Process regulation of the electrochemical exfoliation for graphene production with graphite powder as starting materials
Source abstract
Abstract
Graphite powder as a raw material for the production of graphene by electrochemical exfoliation is superior to bulk graphite in terms of cost-effectiveness and manufacturing process. However, the current technology is still in its infancy and lacks preliminary systematic research. Therefore, there is a blank in the theoretical basis for process optimization and production regulation. Here, the effects of the main process parameters including graphite powder category, electric field driving force, electrolyte type, and corresponding concentration were systematically investigated on the electrochemical exfoliation and graphene quality. Expanded graphite powder with flake structure, regular graphite layer arrangement, and large graphite layer spacing is superior to natural flake graphite powder and artificial graphite powder for the electrochemical exfoliation to produce graphene. Sulfate ion with large ionic radius is best suitable for intercalation and subsequent expansion to obtain a high graphene yield and a low ID/IG in graphene in aqueous solution. For graphite powder as raw material, there exist optimal values for both electrolyte concentration and driving voltage for graphene production. A high graphene yield of 42.5% with low defect density (ID/IG = 0.14–1.43) and oxygen content of 30.54% can be obtained using Na2SO4 at a concentration of 0.1 M at a voltage of 10 V for 4 h. The process optimization and regulation and corresponding influencing mechanisms of process parameters revealed here will provide guidance for the further development of graphene production by electrochemical exfoliation of graphite powder.
Source: expertdata · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Graphene research and applications · Advancements in Battery Materials · Supercapacitor Materials and Fabrication
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (53)
Show source-provided references
1. Novoselov KS, Fal’ko VI, Colombo L, Gellert PR, Schwab MG, Kim K (2012) A roadmap for graphene. Nature 490:192–200. https://doi.org/10.1038/nature1145810.1038/nature11458 ↗
2. Parvez K, Yang S, Feng X, Müllen K (2015) Exfoliation of graphene via wet chemical routes. Synth Met 210:123–132. https://doi.org/10.1016/j.synthmet.2015.07.01410.1016/j.synthmet.2015.07.014 ↗
3. Meyer JC, Geim AK, Katsnelson MI, Novoselov KS, Booth TJ, Roth S (2007) The structure of suspended graphene sheets. Nature 446:60–63. https://doi.org/10.1038/nature0554510.1038/nature05545 ↗
4. Lui CH, Liu L, Mak KF, Flynn GW, Heinz TF (2009) Ultraflat graphene. Nature 462:339–341. https://doi.org/10.1038/nature0856910.1038/nature08569 ↗
5. Geim AK (2009) Graphene: status and prospects. Science 324:1530–1534. https://doi.org/10.1126/science.115887710.1126/science.1158877 ↗
6. Fei Y, Fang S, Hu YH (2020) Synthesis, properties and potential applications of hydrogenated graphene. Chem Eng J 397:125408. https://doi.org/10.1016/j.cej.2020.12540810.1016/j.cej.2020.125408 ↗
7. Yu Q, Jiang J, Jiang L, Yang Q, Yan N (2021) Advances in green synthesis and applications of graphene. Nano Res 14:3724–3743. https://doi.org/10.1007/s12274-021-3336-910.1007/s12274-021-3336-9 ↗
8. Yao J, Sun Y, Yang M, Duan Y (2012) Chemistry, physics and biology of graphene-based nanomaterials: new horizons for sensing, imaging and medicine. J Mater Chem 22:14313–14329. https://doi.org/10.1039/C2JM31632C10.1039/C2JM31632C ↗
