Abstract
Oxygenates production from the partial oxidation of liquid fuel is required for a cleaner combustion. The effect of Mn/Fe ratio was investigated to improve the oxygenates formation via plasma catalytic n-C5H12 partial oxidation over FeMn/Al2O3 catalyst. The oxygenates selectivities exhibited a volcano shape with the Mn/Fe ratio and the highest value of 69% was obtained at Mn/Fe ratio of 7/3. The oxygenates selectivities were dominated by both the acidity and active oxygen species of catalyst, which could be tuned by Mn/Fe ratio. A close relationship between oxygenates selectivities, acidity, and active oxygen species of catalyst was established. The higher the active oxygen species content and the lower the acidity, the higher the oxygenates selectivities.
Similar content being viewed by others
References
Buttner W, Rivkin C, Burgess R, Hartmann K, Bloomfield I, Bubar M, Post M, Boon-Brett L, Weidner E, Moretto P (2017) Hydrogen monitoring requirements in the global technical regulation on hydrogen and fuel cell vehicles. Int J Hydrog Energy 42:7664–7671
Lim CS, Lim JH, Cha JS, Lim JY (2019) Comparative effects of oxygenates-gasoline blended fuels on the exhaust emissions in gasoline-powered vehicles. J Environ Manage 239:103–113
Bkour Q, Che F, Lee KM, Zhou C, Akter N, Boscoboinik JA, Zhao K, Gray JT, Saunders SR, Grant Norton M, McEwen JS, Kim T, Ha S (2020) Enhancing the partial oxidation of gasoline with Mo-doped ni catalysts for SOFC applications: an integrated experimental and DFT study. Appl Catal B 266:118626
Liu Y, Qin L, Cheng Z, Goetze JW, Kong F, Fan JA, Fan LS (2019) Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation. Nat Commun 10:5503
Gallagher MJ, Geiger R, Polevich A, Rabinovich A, Gutsol A, Fridman A (2010) On-board plasma-assisted conversion of heavy hydrocarbons into synthesis gas. Fuel 89:1187–1192
Shirazi M, Neyts EC, Bogaerts A (2017) DFT study of Ni-catalyzed plasma dry reforming of methane. Appl Catal B 205:605–614
Fadaeerayeni S, Yu X, Sarnello E, Bao Z, Jiang X, Unocic RR, Fang L, Wu Z, Li T, Xiang Y (2022) Ammonia-assisted light alkane anti-coke reforming on isolated ReOx sites in zeolite. ACS Catal 12:3165–3172
Diao Y, Zhang X, Liu Y, Chen B, Wu G, Shi C (2022) Plasma-assisted dry reforming of methane over Mo2C-Ni/Al2O3 catalysts: effects of β-Mo2C promoter. Appl Catal B 301:120779
Alharbi AA, Alqahtani NB, Alkhedhair AM, Alabduly AJ, Almaleki AA, Almadih MH, Albishi MS, Almayeef AA (2022) A developed plasmatron design to enhance production of hydrogen in synthesis gas produced by a fuel reformer system, Energies,
Li K, Liu JL, Li XS, Lian HY, Zhu X, Bogaerts A, Zhu AM (2018) Novel power-to-syngas concept for plasma catalytic reforming coupled with water electrolysis. Chem Eng J 353:297–304
Yi Y, Wang X, Jafarzadeh A, Wang L, Liu P, He B, Yan J, Zhang R, Zhang H, Liu X, Guo H, Neyts EC, Bogaerts A (2021) Plasma-catalytic ammonia reforming of methane over Cu-based catalysts for the production of HCN and H2 at reduced temperature. ACS Catal 11:1765–1773
Nguyen DB, Trinh QH, Hossain MM, Lee WG, Mok YS (2020) Enhancement of plasma-assisted catalytic CO2 reforming of CH4 to syngas by avoiding outside air discharges from ground electrode. Int J Hydrog Energy 45:18519–18532
Matyakubov N, Nguyen DB, Saud S, Mok YS (2022) Enhancing the selective catalytic reduction of NOx at low temperature by pretreatment of hydrocarbons in a gliding arc plasma. Ind Eng Chem Res 61:3365–3373
Liu S, Winter LR, Chen JG (2020) Review of plasma-assisted catalysis for selective generation of oxygenates from CO2 and CH4. ACS Catal 10:2855–2871
Fan Y, Zhao W, Shao S, Cai Y, Chen Y, Jin L (2018) Promotion of the vapors from biomass vacuum pyrolysis for biofuels under non-thermal plasma synergistic catalysis (NPSC) system. Energy 142:462–472
