]; Caiola, Ashley ^[1]; Shekhawat, Dushyant ^[3]; Jiang, Changle ^[1]; Hu, Jianli ^[1]

West Virginia University, Morgantown, WV (United States)
National Energy Technology Lab. (NETL), Morgantown, WV (United States); National Energy Technology Lab. (NETL), Morgantown, WV (United States). Leidos Research Support Team
National Energy Technology Lab. (NETL), Morgantown, WV (United States)

We report the challenges in direct methane conversion to higher-value chemicals include rapid catalyst deactivation and comparatively low single-pass conversion. The most important step in direct methane conversion is the activation of strong C-H bonds. In this paper, we integrated microwave irradiation with heterogeneous catalysis to enable a higher methane conversion to C2 and aromatics at low temperature. The results showed that the methane conversion can reach 18% at 550 °C under microwave irradiation, while a temperature higher than 800 °C was required to achieve the same level of methane conversion in a traditional fixed-bed reactor. The microwave radiation may facilitate this heterogeneous catalysis process both thermally and non-thermally. Thermal effect, as known as “hot spots”, can be characterized experimentally. The results indicated the “hot spot” temperature can reach as high as 800 °C while the bulk temperature stayed at 550 °C. However, the non-thermal effect is difficult to characterize due to the limitations of existing in-situ instrumentations. Finite-element modeling can be a powerful engineering tool to simulate and understand complex physic fields. The simulation results show that between spherical catalyst particles the electric field on the catalyst bed was at a level of 10⁴ V/m and the non-uniform electric field distribution on the catalyst bed. Under this level of external electric field, methane activation on the catalyst surface was possible. These field distributions can explain the non-thermal effects of microwave-assisted catalytic chemical reactions, supported by the observation of benzene hydrogenolysis side reaction. With the thermal and non-thermal effects from microwave radiation, microwave-assisted heterogeneous catalytic process can be an attractive solution to activate stable feedstock molecules and can be applied to direct methane conversion process.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: 89243318CFE000003

OSTI ID:: 1888743

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Journal Issue: N/A Vol. 433; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (63)

Gas-Phase Hydrogenolysis of Benzene and Derivatives at Elevated Pressure; Methane Formation van Scheppingen, Wibo B.; Cieplik, Mariusz K.; Louw, Robert European Journal of Organic Chemistry, Vol. 2001, Issue 11 https://doi.org/10.1002/1099-0690(200106)2001:11<2101::AID-EJOC2101>3.0.CO;2-E	journal	June 2001
Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts Kumar, Anurag; Song, Kepeng; Liu, Lingmei Angewandte Chemie International Edition, Vol. 57, Issue 47 https://doi.org/10.1002/anie.201809433	journal	November 2018
Multilayered Two‐Dimensional V ₂ CT _x MXene for Methane Dehydroaromatization Thakur, Raj; Hoffman, Megan; VahidMohammadi, Armin ChemCatChem, Vol. 12, Issue 14 https://doi.org/10.1002/cctc.201902366	journal	March 2020
On the Energy Efficiency of Microwave-Assisted Organic Reactions Razzaq, Tahseen; Kappe, C. Oliver ChemSusChem, Vol. 1, Issue 1-2 https://doi.org/10.1002/cssc.200700036	journal	February 2008
Promotional Effect of Cr in Sulfated Zirconia‐Based Mo Catalyst for Methane Dehydroaromatization Abedin, Md Ashraful; Kanitkar, Swarom; Bhattar, Srikar Energy Technology, Vol. 8, Issue 8 https://doi.org/10.1002/ente.201900555	journal	August 2019
