journal article·2025-08Open access

Novel concept for synthesizing carbon nano-onion, graphene layers, and graphene nano-ribbons from polypropylene waste over Fe2O3 nanoparticles

Ahmed M. Haggar, Ateyya A. Aboul-Enein, Ahmed E. Awadallah, Mostafa A. Azab

Carbon Letters· Volume 35· Issue 4

Abstract

Abstract In order to optimize the manufacturing of polypropylene-derived few-layer graphene, an innovative utilization of non-supported iron oxide nanoparticles generated under various fuel environment conditions was studied. Three distinct fuel combustion environment circumstances (fusion, fuel shortage, and fuel excess) produced a variety of Fe2O3 nanoparticles for cost-effective and green graphene deposition. XRD, H2-TPR, Raman, and TGA measurements were used to characterize both new and spent catalysts. Remarkably, the microstructure of the generated Fe2O3 nanoparticles could be controlled by the citric acid/iron nitrate ratio, ranging from spheroids (Fe2O3(0)) to sheets (Fe2O3(0.5-0.75)) and a hybrid microstructure that consists of sheets, spheroids, and interconnected strips (Fe2O3(1-2)). According to fuel situation (citric acid/iron nitrate ratio, Fe2O3(0-2)), various graphitization level and yields of graphene derivatives including sheets, ribbons, and onions have been developed. With the ideal fuel/oxidant ratio (ɸ = 1), the Fe2O3(0.75) catalyst demonstrated the best catalytic activity to deposit the largest yield of highly graphitized few graphene layers (280%). Lean and rich fuel conditions (1 > ɸ > 1) have detrimental effects on the amount and quality of graphene deposition. It is interesting to note that in addition to graphene sheets, an excess of citric acid caused the production of metallic cores, hollow, and merged carbon nano-onions, and graphene nano-ribbons. It was suggested that carbon nano-onions be converted into graphene nano-ribbons and semi-onion shell-like graphene layers. Graphical abstract
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Graphene research and applications · Graphene and Nanomaterials Applications · Nanomaterials for catalytic reactions

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (55)

