Energetically efficient and electrochemically tuneable exfoliation of graphite: process monitoring and product characterization
Source abstract
Abstract
In this work, graphene oxide was prepared by electrochemical exfoliation of graphite in sodium dodecylsulfate and sodiumdodecylbenzene sulfonate aqueous solution. Two different working electrodes were used: an electrode prepared from natural graphite flakes and a commercial natural graphite rod. The electrodes were polarized in a two electrode system by a multistep change of polarity or by single anodic and cathodic polarization. The voltage value ranged from 2.5 V to 3.2 V. By monitoring the current transients and the colour of the resultant solutions, it was shown that the exfoliation process depends on the type of working electrode, surfactants and applied voltage value. The multistep change of polarity was more effective compared to single polarization. The ultraviolet-visible spectrophotometry and Raman spectroscopy indicated the presence of defects within the graphene structure while FTIR spectroscopy indicated presence of oxygen functional groups, which is characteristic of graphene oxide (GO). Dynamic light scattering revealed that the solutions obtained in this work contained GO sheets within the size of 10-600 nm. Atomic force microscopy measurements proved that the obtained product contains multi-layer sheets. The energy consumption for the process carried out in this work ranges from 0.084 kWh g-1 to 0.038 kWh g-1 and therefore this process is considered to be a low energy and cost- effective process.
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Research context
OpenAlex topics: Graphene research and applications · Advancements in Battery Materials · Supercapacitor Materials and Fabrication
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References (65)
Show source-provided references
1. Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV, Grigorieva IV, Firsovet AA (2004) Electric field effect in atomically thin carbon films. Science 306:666–669. https://doi.org/10.1126/science.110289610.1126/science.1102896 ↗
2. Alanyalıoğlu M, Segura JJ, Oró –Solè J, Casañ-Pastor N (2012) The synthesis of graphene sheets with controlled thickness and order using surfactant-assisted electrochemical processes. Carbon 50:142–152. https://doi.org/10.1016/j.carbon.2011.07.06410.1016/j.carbon.2011.07.064 ↗
3. Du X, Skachko IS, Barker A, Andrei EY (2008) Approaching ballistic transport in suspended grapheme. Nat Nanotechnol 3:491–495. https://doi.org/10.1038/nnano.2008.19910.1038/nnano.2008.199 ↗
4. Stankovich S, Dikin DA, Dommett GHB, Kohlhaas KM, Zimney EJ, Stach EA, Piner RD, Nguyen ST, Ruoff RS (2006) Graphene-based composite materials. Nature 442:282–286. https://doi.org/10.1038/nature0496910.1038/nature04969 ↗
5. Stoller MD, Park S, Zhu Y, An J, Ruoff RS (2008) Graphene-based ultracapacitors. Nano Lett 8:3498–3502. https://doi.org/10.1021/nl802558y10.1021/nl802558y ↗
6. Lee C, Wei X, Li Q, Carpick R, Kysar JW, Hone J (2009) Elastic and frictional properties of graphene. Phys Status Solidi B 246:2562–2567. https://doi.org/10.1002/pssb.2009823210.1002/pssb.20098232 ↗
7. Nair RR, Blake P, Grigorenko AN, Novoselov KS, Booth TJ, Stauber T, Peres NMR, Geim AK (2008) Fine structure constant defines visual transparency of grapheme. Science 320:1308. https://doi.org/10.1126/science.115696510.1126/science.1156965 ↗