Investigation of the effect of microwave heated reactor on ethane dehydrogenation over KIT-6 supported catalysts Eslek Koyuncu, Dilsad Dolunay Reaction Kinetics, Mechanisms and Catalysis, Vol. 132, Issue 1 https://doi.org/10.1007/s11144-021-01928-7	journal	January 2021
Percolation exponents and threshold in two nearly ideal anisotropic continuum systems Wu, Junjie; McLachlan, D. S. Physica A: Statistical Mechanics and its Applications, Vol. 241, Issue 1-2 https://doi.org/10.1016/S0378-4371(97)00108-8	journal	July 1997
Vapor-phase transport (VPT) modification of ZSM-5/SiC foam catalyst using TPAOH vapor to improve the methanol-to-propylene (MTP) reaction Jiao, Yilai; Fan, Xiaolei; Perdjon, Michal Applied Catalysis A: General, Vol. 545 https://doi.org/10.1016/j.apcata.2017.07.036	journal	September 2017
Hollow ZSM-5 zeolite grass ball catalyst in methane dehydroaromatization: One-step synthesis and the exceptional catalytic performance Wang, Kai; Huang, Xin; Li, Debao Applied Catalysis A: General, Vol. 556 https://doi.org/10.1016/j.apcata.2018.02.030	journal	April 2018
Methane dehydroaromatization over molybdenum supported on sulfated zirconia catalysts Kanitkar, Swarom; Abedin, Md Ashraful; Bhattar, Srikar Applied Catalysis A: General, Vol. 575 https://doi.org/10.1016/j.apcata.2019.01.013	journal	April 2019
Microwave-assisted ammonia decomposition reaction over iron incorporated mesoporous carbon catalysts Varisli, Dilek; Korkusuz, Cansu; Dogu, Timur Applied Catalysis B: Environmental, Vol. 201 https://doi.org/10.1016/j.apcatb.2016.08.032	journal	February 2017
Hydrogen production over molybdenum loaded mesoporous carbon catalysts in microwave heated reactor system Guler, Melih; Dogu, Timur; Varisli, Dilek Applied Catalysis B: Environmental, Vol. 219 https://doi.org/10.1016/j.apcatb.2017.07.043	journal	December 2017
Ambient pressure synthesis of ammonia using a microwave reactor Wildfire, Christina; Abdelsayed, Victor; Shekhawat, Dushyant Catalysis Communications, Vol. 115 https://doi.org/10.1016/j.catcom.2018.07.010	journal	September 2018
Sulfated hafnia as a support for Mo oxide: A novel catalyst for methane dehydroaromatization Abedin, Md Ashraful; Kanitkar, Swarom; Bhattar, Srikar Catalysis Today, Vol. 343 https://doi.org/10.1016/j.cattod.2019.02.021	journal	March 2020
Catalytic direct conversion of ethane to value-added chemicals under microwave irradiation Robinson, Brandon; Caiola, Ashley; Bai, Xinwei Catalysis Today, Vol. 356 https://doi.org/10.1016/j.cattod.2020.03.001	journal	October 2020
Microwave-assisted ammonia synthesis over Ru/MgO catalysts at ambient pressure Wildfire, Christina; Abdelsayed, Victor; Shekhawat, Dushyant Catalysis Today, Vol. 365 https://doi.org/10.1016/j.cattod.2020.06.013	journal	April 2021
Methane-to-aromatics in a gas recycle methane reactor/hydrogen membrane separator Sakbodin, Mann; Schulman, Emily; Pan, Ying Catalysis Today, Vol. 365 https://doi.org/10.1016/j.cattod.2020.06.028	journal	April 2021
From bench scale to pilot plant: A 150x scaled-up configuration of a microwave-driven structured reactor for methane dehydroaromatization Julian, I.; Pedersen, C. M.; Jensen, A. B. Catalysis Today, Vol. 383 https://doi.org/10.1016/j.cattod.2021.04.013	journal	January 2022
Production of carbon nanotubes from methaneUse of Co-Zn-Al catalysts prepared by microwave-assisted synthesis Benito, P.; Herrero, M.; Labajos, F. M. Chemical Engineering Journal, Vol. 149, Issue 1-3 https://doi.org/10.1016/j.cej.2009.02.022	journal	July 2009