Xia Y, Lu N, Li J, Jiang N, Shang K, Wu Y (2020) Combined steam and CO2 reforming of CH4 for syngas production in a gliding arc discharge plasma. J CO2 Utilization 37:248–259
Wang B, Liu S, Peng Y, Wang C, Zou J (2021) Heptane dry reforming and coupling with partial oxidation in gliding arc discharge plasma for H2 production. Fuel Process Technol 221:106943
Liu S, Wang B, Cheng Y, Wang C, Zou J (2022) Ethanol partial oxidative reforming in gliding arc discharge plasma: a better understanding by a kinetic model study. Fuel 328:125309
Lian HY, Liu JL, Li XS, Zhu AM (2020) Disclosure of water roles in gliding arc plasma reforming of methanol for hydrogen production. Plasma Processes Polym 17:2000069
Zhang H, Zhu F, Li X, Cen K, Du C, Tu X (2016) Enhanced hydrogen production by methanol decomposition using a novel rotating gliding arc discharge plasma. RSC Adv 6:12770–12781
Piavis W, Turn S, Ali Mousavi SM (2015) Non-thermal gliding-arc plasma reforming of dodecane and hydroprocessed renewable diesel. Int J Hydrog Energy 40:13295–13305
Tamošiūnas A, Gimžauskaitė D, Uscila R, Aikas M (2019) Thermal arc plasma gasification of waste glycerol to syngas. Appl Energy 251:113306
Tu X, Whitehead JC (2014) Plasma dry reforming of methane in an atmospheric pressure AC gliding arc discharge: co-generation of syngas and carbon nanomaterials. Int J Hydrog Energy 39:9658–9669
Song F, Wu Y, Xu S, Yang X, Xuan Y (2020) N-Decane reforming by gliding arc plasma in air and nitrogen. Plasma Chem Plasma Process 40:1429–1443
Wang B, Peng Y, Yao S (2019) Oxidative reforming of n-heptane in gliding arc plasma reformer for hydrogen production. Int J Hydrog Energy 44:22831–22840
Rahmati H, Ghorbanzadeh A (2021) Parallel electrodes gliding plasma: working principles and application in dry reforming of methane. Energy 230:120753
Rahmani A, Nikravech M (2018) Impact of argon in reforming of (CH4 + CO2) in surface dielectric barrier discharge reactor to produce syngas and liquid fuels. Plasma Chem Plasma Process 38:517–534
Michielsen I, Uytdenhouwen Y, Bogaerts A, Meynen V (2019) Altering conversion and product selectivity of dry reforming of methane in a dielectric barrier discharge by changing the dielectric packing material, Catalysts,
Zhang X, Wenren Y, Chen J, Zhang L, Jin Y, Liu Z, Jin H, Liu Q, Zhu Z (2022) Partial oxidation of n-pentane to syngas and oxygenates in a dielectric barrier discharge reactor. Fuel 307:121814
Chawdhury P, Bhargavi KVSS, Subrahmanyam C (2020) Enhanced synergy by plasma reduced pd nanoparticles on in-plasma catalytic methane conversion to liquid oxygenates. Catal Commun 147:106139
Li J, Dou L, Gao Y, Hei X, Yu F, Shao T (2021) Revealing the active sites of the structured Ni-based catalysts for one-step CO2/CH4 conversion into oxygenates by plasma-catalysis. J CO2 Utilization 52:101675
Andersen JA, Christensen JM, Østberg M, Bogaerts A, Jensen AD (2020) Plasma-catalytic dry reforming of methane: screening of catalytic materials in a coaxial packed-bed DBD reactor. Chem Eng J 397:125519
Bouchoul N, Fourré E, Duarte A, Tanchoux N, Louste C, Batiot C, Dupeyrat (2021) Plasma-metal oxides coupling for CH4-CO2 transformation into syngas and/or hydrocarbons, oxygenates. Catal Today 369:62–68
Wang Y, Chen Y, Harding J, He H, Bogaerts A, Tu X (2022) Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions. Chem Eng J 450:137860
Mei D, Sun M, Liu S, Zhang P, Fang Z, Tu X (2023) Plasma-enabled catalytic dry reforming of CH4 into syngas, hydrocarbons and oxygenates: insight into the active metals of γ-Al2O3 supported catalysts. J CO2 Utilization 67:102307
Lašič Jurković D, Puliyalil H, Pohar A, Likozar B (2019) Plasma-activated methane partial oxidation reaction to oxygenate platform chemicals over Fe, Mo, pd and zeolite catalysts. Int J Energy Res 43:8085–8099
Wang A, Harrhy JH, Meng S, He P, Liu L, Song H (2019) Nonthermal plasma-catalytic conversion of biogas to liquid chemicals with low coke formation. Energy Conv Manag 191:93–101