Show source-provided references
1. Plastics—the Facts 2020 An analysis of European plastics production, demand and waste data. https://plasticseurope.org/knowledge-hub/plastics-the-facts-2020/. Accessed 11 Feb 2025
2. Vieira O, Ribeiro RS, de Tuesta JLD et al (2022) A systematic literature review on the conversion of plastic wastes into valuable 2D graphene-based materials. Chem Eng J 428:13139910.1016/j.cej.2021.131399 ↗
3. Miranda MN, Silva AMT, Pereira MFR (2020) Microplastics in the environment: a DPSIR analysis with focus on the responses. Sci Total Environ 718:13496810.1016/j.scitotenv.2019.134968 ↗
4. Park JH, Yang J, Kim D et al (2022) Review of recent technologies for transforming carbon dioxide to carbon materials. Chem Eng J 427:13098010.1016/j.cej.2021.130980 ↗
5. Mbayachi VB, Ndayiragije E, Sammani T et al (2021) Graphene synthesis, characterization and its applications: a review. Results Chem 3:10016310.1016/j.rechem.2021.100163 ↗
6. Pudukudy M, Yaakob Z, Dahani N et al (2017) Production of COx free hydrogen and nanocarbon via methane decomposition over unsupported porous nickel and iron catalysts. J Clust Sci 28:1579–159410.1007/s10876-017-1173-5 ↗
7. Shudin NH, Aziz M, Othman MHD et al (2021) The role of solid, liquid and gaseous hydrocarbon precursors on chemical vapor deposition grown carbon nanomaterials’ growth temperature. Synth Met 274:11673510.1016/j.synthmet.2021.116735 ↗
8. Aboul-Enein AA, Haggar AM, Awadallah AE, Azab MA (2024) Synthesis of polypropylene waste-derived graphene sheets in the presence of metal oxide nanoparticles. Mater Chem Phys 315:129021. https://doi.org/10.1016/j.matchemphys.2024.12902110.1016/j.matchemphys.2024.129021 ↗
9. Liu X, Ma C, Wen Y et al (2021) Highly efficient conversion of waste plastic into thin carbon nanosheets for superior capacitive energy storage. Carbon N Y 171:819–82810.1016/j.carbon.2020.09.057 ↗
10. Cui L, Wang X, Chen N et al (2017) Trash to treasure: converting plastic waste into a useful graphene foil. Nanoscale 9:9089–9094. https://doi.org/10.1039/c7nr03580b10.1039/c7nr03580b ↗
11. Edwards RS, Coleman KS (2013) Graphene synthesis: relationship to applications. Nanoscale 5:38–5110.1039/C2NR32629A ↗
12. Ruan G, Sun Z, Peng Z, Tour JM (2011) Growth of graphene from food, insects, and waste. ACS Nano 5:7601–760710.1021/nn202625c ↗
13. You Y, Mayyas M, Xu S et al (2017) Growth of NiO nanorods, SiC nanowires and monolayer graphene via a CVD method. Green Chem 19:5599–560710.1039/C7GC02523H ↗
14. Sharma S, Kalita G, Hirano R et al (2014) Synthesis of graphene crystals from solid waste plastic by chemical vapor deposition. Carbon N Y 72:66–7310.1016/j.carbon.2014.01.051 ↗
15. Gu J, Pang A, Guo X et al (2021) Green preparation of high-quality and low-cost graphene from discarded polyethylene plastic bags. Chem Commun 57:129–13210.1039/D0CC06999J ↗
16. Pudukudy M, Yaakob Z (2015) Methane decomposition over Ni, Co and Fe based monometallic catalysts supported on sol gel derived SiO2 microflakes. Chem Eng J 262:1009–102110.1016/j.cej.2014.10.077 ↗
17. Shen Y, Lua AC (2013) A facile method for the large-scale continuous synthesis of graphene sheets using a novel catalyst. Sci Rep 3:303710.1038/srep03037 ↗
18. El-Ahwany OM, Awadallah AE, Aboul-Enein AA et al (2020) Dual growth of graphene nanoplatelets and carbon nanotubes hybrid structure via chemical vapor deposition of methane over Fe–MgO catalysts. Fullerenes Nanotub Carbon Nanostruct 28:435–44510.1080/1536383X.2019.1697243 ↗
19. Awadallah AE, Aboul-Enein AA, Kandil UF, Taha MR (2017) Facile and large-scale synthesis of high quality few-layered graphene nano-platelets via methane decomposition over unsupported iron family catalysts. Mater Chem Phys 191:75–8510.1016/j.matchemphys.2017.01.007 ↗