Non-oxidative methane conversion in microwave-assisted structured reactors Julian, Ignacio; Ramirez, Heidy; Hueso, Jose L. Chemical Engineering Journal, Vol. 377 https://doi.org/10.1016/j.cej.2018.08.150	journal	December 2019
Microwave-driven heterogeneous catalysis for activation of dinitrogen to ammonia under atmospheric pressure Hu, Jianli; Wildfire, Christina; Stiegman, Albert E. Chemical Engineering Journal, Vol. 397 https://doi.org/10.1016/j.cej.2020.125388	journal	October 2020
An integrated methane dehydroaromatization and chemical looping process Brady, Casper; Debruyne, Quinten; Majumder, Ankita Chemical Engineering Journal, Vol. 406 https://doi.org/10.1016/j.cej.2020.127168	journal	February 2021
Microwave-assisted conversion of methane over H-(Fe)-ZSM-5: Evidence for formation of hot metal sites Deng, Yifan; Bai, Xinwei; Abdelsayed, Victor Chemical Engineering Journal, Vol. 420 https://doi.org/10.1016/j.cej.2021.129670	journal	September 2021
Dynamic data reconciliation, parameter estimation, and multi-scale, multi-physics modeling of the microwave-assisted methane dehydroaromatization process Mevawala, Chirag; Bai, Xinwei; Bhattacharyya, Debangsu Chemical Engineering Science, Vol. 239 https://doi.org/10.1016/j.ces.2021.116624	journal	August 2021
Innovative non–oxidative methane dehydroaromatization via solar membrane reactor Wang, Hongsheng; Wang, Bingzheng; Qi, Xingyu Energy, Vol. 216 https://doi.org/10.1016/j.energy.2020.119265	journal	February 2021
Microwave catalytic reactor for upgrading stranded shale gas to aromatics Bai, Xinwei; Robinson, Brandon; Killmer, Casey Fuel, Vol. 243 https://doi.org/10.1016/j.fuel.2019.01.147	journal	May 2019
Promotional effect of Au on Fe/HZSM-5 catalyst for methane dehydroaromatization Sim, Jaeik Paul; Lee, Byung Jin; Han, Geun-Ho Fuel, Vol. 274 https://doi.org/10.1016/j.fuel.2020.117852	journal	August 2020
Microwave-assisted catalytic decomposition of methane over activated carbon for CO2CO2-free hydrogen production Dominguez, A.; Fidalgo, B.; Fernandez, Y. International Journal of Hydrogen Energy, Vol. 32, Issue 18 https://doi.org/10.1016/j.ijhydene.2007.07.041	journal	December 2007
Microwave-assisted methane decomposition over pyrolysis residue of sewage sludge for hydrogen production Deng, Wenyi; Su, Yaxin; Liu, Shugang International Journal of Hydrogen Energy, Vol. 39, Issue 17 https://doi.org/10.1016/j.ijhydene.2014.04.033	journal	June 2014
Numerical analysis of microwave assisted thermocatalytic decomposition of methane Gadkari, Siddharth; Fidalgo, Beatriz; Gu, Sai International Journal of Hydrogen Energy, Vol. 42, Issue 7 https://doi.org/10.1016/j.ijhydene.2016.09.126	journal	February 2017
Ammonia decomposition reaction to produce COx-free hydrogen using carbon supported cobalt catalysts in microwave heated reactor system Can Seyfeli, Rukan; Varisli, Dilek International Journal of Hydrogen Energy, Vol. 45, Issue 60 https://doi.org/10.1016/j.ijhydene.2020.01.124	journal	December 2020
Comparison of microwave and conventionally heated reactor performances in catalytic dehydrogenation of ethane Eryildirim, Busra; Arbag, Huseyin; Oktar, Nuray International Journal of Hydrogen Energy, Vol. 46, Issue 7 https://doi.org/10.1016/j.ijhydene.2020.11.067	journal	January 2021
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 Journal of Catalysis, Vol. 372 https://doi.org/10.1016/j.jcat.2019.03.016	journal	April 2019
Probing cobalt localization on HZSM-5 for efficient methane dehydroaromatization catalysts Xu, Yuebing; Chen, Mengyao; Wang, Ting Journal of Catalysis, Vol. 387 https://doi.org/10.1016/j.jcat.2020.04.021	journal	July 2020
