Microwave-Assisted dry reforming of toluene as a model tar compound using low-cost iron catalyst for syngas clean-up

Bai, Xinwei; Abedin, Ashraf; Linge Gowda, Anitha Shankara; Abdelsayed, Victor; Muley, Pranjali

doi:10.1016/j.fuel.2024.131843

Microwave-Assisted dry reforming of toluene as a model tar compound using low-cost iron catalyst for syngas clean-up

Journal Article · Thu May 09 00:00:00 EDT 2024 · Fuel

DOI:https://doi.org/10.1016/j.fuel.2024.131843· OSTI ID:2432324

Bai, Xinwei ^[1]; Abedin, Ashraf ^[1]; Linge Gowda, Anitha Shankara ^[1]; Abdelsayed, Victor ^[1]; Muley, Pranjali ^[1]

National Energy Technology Lab. (NETL), Morgantown, WV (United States)

Gasification of waste feedstock such as biomass, waste plastics suffers from high tar yields during hydrogen-rich syngas production. The presence of tars result in lower quality syngas, lower syngas yields, reactor blockage, reactor down time, and costly maintenance. Therefore, removal of tar from syngas during gasification is essential. Catalytic reforming of tars via in-situ syngas cleanup is an effective way of mitigating tars. This work explores the possibility of microwave-assisted catalytic dry reforming of tars for syngas production. Further, due to its chemical complexity, toluene, which is one of the main tar constituents, could be used as a model tar compound. Toluene dry reforming was studied using the Fe/Al₂O₃ catalyst under CO₂ under the temperature range of 400–700 °C. The toluene reforming reaction was conducted using microwave and conventional thermal reactors. Under microwave irradiation, CO₂ and toluene conversions are boosted to 80% at 500 °C. Hydrogen and carbon monoxide yields were approximately five times and ten times higher in the microwave reactor at 500 °C, respectively, compared to the productions obtained in the conventional fixed-bed reactor at 700 °C. Filamentous carbon was also produced as a valuable side product to improve the economy of this process and such value-added carbon was only observed in the microwave reactor. Three reaction pathways were observed during microwave reaction: the toluene decomposition produces an initial hydrogen and carbon deposit on the catalyst; the formation of methane and benzene suggests toluene hydrodemethylation as a secondary reaction; and toluene hydrogenolysis forms light alkanes such as methane, and through reforming reaction under CO₂ to syngas.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Fossil Energy and Carbon Management (FECM)

OSTI ID:: 2432324

Journal Information:: Fuel, Journal Name: Fuel Vol. 370; ISSN 0016-2361

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (52)

