Structural Characteristics and Graphitizability of Tars from Thermal versus Microwave Plasma Pyrolysis of Coals

Gharpure, Akshay; Viswanathan, Vignesh; Mantri, Aayush; Skoptsov, George; Vander Wal, Randy L.

doi:10.1021/acsomega.3c06666

Structural Characteristics and Graphitizability of Tars from Thermal versus Microwave Plasma Pyrolysis of Coals

Journal Article · Thu Jan 11 00:00:00 EST 2024 · ACS Omega

DOI:https://doi.org/10.1021/acsomega.3c06666· OSTI ID:2471896

^[1]; Viswanathan, Vignesh ^[2]; Mantri, Aayush ^[2]; Skoptsov, George ^[2]; ^[3]

Pennsylvania State University, University Park, PA (United States); Pennsylvania State Univ., University Park, PA (United States)
H Quest Vanguard, Inc., Pittsburgh, PA (United States)
Pennsylvania State University, University Park, PA (United States)

This work investigates the structural characteristics and graphitizability of tars obtained from thermal pyrolysis versus the reactive microwave (MW) plasma pyrolysis of coals. Powder River Basin (PRB) coal tars obtained by thermal pyrolysis have been compared with tars obtained from MW plasma pyrolysis containing H₂. To study the effect of coal rank and MW plasma environment, the PRB tars have been compared with Middle Kittanning (MK) coal tars obtained from an argon–hydrogen MW plasma (hp) and an argon-CO₂ MW plasma (cdp) environment. Fourier transform infrared spectroscopy has been used for investigating the structural differences among the tar samples. The tars have been graphitized (GR-) at 2500 °C and the graphitic quality assessment has been performed using X-ray diffraction and transmission electron microscopy. MW plasma-derived tars have higher aromaticity, lower condensation, and lower oxygenated molecules compared to thermally derived tars. These advantageous features of MW plasma-derived tars lead to the formation of crystallites several times larger than thermally derived tars after graphitization. When considering coal of the same rank (bituminous), the choice of the MW plasma environment has a substantial impact on the graphitic quality of the tars. The utilization of MW plasma containing H₂ leads to a significant increase in both the crystallite diameter (by 60%) and stacking height (by 40%) compared to MW plasma containing CO₂. Furthermore, within the same MW plasma environment, the coal rank plays a significant role in determining the crystallite diameter and stacking height of the GR-tars. In particular, GR-MK tar obtained from hp exhibits a 135% larger crystallite diameter and 85% larger stacking height compared with GR-PRB tar obtained from hp. These findings demonstrate the potential to tailor the composition of coal-derived tars and consequently influence their graphitizability by adjusting the reactive environment during MW plasma treatment.

View Accepted Manuscript (DOE)

Research Organization:: H Quest Vanguard, Inc., Pittsburgh, PA (United States)

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

Grant/Contract Number:: FE0031793

OSTI ID:: 2471896

Journal Information:: ACS Omega, Journal Name: ACS Omega Journal Issue: 3 Vol. 9; ISSN 2470-1343

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (35)