Low-temperature oxidative coupling of methane in an electric field using carbon dioxide over Ca-doped LaAlO3 perovskite oxide catalysts Yabe, Tomohiro; Kamite, Yukiko; Sugiura, Kei Journal of CO2 Utilization, Vol. 20 https://doi.org/10.1016/j.jcou.2017.05.001	journal	July 2017
Study of Cu2O particle morphology on microwave field enhancement Musho, T. D.; Wildfire, C.; Houlihan, N. M. Materials Chemistry and Physics, Vol. 216 https://doi.org/10.1016/j.matchemphys.2018.05.059	journal	September 2018
Performance of Co-Fe@Alumina catalysts in comparison to monometallic Co@Alumina and Fe@Alumina catalysts for microwave assisted COx-free hydrogen production Akca, Merve; Varisli, Dilek Molecular Catalysis, Vol. 485 https://doi.org/10.1016/j.mcat.2020.110823	journal	April 2020
Methane dehydroaromatization over Fe-M/ZSM-5 catalysts (M= Zr, Nb, Mo) Denardin, Felipe G.; Perez-Lopez, Oscar W. Microporous and Mesoporous Materials, Vol. 295 https://doi.org/10.1016/j.micromeso.2019.109961	journal	March 2020
Stability of Fe- and Zn-Promoted Mo/ZSM-5 Catalysts for Ethane Dehydroaromatization in Cyclic Operation Mode Robinson, Brandon; Bai, Xinwei; Samanta, Anupam Energy & Fuels, Vol. 32, Issue 7 https://doi.org/10.1021/acs.energyfuels.8b01516	journal	June 2018
Scaleup of a Single-Mode Microwave Reactor Goyal, Himanshu; Mehdad, Ali; Lobo, Raul F. Industrial & Engineering Chemistry Research, Vol. 59, Issue 6 https://doi.org/10.1021/acs.iecr.9b04491	journal	October 2019
Numerical Study on the Partitioning of the Molecular Polarizability into Fluctuating Charge and Induced Atomic Dipole Contributions Mei, Ye; Simmonett, Andrew C.; Pickard, Frank C. The Journal of Physical Chemistry A, Vol. 119, Issue 22 https://doi.org/10.1021/acs.jpca.5b03159	journal	May 2015
Intrinsic Structural, Electrical, Thermal, and Mechanical Properties of the Promising Conductor Mo ₂ C MXene Zha, Xian-Hu; Yin, Jingshuo; Zhou, Yuhong The Journal of Physical Chemistry C, Vol. 120, Issue 28 https://doi.org/10.1021/acs.jpcc.6b04192	journal	July 2016
Enhanced Methane Dehydroaromatization via Coupling with Chemical Looping Brady, Casper; Murphy, Brian; Xu, Bingjun ACS Catalysis, Vol. 7, Issue 6 https://doi.org/10.1021/acscatal.7b00879	journal	May 2017
Effect of External Electric Field on Methane Conversion on IrO ₂ (110) Surface: A Density Functional Theory Study Yeh, Chen-Hao; Pham, Thong Minh Le; Nachimuthu, Santhanamoorthi ACS Catalysis, Vol. 9, Issue 9 https://doi.org/10.1021/acscatal.9b01910	journal	July 2019
Microwave Hydrothermal Synthesis of Ni-based Metal–Organic Frameworks and Their Derived Yolk–Shell NiO for Li-Ion Storage and Supported Ammonia Borane for Hydrogen Desorption Kong, Shaofeng; Dai, Ruoling; Li, Hao ACS Sustainable Chemistry & Engineering, Vol. 3, Issue 8 https://doi.org/10.1021/acssuschemeng.5b00556	journal	July 2015
Microwave-Assisted Organic Synthesis and Transformations using Benign Reaction Media Polshettiwar, Vivek; Varma, Rajender S. Accounts of Chemical Research, Vol. 41, Issue 5 https://doi.org/10.1021/ar700238s	journal	May 2008
Adsorption and Catalytic Activation of O₂ Molecule on the Surface of Au-Doped Graphene under an External Electric Field Zhang, Teng; Xue, Qingzhong; Shan, Meixia The Journal of Physical Chemistry C, Vol. 116, Issue 37 https://doi.org/10.1021/jp3073359	journal	September 2012
Enhancement of Fixed-bed Flow Reactions under Microwave Irradiation by Local Heating at the Vicinal Contact Points of Catalyst Particles Haneishi, Naoto; Tsubaki, Shuntaro; Abe, Eriko Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-018-35988-y	journal	January 2019