Temperature Programmed Oxidation Coupled with In Situ Techniques Reveal the Nature and Location of Coke Deposited on a Ni/La₂ O₃ -αAl₂ O₃ Catalyst in the Steam Reforming of Bio-oil Ochoa, Aitor; Valle, Beatriz; Resasco, Daniel E. ChemCatChem, Vol. 10, Issue 10 https://doi.org/10.1002/cctc.201701942	journal	March 2018
Structure–Property Correlation in Fe-Al2O3 In Situ Nanocomposite Synthesized by High-Energy Ball Milling and Spark Plasma Sintering Udhayabanu, V.; Ravi, K. R.; Murty, B. S. Metallurgical and Materials Transactions A, Vol. 47, Issue 10 https://doi.org/10.1007/s11661-016-3627-z	journal	July 2016
Catalytic tar conversion and the prospective use of iron-based catalyst in the future development of biomass gasification: a review Ramadhani, Bakari; Kivevele, Thomas; Kihedu, Joseph H. Biomass Conversion and Biorefinery, Vol. 12, Issue 4 https://doi.org/10.1007/s13399-020-00814-x	journal	June 2020
Reaction mechanisms for toluene pyrolysis Colket, M. B.; Seery, D. J. Symposium (International) on Combustion, Vol. 25, Issue 1 https://doi.org/10.1016/S0082-0784(06)80723-X	journal	January 1994
Effect of iron oxide on isobutane dehydrogenation over Pt/Fe2O3-Al2O3 catalyst Kobayashi, Shingo; Kaneko, Shinji; Ohshima, Masa-aki Applied Catalysis A: General, Vol. 417-418 https://doi.org/10.1016/j.apcata.2012.01.007	journal	February 2012
Perovskite LaxM1−xNi0.8Fe0.2O3 catalyst for steam reforming of toluene: Crucial role of alkaline earth metal at low steam condition Oemar, U.; Ang, M. L.; Hee, W. F. Applied Catalysis B: Environmental, Vol. 148-149 https://doi.org/10.1016/j.apcatb.2013.10.001	journal	April 2014
Investigation on model compound of biomass gasification tar cracking in microwave furnace: Comparative research Chen, Guanyi; Li, Jian; Cheng, Zhanjun Applied Energy, Vol. 217 https://doi.org/10.1016/j.apenergy.2018.02.028	journal	May 2018
X-ray diffraction patterns of graphite and turbostratic carbon Li, Z. Q.; Lu, C. J.; Xia, Z. P. Carbon, Vol. 45, Issue 8 https://doi.org/10.1016/j.carbon.2007.03.038	journal	July 2007
Steam reforming of model gasification tars compounds on nickel based ceria-zirconia catalysts Łamacz, Agata; Krztoń, Andrzej; Djéga-Mariadassou, Gérald Catalysis Today, Vol. 176, Issue 1 https://doi.org/10.1016/j.cattod.2010.11.067	journal	November 2011
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
Preparation and investigation of the structural properties of α-Al2O3 nanoparticles using the sol-gel method Mohammed, Adnan A.; Khodair, Ziad T.; Khadom, Anees A. Chemical Data Collections, Vol. 29 https://doi.org/10.1016/j.cdc.2020.100531	journal	October 2020
Microwave-induced cracking and CO 2 reforming of toluene on biomass derived char Li, Longzhi; Song, Zhanlong; Zhao, Xiqiang Chemical Engineering Journal, Vol. 284 https://doi.org/10.1016/j.cej.2015.09.040	journal	January 2016
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
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
Few-layer graphene prepared via microwave irradiation of black sesame for supercapacitor applications Xu, Xinghe; Sun, Shichang; Luo, Juan Chemical Engineering Journal, Vol. 425 https://doi.org/10.1016/j.cej.2021.130664	journal	December 2021
A review of microwave-assisted process intensified multiphase reactors Goyal, Himanshu; Chen, Tai-Ying; Chen, Weiqi Chemical Engineering Journal, Vol. 430 https://doi.org/10.1016/j.cej.2021.133183	journal	February 2022
A combined experimental and modeling study of Microwave-assisted methane dehydroaromatization process Bai, Xinwei; Muley, Pranjali D.; Musho, Terence Chemical Engineering Journal, Vol. 433 https://doi.org/10.1016/j.cej.2021.134445	journal	April 2022
Design of continuous-flow microwave reactor based on a leaky waveguide Xu, Chong; Lan, Junqin; Ye, Jinghua Chemical Engineering Journal, Vol. 452 https://doi.org/10.1016/j.cej.2022.139690	journal	January 2023