20. Calgaro CO, Perez-Lopez OW (2019) Graphene and carbon nanotubes by CH4 decomposition over CoAl catalysts. Mater Chem Phys 226:6–1910.1016/j.matchemphys.2018.12.094 ↗
21. Jana P, Coronado JM, Serrano DP (2011) Co-production of graphene sheets and hydrogen by decomposition of methane using cobalt based catalysts. Energy Environ Sci 4:778–78310.1039/c0ee00490a ↗
22. Bacsa RR, Cameán I, Ramos A et al (2015) Few layer graphene synthesis on transition metal ferrite catalysts. Carbon N Y 89:350–36010.1016/j.carbon.2015.03.054 ↗
23. Parauha YR, Sahu V, Dhoble SJ (2021) Prospective of combustion method for preparation of nanomaterials: a challenge. Mater Sci Eng B 267:11505410.1016/j.mseb.2021.115054 ↗
24. Fathi H, Masoudpanah SM, Alamolhoda S, Parnianfar H (2017) Effect of fuel type on the microstructure and magnetic properties of solution combusted Fe3O4 powders. Ceram Int 43:7448–745310.1016/j.ceramint.2017.03.017 ↗
25. Radpour M, Masoudpanah SM, Alamolhoda S (2017) Microwave-assisted solution combustion synthesis of Fe3O4 powders. Ceram Int 43:14756–1476210.1016/j.ceramint.2017.07.216 ↗
26. Radpour M, Alamolhoda S, Masoudpanah SM (2017) Effects of pH value on the microstructure and magnetic properties of solution combusted Fe3O4 powders. Ceram Int 43:13729–1373410.1016/j.ceramint.2017.07.085 ↗
27. Lazarova T, Georgieva M, Tzankov D et al (2017) Influence of the type of fuel used for the solution combustion synthesis on the structure, morphology and magnetic properties of nanosized NiFe2O4. J Alloys Compd 700:272–28310.1016/j.jallcom.2017.01.055 ↗
28. Parnianfar H, Masoudpanah SM, Alamolhoda S, Fathi H (2017) Mixture of fuels for solution combustion synthesis of porous Fe3O4 powders. J Magn Magn Mater 432:24–2910.1016/j.jmmm.2017.01.084 ↗
29. González-Cortés SL, Imbert FE (2013) Fundamentals, properties and applications of solid catalysts prepared by solution combustion synthesis (SCS). Appl Catal A Gen 452:117–13110.1016/j.apcata.2012.11.024 ↗
30. Li C, Xiong Z, He J et al (2020) Influence of ignition atmosphere on the structural properties of magnetic iron oxides synthesized via solution combustion and the NH3-SCR activity of W/Fe2O3 catalyst. Appl Catal A Gen 602:11772610.1016/j.apcata.2020.117726 ↗
31. Sun K, Cheng F, Liu Y et al (2022) Microwave-assisted iron oxide process for efficient removal of tetracycline. J Environ Manage 307:11460010.1016/j.jenvman.2022.114600 ↗
32. Chandane P, Ladke J, Jori C et al (2019) Synthesis of magnetic Fe3O4 nanoparticles from scrap iron and use of their peroxidase like activity for phenol detection. J Environ Chem Eng 7:10308310.1016/j.jece.2019.103083 ↗
33. Haggar AM, Awadallah AE, Aboul-Enein AA, Sayed GH (2022) Non-oxidative conversion of real low density polyethylene waste into hydrogen and carbon nanomaterials over MgO supported bimetallic Co-Mo catalysts with different total Co-Mo contents. Chem Eng Sci 247:11709210.1016/j.ces.2021.117092 ↗
34. Acomb JC, Wu C, Williams PT (2016) The use of different metal catalysts for the simultaneous production of carbon nanotubes and hydrogen from pyrolysis of plastic feedstocks. Appl Catal B Environ 180:497–51010.1016/j.apcatb.2015.06.054 ↗
35. Ibrahim AA, Fakeeha AH, Al-Fatesh AS et al (2015) Methane decomposition over iron catalyst for hydrogen production. Int J Hydrogen Energy 40:7593–760010.1016/j.ijhydene.2014.10.058 ↗
36. Qian JX, Chen TW, Enakonda LR et al (2020) Methane decomposition to pure hydrogen and carbon nano materials: State-of-the-art and future perspectives. Int J Hydrogen Energy 45:15721–1574310.1016/j.ijhydene.2020.04.100 ↗