Gao Y, Dou L, Feng B, Zhang C, Shao T (2023) Catalyst-free activation of CH4 and air into platform chemicals and H2 using parametrized nanosecond pulsed plasma. Energy Conv Manag 276:116570
Indarto A (2016) Partial oxidation of methane to methanol with nitrogen dioxide in dielectric barrier discharge plasma: experimental and molecular modeling. Plasma Sources Sci Technol 25:025002
Chawdhury P, Kumar D, Subrahmanyam C (2019) NTP reactor for a single stage methane conversion to methanol: influence of catalyst addition and effect of promoters. Chem Eng J 372:638–647
Zhang X, He Z, Wenren Y, Wang D, Pan H, Jin Y, Zhu Z, Zhang L, Li K (2023) Enhanced oxygenates production from plasma catalytic partial oxidation of n-pentane over Fe/Al2O3 catalyst. Catal Today 420:114033
Yi Y, Li S, Cui Z, Hao Y, Zhang Y, Wang L, Liu P, Tu X, Xu X, Guo H, Bogaerts A (2021) Selective oxidation of CH4 to CH3OH through plasma catalysis: insights from catalyst characterization and chemical kinetics modelling. Appl Catal B 296:120384
Dou L, Liu Y, Gao Y, Li J, Hu X, Zhang S, Ostrikov K, Shao T (2022) Disentangling metallic cobalt sites and oxygen vacancy effects in synergistic plasma-catalytic CO2/CH4 conversion into oxygenates. Appl Catal B 318:121830
Kalamaras C, Palomas D, Bos R, Horton A, Crimmin M, Hellgardt K (2016) Selective oxidation of methane to methanol over Cu- and Fe-Exchanged zeolites: the Effect of Si/Al Molar ratio. Catal Lett 146:483–492
Wang Y, Fan L, Xu H, Du X, Xiao H, Qian J, Zhu Y, Tu X, Wang L (2022) Insight into the synthesis of alcohols and acids in plasma-driven conversion of CO2 and CH4 over copper-based catalysts. Appl Catal B 315:121583
Chawdhury P, Wang Y, Ray D, Mathieu S, Wang N, Harding J, Bin F, Tu X, Subrahmanyam C (2021) A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature. Appl Catal B 284:119735
Kogelschatz U (2003) Dielectric-barrier discharges: their history, discharge physics, and industrial applications. Plasma Chem Plasma Process 23:1–46
Wu Z, Hao X, Zhou W, Yao S, Han J, Tang X, Zhang X (2018) N-pentane activation and products formation in a temperature-controlled dielectric barrier discharge reactor. Plasma Sources Sci Technol 27:115002
Acknowledgements
This work was supported by the National Natural Science Foundation of China (11775189 and U1709209, 22006166), the Key Research and Development Program of Zhejiang Province (2019C03117 and 2021C01102), the top-notch talent support program of Zhejiang Province (2019R51002), and the National Natural Science Foundation of China (51876194 and U1909216), Public Welfare Research Projects of Zhejiang Province (LGF21B070003), Science Foundation of Zhejiang Sci-Tech University (19022108-Y, 21022310-Y and 21022092-Y), the Achievement Cultivation Project from Shaoxing-keqiao Institute of Zhejiang Sci-Tech University (KYY2022001C).
Author information
Authors and Affiliations
Contributions
X.M. Z.: Conceptualization, Methodology, Formal analysis. W.Q. S.: Visualization, Methodology, Formal analysis. Z.J. H.: Investigation, Formal analysis. Y. L.: Visualization. D.D. W.: Visualization. H. P.: Writing - review & editing. Y.Z. J.: Formal analysis. Z.C. Z.: Writing - review & editing. L.C. Z.: Formal analysis. K. L.: Formal analysis, Conceptualization, Supervision, Writing - review & editing.
Corresponding author
Ethics declarations
Competing Interests
The authors declare no competing interests.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Zhang, X., Shen, W., He, Z. et al. The Effect of Mn/Fe Ratio on the Oxygenates Distribution from Partial Oxidation of n-C5H12 by Plasma Catalysis Over FeMn/Al2O3 Catalyst. Plasma Chem Plasma Process 44, 837–852 (2024). https://doi.org/10.1007/s11090-024-10445-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11090-024-10445-z