Study of steam reforming of toluene used as model compound of tar produced by biomass gasification Swierczynski, Dariusz; Courson, Claire; Kiennemann, Alain Chemical Engineering and Processing: Process Intensification, Vol. 47, Issue 3 https://doi.org/10.1016/j.cep.2007.01.012	journal	March 2008
Microwave-assisted co-gasification of mixed plastics and corn stover: A synergistic approach to produce clean hydrogen Abedin, Ashraf; Bai, Xinwei; Smith, Mark Energy Conversion and Management, Vol. 280 https://doi.org/10.1016/j.enconman.2023.116774	journal	March 2023
Plasma enhanced catalytic reforming of biomass tar model compound to syngas Tao, Kai; Ohta, Naoko; Liu, Guiqing Fuel, Vol. 104 https://doi.org/10.1016/j.fuel.2010.05.044	journal	February 2013
Catalytic reforming of tar during gasification. Part I. Steam reforming of biomass tar using ilmenite as a catalyst Min, Zhenhua; Asadullah, Mohammad; Yimsiri, Piyachat Fuel, Vol. 90, Issue 5 https://doi.org/10.1016/j.fuel.2010.12.039	journal	May 2011
Catalytic performance of manganese-promoted nickel catalysts for the steam reforming of tar from biomass pyrolysis to synthesis gas Koike, Mitsuru; Ishikawa, Chiaki; Li, Dalin Fuel, Vol. 103 https://doi.org/10.1016/j.fuel.2011.04.009	journal	January 2013
Steam reforming of naphthalene/benzene with various types of Pt- and Ni-based catalysts for hydrogen production Furusawa, Takeshi; Saito, Katsuhiko; Kori, Yoshihiko Fuel, Vol. 103 https://doi.org/10.1016/j.fuel.2011.09.026	journal	January 2013
Microwave-assisted pyrolysis of Mississippi coal: A comparative study with conventional pyrolysis Abdelsayed, Victor; Shekhawat, Dushyant; Smith, Mark W. Fuel, Vol. 217 https://doi.org/10.1016/j.fuel.2017.12.099	journal	April 2018
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
Iron-based catalyst (Fe2-xNixTiO5) for tar decomposition in biomass gasification Ruivo, L. C. M.; Pio, D. T.; Yaremchenko, A. A. Fuel, Vol. 300 https://doi.org/10.1016/j.fuel.2021.120859	journal	September 2021
Development of new nickel based catalyst for biomass tar steam reforming producing H2-rich syngas Li, Chunshan; Hirabayashi, Daisuke; Suzuki, Kenzi Fuel Processing Technology, Vol. 90, Issue 6 https://doi.org/10.1016/j.fuproc.2009.02.007	journal	June 2009
The catalytic reforming of tar from pyrolysis and gasification of brown coal: Effects of parental carbon materials on the performance of char catalysts Zhang, Shu; Chen, Zongding; Zhang, Haiyong Fuel Processing Technology, Vol. 174 https://doi.org/10.1016/j.fuproc.2018.02.022	journal	June 2018
Technoeconomic analysis for hydrogen and carbon Co-Production via catalytic pyrolysis of methane Riley, Jarrett; Atallah, Chris; Siriwardane, Ranjani International Journal of Hydrogen Energy, Vol. 46, Issue 39 https://doi.org/10.1016/j.ijhydene.2021.03.151	journal	June 2021
Steam reforming of toluene as model compound of biomass tar over Ni–Co/La2O3 nano-catalysts: Synergy of Ni and Co Gao, Xingyuan; Ashok, Jangam; Kawi, Sibudjing International Journal of Hydrogen Energy, Vol. 46, Issue 60 https://doi.org/10.1016/j.ijhydene.2021.04.047	journal	September 2021
Investigation of methane and ethane pyrolysis with highly active and durable iron-alumina catalyst to produce hydrogen and valuable nano carbons: Continuous fluidized bed tests and reaction rate analysis Siriwardane, Ranjani; Riley, Jarrett; Atallah, Christopher International Journal of Hydrogen Energy, Vol. 48, Issue 38 https://doi.org/10.1016/j.ijhydene.2022.12.268	journal	May 2023
The phenol steam reforming reaction over MgO-based supported Rh catalysts Polychronopoulou, K.; Fierro, J. L. G.; Efstathiou, A. M. Journal of Catalysis, Vol. 228, Issue 2 https://doi.org/10.1016/j.jcat.2004.09.016	journal	December 2004
Effects of cerium and lanthanum on Ni-based catalysts for CO2 reforming of toluene Abou Rached, Jihane; Cesario, Moisés R.; Estephane, Jane Journal of Environmental Chemical Engineering, Vol. 6, Issue 4 https://doi.org/10.1016/j.jece.2018.06.054	journal	August 2018