37. Dhand V, Yadav M, Kim SH, Rhee KY (2021) A comprehensive review on the prospects of multi-functional carbon nano onions as an effective, high-performance energy storage material. Carbon N Y 175:534–57510.1016/j.carbon.2020.12.083 ↗
38. Nisticò R, Carlos L (2019) High yield of nano zero-valent iron (nZVI) from carbothermal synthesis using lignin-derived substances from municipal biowaste. J Anal Appl Pyrolysis 140:239–24410.1016/j.jaap.2019.03.022 ↗
39. Zhou L, Enakonda LR, Harb M et al (2017) Fe catalysts for methane decomposition to produce hydrogen and carbon nano materials. Appl Catal B Environ 208:44–5910.1016/j.apcatb.2017.02.052 ↗
40. Ricciardella F, Vollebregt S, Tilmann R et al (2021) Influence of defect density on the gas sensing properties of multi-layered graphene grown by chemical vapor deposition. Carbon Trends 3:10002410.1016/j.cartre.2021.100024 ↗
41. Pandey S, Kumar A, Karakoti M et al (2021) 3D graphene nanosheets from plastic waste for highly efficient HTM free perovskite solar cells. Nanoscale Adv 3:4726–473810.1039/D1NA00183C ↗
42. Giang NH, Hanh TTT, Nga NT, Van Hoang V (2018) Formation of graphene on BN substrate by vapor deposition method and size effects on its structure. Phys B Condens Matter 534:26–3310.1016/j.physb.2017.12.066 ↗
43. Sharma R, Moore E, Rez P, Treacy MMJ (2009) Site-specific fabrication of Fe particles for carbon nanotube growth. Nano Lett 9:689–69410.1021/nl803180e ↗
44. Wirth CT, Bayer BC, Gamalski AD et al (2012) The phase of iron catalyst nanoparticles during carbon nanotube growth. Chem Mater 24:4633–464010.1021/cm301402g ↗
45. Schaper AK, Hou H, Greiner A, Phillipp F (2004) The role of iron carbide in multiwalled carbon nanotube growth. J Catal 222:250–25410.1016/j.jcat.2003.11.011 ↗
46. Shaikjee A, Coville NJ (2012) The role of the hydrocarbon source on the growth of carbon materials. Carbon N Y 50:3376–339810.1016/j.carbon.2012.03.024 ↗
47. Wrobel RJ, Hełminiak A, Arabczyk W, Narkiewicz U (2014) Studies on the kinetics of carbon deposit formation on nanocrystalline iron stabilized with structural promoters. J Phys Chem C 118:15434–1543910.1021/jp4108377 ↗
48. Ni L, Kuroda K, Zhou L-P et al (2009) Decomposition of metal carbides as an elementary step of carbon nanotube synthesis. Carbon N Y 47:3054–306210.1016/j.carbon.2009.07.009 ↗
49. Pinilla JL, Utrilla R, Karn RK et al (2011) High temperature iron-based catalysts for hydrogen and nanostructured carbon production by methane decomposition. Int J Hydrogen Energy 36:7832–784310.1016/j.ijhydene.2011.01.184 ↗
50. Reddy Enakonda L, Zhou L, Saih Y et al (2016) Methane-induced activation mechanism of fused ferric oxide-alumina catalysts during methane decomposition. Chemsuschem 9:1911–191510.1002/cssc.201600500 ↗
51. Velasquez M, Batiot-Dupeyrat C, Gallego J et al (2016) Synthesis of carbon nano-chains from glycerol-ethanol decomposition over Ni-Fe alloy catalyst. Diam Relat Mater 70:105–11310.1016/j.diamond.2016.10.019 ↗
52. Zhang C, Li J, Liu E et al (2012) Synthesis of hollow carbon nano-onions and their use for electrochemical hydrogen storage. Carbon N Y 50:3513–352110.1016/j.carbon.2012.03.019 ↗
53. Luo C, Fu Q, Pan C (2015) Strong magnetic field-assisted growth of carbon nanofibers and its microstructural transformation mechanism. Sci Rep 5:906210.1038/srep09062 ↗
54. Guo W, Xu C, Xu K et al (2016) Rapid chemical vapor deposition of graphene on liquid copper. Synth Met 216:93–9710.1016/j.synthmet.2015.09.011 ↗
55. Kang JL, Li JJ, Du XW et al (2008) Synthesis and growth mechanism of metal filled carbon nanostructures by CVD using Ni/Y catalyst supported on copper. J Alloys Compd 456:290–29610.1016/j.jallcom.2007.02.078 ↗