8. Pumera M, Ambrosi A, Bonanni A, Chang ELK, Poh HL (2010) Graphene for electrochemical sensing and biosensing. Trends Anal Chem 29:954–965. https://doi.org/10.1016/j.trac.2010.05.01110.1016/j.trac.2010.05.011 ↗
9. Low CTJ, Walsh FC, Chakrabarti MH, Hashim MA, Hussain MA (2013) Electrochemical approaches to the production of graphene flakes and their potential applications. Carbon 54:1–21. https://doi.org/10.1016/j.carbon.2012.11.03010.1016/j.carbon.2012.11.030 ↗
10. Novoselov KS, Jiang D, Schedin F, Booth TJ, Khotkevich VV, Morozov SV, Geim AK (2005) Two-dimensional atomic crystals. Proc Nat Aca Sci USA 102:10451–10453. https://doi.org/10.1073/pnas.050284810210.1073/pnas.0502848102 ↗
11. Malesevic A, Vitchev R, Schouteden K, Volodin A, Zhang L, Tendeloo GV, Vanhulsel A, Haesendonck CV (2008) Synthesis of few-layer graphene via microwave plasma-enhanced chemical vapour deposition. Nanotechnology 19:305604. https://doi.org/10.1088/0957-4484/19/30/30560410.1088/0957-4484/19/30/305604 ↗
12. Kim KS, Zhao Y, Jang H, Lee SY, Kim JM, Kim KS, Ahn JH, Kim P, Choi JY, Hong BH (2009) Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 457:706–710. https://doi.org/10.1038/nature0771910.1038/nature07719 ↗
13. Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y, Wu Y, Nguyen ST, Ruof RS (2007) Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45:1558–1565. https://doi.org/10.1016/j.carbon.2007.02.03410.1016/j.carbon.2007.02.034 ↗
14. Wang G, Wang B, Park J, Wang Y, Sun B, Yao J (2009) Highly efficient and large-scale synthesis of graphene by electrolytic exfoliation. Carbon 47:3242–3246. https://doi.org/10.1016/j.carbon.2009.07.04010.1016/j.carbon.2009.07.040 ↗
15. Zhong YL, Tian Z, Simon GP, Li D (2015) Scalable production of graphene via wet chemistry: progress and challenges. Mater Today 18:73–78. https://doi.org/10.1016/j.mattod.2014.08.01910.1016/j.mattod.2014.08.019 ↗
16. Parvez K, Wu ZS, Li R, Liu X, Graf R, Feng X, Müllen K (2014) Exfoliation of graphite into graphene in aqueous solutions of inorganic salts. J Am Chem Soc 136:6083–6091. https://doi.org/10.1021/ja501715610.1021/ja5017156 ↗
17. Lu J, Yang J, Wang J, Lim A, Wang S, Loh KP (2009) One-pot synthesis of fluorescent carbon graphene by the exfoliation of graphite in ionic liquids. ASC Nano 3:2367–2375. https://doi.org/10.1021/nn900546b10.1021/nn900546b ↗
18. USPat.8,858,776 B2(Oct. 14, 2014), Li LJ, Su CY(AcademiaSinica, Taipei (TW))
19. Xia ZY, Pezzini S, Treossi E, Giambastiani G, Corticelli F, Morandi V, Zanelli A, Bellani V et al (2013) The exfoliation of graphene in liquids by electrochemical, chemical, and sonication-assisted techniques: a nanoscale study. Adv Funct Mater 37:4684–4693. https://doi.org/10.1002/adfm.20120368610.1002/adfm.201203686 ↗
20. Yu P, Lowe SE, Simon GP, Zhong YL (2015) Electrochemical exfoliation of graphite and production of functional grapheme. Curr Opin Colloid Interface Sci 20:329–338. https://doi.org/10.1016/j.cocis.2015.10.00710.1016/j.cocis.2015.10.007 ↗
21. Chen D, Wang F, Li Y, Wang WW, Huang TX, Li YF, Novoselov KS, Tiana ZQ, Zhan D (2019) Programmed electrochemical exfoliation of graphite to high quality graphene. Chem Comm 55:3379–3382. https://doi.org/10.1039/C9CC00393B10.1039/C9CC00393B ↗
22. Munuera JM, Paredes JI, Villar-Rodil S, Ayán-Varela M, Martínez-Alonso A, Tascón JMD (2016) Electrolytic exfoliation of graphite in water with multifunctional electrolytes: en route towards high quality, oxide-free graphene flakes. Nanoscale 8:2982–2998. https://doi.org/10.1039/C5NR06882G10.1039/C5NR06882G ↗