A short overview on purification and conditioning of syngas produced by biomass gasification: Catalytic strategies, process intensification and new concepts Richardson, Yohan; Blin, Joël; Julbe, Anne Progress in Energy and Combustion Science, Vol. 38, Issue 6 https://doi.org/10.1016/j.pecs.2011.12.001	journal	December 2012
Catalytic decomposition of biomass tars: use of dolomite and untreated olivine Devi, Lopamudra; Ptasinski, Krzysztof J.; Janssen, Frans J. J. G. Renewable Energy, Vol. 30, Issue 4 https://doi.org/10.1016/j.renene.2004.07.014	journal	April 2005
Tar reduction in biomass producer gas via mechanical, catalytic and thermal methods: A review Anis, Samsudin; Zainal, Z. A. Renewable and Sustainable Energy Reviews, Vol. 15, Issue 5 https://doi.org/10.1016/j.rser.2011.02.018	journal	June 2011
Barriers of commercial power generation using biomass gasification gas: A review Asadullah, Mohammad Renewable and Sustainable Energy Reviews, Vol. 29 https://doi.org/10.1016/j.rser.2013.08.074	journal	January 2014
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
Methane Pyrolysis for Carbon Nanotubes and CO _x -Free H ₂ over Transition-Metal Catalysts Wang, I-Wen; Kutteri, Deepa Ayillath; Gao, Bingying Energy & Fuels, Vol. 33, Issue 1 https://doi.org/10.1021/acs.energyfuels.8b03502	journal	December 2018
Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency Jiang, Changle; Wang, I-Wen; Bai, Xinwei Industrial & Engineering Chemistry Research, Vol. 61, Issue 15 https://doi.org/10.1021/acs.iecr.1c05082	journal	April 2022
Microwave-Specific Enhancement of the Carbon–Carbon Dioxide (Boudouard) Reaction Hunt, Jacob; Ferrari, Anthony; Lita, Adrian The Journal of Physical Chemistry C, Vol. 117, Issue 51, p. 26871-26880 https://doi.org/10.1021/jp4076965	journal	November 2013
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
Microwave-assisted heterogeneous catalysis Muley, Pranjali D.; Wang, Yuxin; Hu, Jianli Catalysis https://doi.org/10.1039/9781839163128-00001	book	June 2021
Microwave catalytic effect: a new exact reason for microwave-driven heterogeneous gas-phase catalytic reactions Xu, Wentao; Zhou, Jicheng; Su, Zhiming Catalysis Science & Technology, Vol. 6, Issue 3 https://doi.org/10.1039/C5CY01802A	journal	January 2016
Microwave catalytic synthesis of ammonia from methane and nitrogen Bai, Xinwei; Tiwari, Sarojini; Robinson, Brandon Catalysis Science & Technology, Vol. 8, Issue 24 https://doi.org/10.1039/C8CY01355A	journal	January 2018
Apparent equilibrium shifts and hot-spot formation for catalytic reactions induced by microwave dielectric heating Zhang, Xunli; Hayward, David O.; Mingos, D. Michael P. Chemical Communications, Issue 11 https://doi.org/10.1039/a901245a	journal	January 1999
Conversion of carbon dioxide to few-layer graphene Chakrabarti, Amartya; Lu, Jun; Skrabutenas, Jennifer C. Journal of Materials Chemistry, Vol. 21, Issue 26 https://doi.org/10.1039/c1jm11227a	journal	January 2011
Electronic Structure of Hollow Graphitic Carbon Nanoparticles Fabricated from Acetylene Carbon Black Ilkiv, Bogdan; Petrovska, Svitlana; Sergiienko, Ruslan Fullerenes, Nanotubes and Carbon Nanostructures, Vol. 23, Issue 5 https://doi.org/10.1080/1536383X.2014.885957	journal	June 2014
Microwave power applications Osepchuk, J. M. IEEE Transactions on Microwave Theory and Techniques, Vol. 50, Issue 3 https://doi.org/10.1109/TMTT.2002.989981	journal	March 2002
Unique Approach for Transforming Glucose to C3 Platform Chemicals Using Metallic Iron and a Pd/C Catalyst in Water Hirano, Yoshiaki; Kasai, Yuka; Sagata, Kunimasa Bulletin of the Chemical Society of Japan, Vol. 89, Issue 9 https://doi.org/10.1246/bcsj.20160114	journal	June 2016
Fe-Promoted Alumina-Supported Ni Catalyst Stabilized by Zirconia for Methane Dry Reforming Fakeeha, Anis H.; Al-Baqmaa, Yousef A.; Ibrahim, Ahmed A. Catalysts, Vol. 13, Issue 5 https://doi.org/10.3390/catal13050806	journal	April 2023

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