Catalytic aromatization of methane Spivey, James J.; Hutchings, Graham Chem. Soc. Rev., Vol. 43, Issue 3 https://doi.org/10.1039/C3CS60259A	journal	January 2014
The physical chemistry and materials science behind sinter-resistant catalysts Dai, Yunqian; Lu, Ping; Cao, Zhenming Chemical Society Reviews, Vol. 47, Issue 12 https://doi.org/10.1039/C7CS00650K	journal	January 2018
A hollow Mo/HZSM-5 zeolite capsule catalyst: preparation and enhanced catalytic properties in methane dehydroaromatization Zhu, Pengfei; Yang, Guohui; Sun, Jian Journal of Materials Chemistry A, Vol. 5, Issue 18 https://doi.org/10.1039/C7TA02345F	journal	January 2017
A novel route to improve methane aromatization by using a simple composite catalyst Zhang, Yan; Jiang, Heqing Chemical Communications, Vol. 54, Issue 73 https://doi.org/10.1039/C8CC05059G	journal	January 2018
A fast method for determination of surface area of zeolite-based catalysts and zeolites using near infrared emission spectroscopy Rebouças, Jicarla Portela; Rodrigues Rohwedder, Jarbas José; Pasquini, Celio Analytical Methods, Vol. 11, Issue 21 https://doi.org/10.1039/C9AY00521H	journal	January 2019
Boric acid treated HZSM-5 for improved catalyst activity in non-oxidative methane dehydroaromatization Balyan, Sonit; Haider, M. Ali; Khan, Tuhin S. Catalysis Science & Technology, Vol. 10, Issue 12 https://doi.org/10.1039/D0CY00286K	journal	January 2020
A critical assessment of the greenness and energy efficiency of microwave-assisted organic synthesis Moseley, Jonathan D.; Kappe, C. Oliver Green Chemistry, Vol. 13, Issue 4 https://doi.org/10.1039/c0gc00823k	journal	January 2011
Thermal Properties and Lattice Dynamics of Polycrystalline MFI Zeolite Films Greenstein, A. M.; Graham, S.; Hudiono, Y. C. Nanoscale and Microscale Thermophysical Engineering, Vol. 10, Issue 4 https://doi.org/10.1080/15567260601009171	journal	December 2006
Optical and Electrical Properties of SiC Films Prepared in a Microwave Discharge Weinreich, O. A.; Ribner, A. Journal of The Electrochemical Society, Vol. 115, Issue 10 https://doi.org/10.1149/1.2410892	journal	January 1968
Microwaves in Nonoxidative Conversion of Natural Gas to Value-Added Products Bai, Xinwei; Robinson, Brandon; Shekhawat, Dushyant Direct Natural Gas Conversion to Value-Added Chemicals https://doi.org/10.1201/9780429022852-2	book	September 2020
Catalytic Oxidative Coupling of Methane Assisted by Electric Power over a Semiconductor Catalyst Tanaka, Keisuke; Sekine, Yasushi; Oshima, Kazumasa Chemistry Letters, Vol. 41, Issue 4 https://doi.org/10.1246/cl.2012.351	journal	April 2012
Mesoporous KIT-6 supported Cr and Co-based catalysts for microwave-assisted non-oxidative ethane dehydrogenation Eslek Koyuncu, Dilsad Dolunay International Journal of Chemical Reactor Engineering, Vol. 19, Issue 2 https://doi.org/10.1515/ijcre-2020-0203	journal	February 2021
Microwave-Assisted Coprecipitation Synthesis of LaCoO3 Nanoparticles and Their Catalytic Activity for Syngas Production by Partial Oxidation of Methane Alvarez-Galvan, Consuelo; Trunschke, Annette; Falcon, Horacio Frontiers in Energy Research, Vol. 6 https://doi.org/10.3389/fenrg.2018.00018	journal	April 2018
Overcoming Stability Problems in Microwave-Assisted Heterogeneous Catalytic Processes Affected by Catalyst Coking Julian, Ignacio; Pedersen, Christoffer M.; Achkasov, Kostiantyn Catalysts, Vol. 9, Issue 10 https://doi.org/10.3390/catal9100867	journal	October 2019
Review on Microwave-Matter Interaction Fundamentals and Efficient Microwave-Associated Heating Strategies Sun, Jing; Wang, Wenlong; Yue, Qinyan Materials, Vol. 9, Issue 4 https://doi.org/10.3390/ma9040231	journal	March 2016