23. Hathcock KW, Brumfield JC, Goss CA, Irene EA, Murray RW (1995) Incipient electrochemical oxidation of highly oriented pyrolytic graphite: correlation between surface blistering and electrolyte anion intercalation. Anal Chem 67:2201–2206. https://doi.org/10.1021/ac00109a04510.1021/ac00109a045 ↗
24. Noel M, Santhanam R (1998) Electrochemistry of graphite intercalation compounds. J Power Sourc 72:53–65. https://doi.org/10.1016/S0378-7753(97)02675-X10.1016/S0378-7753(97)02675-X ↗
25. Savoskin MV, Yaroshenko AP, Whyman GE, Mestechkin MM, Mysyk RD, Mochalin VN (2003) Theoretical study of stability of graphite intercalationcompounds with Brønsted acids. Carbon 41:2757–2760. https://doi.org/10.1016/S0008-6223(03)00385-310.1016/S0008-6223(03)00385-3 ↗
26. Dreyer DR, Park S, Bielawski CW, Ruoff RS (2010) The chemistry of graphene oxide. Chem Soc Rev 39:228–240. https://doi.org/10.1039/b917103g10.1039/b917103g ↗
27. Parvez K, Li R, Puniredd SR, Hernandez Y, Hinkel F, Wang S, Feng X, Müllen K (2013) Electrochemically exfoliated graphene as solution-processable, highly conductive electrodes for organic electronics. ASC Nano 7:3598–3606. https://doi.org/10.1021/nn400576v10.1021/nn400576v ↗
28. Morales GM, Schifani P, Ellis G, Ballesteros C, Martinez G, Barbero C, Salavagione HJ (2011) High-quality few layer graphene produced by electrochemical intercalation and microwave-assisted expansion of graphite. Carbon 49:2809–2816. https://doi.org/10.1016/j.carbon.2011.03.00810.1016/j.carbon.2011.03.008 ↗
29. Wang J, Manga KK, Bao Q, Loh KP (2011) High-yield synthesis of few-layer graphene flakes through electrochemical expansion of graphite in propylene carbonate electrolyte. J Am Chem Soc 133:8888–8891. https://doi.org/10.1021/ja203725d10.1021/ja203725d ↗
30. Zhong YL, Swager TM (2012) Enhanced electrochemical expansion of graphite for in situ electrochemical functionalization. J Am Chem Soc 134:17896–17899. https://doi.org/10.1021/ja309023f10.1021/ja309023f ↗
31. Munuera JM, Paredes JI, Villar-Rodil S, Martínez-Alonso A, Tascón JMD (2017) A simple strategy to improve the yield of graphene nanosheets in the anodic exfoliation of graphite foil. Carbon 115:625–628. https://doi.org/10.1016/j.carbon.2017.01.03810.1016/j.carbon.2017.01.038 ↗
32. Xu M, Sun H, Shen C, Yang S, Que W, Zhang Y, Song X (2015) Lithium-assisted exfoliation of pristine graphite for few-layer graphene nanosheets. Nano Res 8:801–807. https://doi.org/10.1007/s12274-014-0562-410.1007/s12274-014-0562-4 ↗
33. Su C, Lu A, Xu Y, Chen F, Khlobystov AN, Li L (2011) High-quality thin graphene films from fast electrochemical exfoliation. ACS Nano 5:2332–2339. https://doi.org/10.1021/nn200025p10.1021/nn200025p ↗
34. Mohamed A, Ardyani T, Bakar SA, Brown P, Hollamby M, Sagisaka M, Eastoef J (2016) Graphene-philic surfactants for nanocomposites in latex technology. Adv Colloid Interface Sci 230:54–69. https://doi.org/10.1016/j.cis.2016.01.00310.1016/j.cis.2016.01.003 ↗
35. Rao KS, Senthilnathan J, Liu YF, Yoshimura M (2014) Role of peroxide ions in formation of graphene nanosheets by electrochemical exfoliation of graphite. Sci Rep 4:4237–4242. https://doi.org/10.1038/srep0423710.1038/srep04237 ↗
36. Tripathi P, atel CRP, Shaz MA, Srivastava ON, Synthesis of high-quality graphene through electrochemical exfoliation of graphite in alkaline electrolyte, [cond-mat.mtrl-sci]
37. Liu N, Luo F, Wu H, Liu Y, Zhang C, Chen J (2008) One-step ionic-liquid-assisted electrochemical synthesis of ionic-liquid-functionalized graphene sheets directly from graphite. Adv Funct Mater 18:1518–1525. https://doi.org/10.1002/adfm.20070079710.1002/adfm.200700797 ↗