Modifying carbonization properties of pitches. 1. Conversion of benzene-insoluble matter of coal-tar pitch into graphitizable carbon Mochida, Isao; Kudo, Keiko; Takeshita, Kenjiro Fuel, Vol. 53, Issue 4 https://doi.org/10.1016/0016-2361(74)90045-3	journal	October 1974
Effect of coal type on the flash pyrolysis of various coals Xu, W.; Tomita, A. Fuel, Vol. 66, Issue 5 https://doi.org/10.1016/0016-2361(87)90270-5	journal	May 1987
Progress in coal pyrolysis Solomon, P. R.; Fletcher, T. H.; Pugmire, R. J. Fuel, Vol. 72, Issue 5 https://doi.org/10.1016/0016-2361(93)90570-R	journal	May 1993
Rapid microwave pyrolysis of coal Monsef-Mirzai, Parisa; Ravindran, Mythili; McWhinnie, William R. Fuel, Vol. 74, Issue 1 https://doi.org/10.1016/0016-2361(94)P4325-V	journal	January 1995
Fourier transform infrared study of coal tar pitches Guillén, Maria D.; Iglesias, Maria J.; Domínguez, Antonio Fuel, Vol. 74, Issue 11 https://doi.org/10.1016/0016-2361(95)00139-V	journal	November 1995
Characterisation of coal tar pitches by thermal analysis, infrared spectroscopy and solvent fractionation Alcañiz-Monge, J.; Cazorla-Amorós, D.; Linares-Solano, A. Fuel, Vol. 80, Issue 1 https://doi.org/10.1016/S0016-2361(00)00057-0	journal	January 2001
Improving graphenic quality by oxidative liberation of crosslinks in non-graphitizable carbons Gharpure, Akshay; Vander Wal, Randy Carbon, Vol. 209 https://doi.org/10.1016/j.carbon.2023.118010	journal	June 2023
Energy consumption estimation in the scaling-up of microwave heating processes Bermúdez, J. M.; Beneroso, D.; Rey-Raap, N. Chemical Engineering and Processing: Process Intensification, Vol. 95 https://doi.org/10.1016/j.cep.2015.05.001	journal	September 2015
Effects of microwave-assisted pyrolysis on the microstructure of bituminous coals Li, He; Shi, Shiliang; Lin, Baiquan Energy, Vol. 187 https://doi.org/10.1016/j.energy.2019.115986	journal	November 2019
The effect of microwave pre-heating on five different coals Lester, E.; Kingman, S. Fuel, Vol. 83, Issue 14-15 https://doi.org/10.1016/j.fuel.2004.05.006	journal	October 2004
Microwave assisted coal conversion Singh, S.; Neculaes, V. B.; Lissianski, V. Fuel, Vol. 140 https://doi.org/10.1016/j.fuel.2014.09.108	journal	January 2015
Microwave heating processes involving carbon materials Menéndez, J. A.; Arenillas, A.; Fidalgo, B. Fuel Processing Technology, Vol. 91, Issue 1 https://doi.org/10.1016/j.fuproc.2009.08.021	journal	January 2010
Temperature rise characteristics of ZhunDong coal during microwave pyrolysis Liu, Huan-Peng; Chen, Tai-Ping; Li, Yang Fuel Processing Technology, Vol. 148 https://doi.org/10.1016/j.fuproc.2016.03.017	journal	July 2016
Microwave assisted pyrolysis of Indian and Indonesian coals and product characterization Reddy, B. Rajasekhar; Vinu, R. Fuel Processing Technology, Vol. 154 https://doi.org/10.1016/j.fuproc.2016.08.016	journal	December 2016
Microwave drying of a low-rank sub-bituminous coal Pickles, C. A.; Gao, F.; Kelebek, S. Minerals Engineering, Vol. 62 https://doi.org/10.1016/j.mineng.2013.10.011	journal	July 2014
A review on operating parameters for optimum liquid oil yield in biomass pyrolysis Akhtar, Javaid; Saidina Amin, NorAishah Renewable and Sustainable Energy Reviews, Vol. 16, Issue 7 https://doi.org/10.1016/j.rser.2012.05.033	journal	September 2012
A review on microwave assisted pyrolysis of coal and biomass for fuel production Mushtaq, Faisal; Mat, Ramli; Ani, Farid Nasir Renewable and Sustainable Energy Reviews, Vol. 39 https://doi.org/10.1016/j.rser.2014.07.073	journal	November 2014
Reaction of methane with coal Yang, K. Fuel, Vol. 76, Issue 12 https://doi.org/10.1016/s0016-2361(97)00134-8	journal	October 1997