38. Gurzęda B, Buchwald T, Nocuń M, Bąkowicz A, Krawczyk P (2017) Graphene material preparation through thermal treatment of graphite oxide electrochemically synthesized in aqueous sulfuric acid. RCS Adv 32:19904–19911. https://doi.org/10.1039/c7ra01678f10.1039/c7ra01678f ↗
39. Achee TC, Sun W, Hope JT et al (2018) High-yield scalable graphene nanosheet production from compressed graphite using electrochemical exfoliation. Sci Rep 8:14525. https://doi.org/10.1038/s41598-018-32741-310.1038/s41598-018-32741-3 ↗
40. Liu F, Wang C, Sui X, Xu M, Wei L, Chen Y (2019) Synthesis of graphene materials by electrochemical exfoliation: recent progress and future potential. Carbon Energy 1:173–199. https://doi.org/10.1002/cey2.1410.1002/cey2.14 ↗
41. Wong CH, Sofer Z, Pumera M (2015) Geographical and geological origin of natural graphite heavily influence the electrical and electrochemical properties of chemically modified graphenes. Chem Eur J 21:8435–8440. https://doi.org/10.1002/chem.20150011610.1002/chem.201500116 ↗
42. Wissler M (2006) Graphite and carbon powders for electrochemical applications. J Power Sourc 156:142–150. https://doi.org/10.1016/j.jpowsour.2006.02.06410.1016/j.jpowsour.2006.02.064 ↗
43. Horcas I, Fernández R, Gómez-Rodríguez JM, Colchero J, Gómez-Herrero J, Baro AM (2007) WSXM: a software for scanning probe microscopy and a tool for nanotechnology. Rev Sci Instrum 78:013750. https://doi.org/10.1063/1.243241010.1063/1.2432410 ↗
44. Hsieh CT, Hsueh JH (2016) Electrochemical exfoliation of graphene sheets from a natural graphite flask in the presence of sulfate ions at different temperatures. RSC Adv 6:64826–64831. https://doi.org/10.1039/C6RA15447F10.1039/C6RA15447F ↗
45. Choo H, Kinumoto T, Nose M, Miyazakia K, Abe T, Ogumi Z (2008) Electrochemical oxidation of highly oriented pyrolytic graphite during potential cycling in sulfuric acid solution. J Power Sourc 185:740–746. https://doi.org/10.1016/j.jpowsour.2008.07.08610.1016/j.jpowsour.2008.07.086 ↗
46. Choo H, Kinumoto T, Jeong S, Iriyama Y, Abe T, Ogumi Z (2007) Mechanism for electrochemical oxidation of highly oriented pyrolytic graphite in sulfuric acid solution. J Electrochem Soc 154:1017–1023. https://doi.org/10.1149/1.276741110.1149/1.2767411 ↗
47. Yang S, Ricciardulli AG, Liu S, Dong R, Lohe MR, Becker A, Squillaci MA, Samor P et al (2017) Ultrafast delamination of graphite into high-quality graphene using alternating currents. Angew Chem Int Ed 56:1–8. https://doi.org/10.1002/anie.20170207610.1002/anie.201702076 ↗
48. Jamaluddin NA, Mohamed A, Baka SA et al (2020) Highly branched triple-chain surfactant-mediated electrochemical exfoliation of graphite to obtain graphene oxide: colloidal behaviour and application in water treatment. Phys Chem Chem Phys 22:12732. https://doi.org/10.1039/D0CP01243B10.1039/D0CP01243B ↗
49. Yi Y, Weinberg G, Prenzel M, Greiner M, Heumann M, Becker S, Schlögl R (2017) Electrochemical corrosion of a glassy carbon electrode. Catal Today 295:32–40. https://doi.org/10.1016/j.cattod.2017.07.01310.1016/j.cattod.2017.07.013 ↗
50. Piñeiro-Prado I, Salinas-Torres D, Ruiz-Rosas R, Morallón E, Cazorla-Amorós D (2016) Design of activatedcarbon/activated carbonasymmetric capacitors. Front Mater 3:16. https://doi.org/10.3389/fmats.2016.0001610.3389/fmats.2016.00016 ↗