Brown coal conversion by microwave plasma reactions under successive supply of methane Kamei, Osamu; Onoe, Kaoru; Marushima, Wataru Fuel, Vol. 77, Issue 13 https://doi.org/10.1016/s0016-2361(98)00055-6	journal	October 1998
Liquefaction of Turkish coals in tetralin with microwaves Şimşek, Emir H.; Karaduman, Ali; Olcay, Aral Fuel Processing Technology, Vol. 73, Issue 2 https://doi.org/10.1016/s0378-3820(01)00196-5	journal	October 2001
Maxwell–Wagner Effect Applied to Microwave-Induced Self-Ignition: A Novel Approach for Carbon-Based Materials Bizzi, Cezar A.; Cruz, Sandra M.; Schmidt, Lucas Analytical Chemistry, Vol. 90, Issue 7 https://doi.org/10.1021/acs.analchem.7b03731	journal	February 2018
Enhancing Graphitic Carbon Precursors from Coal Pyrolysis: A Comparative Analysis of Microwave Plasma and Conventional Thermal Upgradation Methods Gharpure, Akshay; Vander Wal, Randy L. ACS Omega, Vol. 8, Issue 43 https://doi.org/10.1021/acsomega.3c05382	journal	October 2023
Coal pyrolysis yields from fast and slow heating in a wire-mesh apparatus with a gas sweep Gibbins-Matham, Jon; Kandiyoti, Rafael Energy & Fuels, Vol. 2, Issue 4 https://doi.org/10.1021/ef00010a017	journal	July 1988
An experimental and modeling study of heating rate and particle size effects in bituminous coal pyrolysis Griffin, Thomas P.; Howard, Jack B.; Peters, William A. Energy & Fuels, Vol. 7, Issue 2 https://doi.org/10.1021/ef00038a021	journal	March 1993
Experimental Study on Microwave Pyrolysis of an Indonesian Low-Rank Coal Wang, Nan; Yu, Jianglong; Tahmasebi, Arash Energy & Fuels, Vol. 28, Issue 1 https://doi.org/10.1021/ef401424p	journal	November 2013
Pyrolysis of Coals in a Microwave Discharge Fu, Y. C.; Blaustein, B. D. Industrial & Engineering Chemistry Process Design and Development, Vol. 8, Issue 2 https://doi.org/10.1021/i260030a017	journal	April 1969
Reactions of hydrogen atoms produced by microwave discharge with olefins in acetone and toluene Beeri, Ahuva.; Berman, Elisha.; Vishkautsan, Rosita. Journal of the American Chemical Society, Vol. 108, Issue 20 https://doi.org/10.1021/ja00280a062	journal	October 1986
General equation for the determination of the crystallite size La of nanographite by Raman spectroscopy Cançado, L. G.; Takai, K.; Enoki, T. Applied Physics Letters, Vol. 88, Issue 16 https://doi.org/10.1063/1.2196057	journal	April 2006
A Review of Microwave Coal Processing Binner, Eleanor; Lester, Edward; Kingman, Sam Journal of Microwave Power and Electromagnetic Energy, Vol. 48, Issue 1 https://doi.org/10.1080/08327823.2014.11689870	journal	January 2014
The Scherrer Formula for X-Ray Particle Size Determination Patterson, A. L. Physical Review, Vol. 56, Issue 10 https://doi.org/10.1103/PhysRev.56.978	journal	November 1939
X-Ray Diffraction in Random Layer Lattices Warren, B. E. Physical Review, Vol. 59, Issue 9 https://doi.org/10.1103/PhysRev.59.693	journal	May 1941
Microwave Plasma Formation of Nanographene and Graphitic Carbon Black Kumal, Raju R.; Gharpure, Akshay; Viswanathan, Vignesh C, Vol. 6, Issue 4 https://doi.org/10.3390/c6040070	journal	October 2020
Synthetic Pitch from Solvent Extraction of Coal as a Source for High-Quality Graphite Gharpure, Akshay; Vander Wal, Randy L.; Pisupati, Sarma C, Vol. 9, Issue 2 https://doi.org/10.3390/c9020056	journal	June 2023
A Research on Microwave and Conventional Pyrolysis for Low Rank Coal Song, Yong Hui; Li, Xin; Shi, Jun Wei Advanced Materials Research, Vol. 1044-1045 https://doi.org/10.4028/www.scientific.net/AMR.1044-1045.209	journal	October 2014
Analysis of Products by Conventional and Microwave Induced Pyrolysis for Low Rank Coal Song, Yong Hui; Shi, Jun Wei; Fu, Jian Ping Advanced Materials Research, Vol. 524-527 https://doi.org/10.4028/www.scientific.net/AMR.524-527.871	journal	May 2012