51. Chen J, Zhang X, Zheng X, Liu C, Cui X, Zheng W (2013) Size distribution-controlled preparation of graphene oxide nanosheets with different C/O ratios. Mater Chem Phys 139:8–11. https://doi.org/10.1016/j.matchemphys.2012.12.02510.1016/j.matchemphys.2012.12.025 ↗
52. Li D, Müller MB, Gilje S, Kaner RB, Wallace GG (2008) Processable aqueous dispersions of graphene nanosheets. Nat Nanotechnol 3:101–105. https://doi.org/10.1038/nnano.2007.45110.1038/nnano.2007.451 ↗
53. Raić M, Sačer D, Kraljić Roković M (2019) Structural and capacitive properties of graphene obtained by a green method of graphene oxide reduction. Chem Biochem Eng Q. 33:385–393. https://doi.org/10.15255/CABEQ.2019.160910.15255/CABEQ.2019.1609 ↗
54. Gurzęda B, Florczak P, Kempiński M, Peplińska B, Krawczyka P, Jurga S (2016) Synthesis of graphite oxide by electrochemical oxidation in aqueous perchloric acid. Carbon 100:540–545. https://doi.org/10.1016/j.carbon.2016.01.04410.1016/j.carbon.2016.01.044 ↗
55. Tien HN, Luan VH, Cuong TV, Kong BS, Chung JS, Kim EJ, Hur SH (2012) Fast and simple reduction of graphene oxide in various organic solvents using microwave irradiation. J Nanosci Nanotechnol 12:5658. https://doi.org/10.1166/jnn.2012.634010.1166/jnn.2012.6340 ↗
56. Yang S, Lohe MR, Müllen K, Feng X (2016) New-generation graphene from electrochemical approaches: production and applications. Adv Mater 28:6213–6221. https://doi.org/10.1002/adma.20150532610.1002/adma.201505326 ↗
57. Sačer D, Spajić I, Kraljić Roković M, Mandić Z (2018) New insights into chemical and electrochemical functionalization of graphene oxide electrodes by o-phenylenediamine and their potential applications. J Mater Sci 53:15285. https://doi.org/10.1007/s10853-018-2693-610.1007/s10853-018-2693-6 ↗
58. Tian P, Tang L, Teng KS, Lau SP (2018) Graphene quantum dots from chemistry to applications. Mater Today Chem 10:221–258. https://doi.org/10.1016/j.mtchem.2018.09.0075910.1016/j.mtchem.2018.09.00759 ↗
59. Tian L, Chen F, Ding H, Li X, Li X (2020) The influence of inorganic electrolyte on the properties of carbon quantum dots in electrochemical exfoliation. J Electroanal Chem 878:114673. https://doi.org/10.1016/j.jelechem.2020.11467310.1016/j.jelechem.2020.114673 ↗
60. Xia Z, Maccaferri G, Zanardi C, Christian M, Ortolani L et al (2019) Dispersion stability and surface morphology study of electrochemically exfoliated bilayer graphene oxide. J Phys Chem C 123:15122–15130. https://doi.org/10.1021/acs.jpcc.9b0339510.1021/acs.jpcc.9b03395 ↗
61. Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y, Wu Y, Nguyen SBT, Ruoff RS (2007) Synthesis of graphene-basednanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45:1558–1565. https://doi.org/10.1016/j.carbon.2007.02.03410.1016/j.carbon.2007.02.034 ↗
62. Lindfors T, Boeva ZA, Latonen RM (2014) Electrochemical synthesis of poly(3,4-ethylenedioxythiophene) in aqueous dispersion of high porosity reduced graphene oxide. RCS Adv 4:25279–25286. https://doi.org/10.1039/C4RA03423F10.1039/C4RA03423F ↗
63. Gutić SJ, Jovanović AZ, Dobrota AS, Metarap D, Rafailović LD, Mentus SV (2018) Simple routes for the improvement of hydrogen evolution activity of Ni-Mo catalysts: from sol-gel derived powder catalysts to graphene supported co-electrodeposits. Inter J Hydrogen Energ 43:16864–16858. https://doi.org/10.1016/j.ijhydene.2017.11.13110.1016/j.ijhydene.2017.11.131 ↗
64. https://ec.europa.eu/eurostat/statistics-explained/index.php/Electricity_price_statistics#Electricity_prices_for_non-household_consumers, August27th, 2020.
65. https://www.graphenea.com/collections/all, August27th, 2020.