9. Kashif M, Jaafar E, Bhadja P, Low FW, Sahari SK, Hussain S, Al-Tamrah SA (2021) Effect of potassium permanganate on morphological, structural and electro-optical properties of graphene oxide thin films. Arab J Chem 14:102953. https://doi.org/10.1016/j.arabjc.2020.10295310.1016/j.arabjc.2020.102953 ↗
10. Lu Y, Zheng Y, Zhang H, He X, Yang Q, Wu J (2020) A high performance and flexible in-plane asymmetric micro-supercapacitor (msc) fabricated with functional electrochemical-exfoliated graphene. J Electroanal Chem 866:114169. https://doi.org/10.1016/j.jelechem.2020.11416910.1016/j.jelechem.2020.114169 ↗
11. Liu F, Wang C, Sui X, Riaz MA, 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 ↗
12. Ma H, Shen Z (2020) Exfoliation of graphene nanosheets in aqueous media. Ceram Int 46:21873–21887. https://doi.org/10.1016/j.ceramint.2020.05.31410.1016/j.ceramint.2020.05.314 ↗
13. Sattar T (2019) Current review on synthesis, composites and multifunctional properties of graphene. Top Curr Chem 377:1–45. https://doi.org/10.1007/s41061-019-0235-610.1007/s41061-019-0235-6 ↗
14. Shi Q, Tokarska K, Ta HQ, Yang X, Liu Y, Ullah S, Liu L, Trzebicka B, Bachmatiuk A, Sun J (2020) Substrate developments for the chemical vapor deposition synthesis of graphene. Adv Mater Interfaces 7:1902024. https://doi.org/10.1002/admi.20190202410.1002/admi.201902024 ↗
15. Kauling AP, Seefeldt AT, Pisoni DP, Pradeep RC, Bentini R, Oliveira RV, Novoselov KS, Castro Neto AH (2018) The worldwide graphene flake production. Adv Mater 30:1803784. https://doi.org/10.1002/adma.20180378410.1002/adma.201803784 ↗
16. Allen MJ, Tung VC, Kaner RB (2010) Honeycomb carbon: a review of graphene. Chem Rev 110:132–145. https://doi.org/10.1021/cr900070d10.1021/cr900070d ↗
17. Chen L, Hernandez Y, Feng X, Müllen K (2012) From nanographene and graphene nanoribbons to graphene sheets: chemical synthesis. Angew Chem Int Ed 51:7640–7654. https://doi.org/10.1002/adma.20180378410.1002/adma.201803784 ↗
18. Wang X-Y, Narita A, Müllen K (2017) Precision synthesis versus bulk-scale fabrication of graphenes. Nat Rev Chem 2:1–10. https://doi.org/10.1038/s41570-017-010010.1038/s41570-017-0100 ↗
19. Liu XH, Guan CZ, Wang D, Wan LJ (2014) Graphene-like single-layered covalent organic frameworks: synthesis strategies and application prospects. Adv Mater 26:6912–6920. https://doi.org/10.1002/adma.20130531710.1002/adma.201305317 ↗
20. Dong R, Zhang T, Feng X (2018) Interface-assisted synthesis of 2d materials: trend and challenges. Chem Rev 118:6189–6235. https://doi.org/10.1021/acs.chemrev.8b0005610.1021/acs.chemrev.8b00056 ↗
21. Kumar N, Salehiyan R, Chauke V, Botlhoko OJ, Setshedi K, Scriba M, Masukume M, Ray SS (2021) Top-down synthesis of graphene: a comprehensive review. FlatChem 27:100224. https://doi.org/10.1016/j.flatc.2021.10022410.1016/j.flatc.2021.100224 ↗
22. Cheng C, Jia P, Xiao L, Geng J (2019) Tandem chemical modification/mechanical exfoliation of graphite: scalable synthesis of high-quality, surface-functionalized graphene. Carbon 145:668–676. https://doi.org/10.1016/j.carbon.2019.01.07910.1016/j.carbon.2019.01.079 ↗
23. Zhang Y, Xu Y (2019) Simultaneous electrochemical dual-electrode exfoliation of graphite toward scalable production of high-quality graphene. Adv Funct Mater. https://doi.org/10.1002/adfm.20190217110.1002/adfm.201902171 ↗
24. Yang Y, Hou H, Zou G, Shi W, Shuai H, Li J, Ji X (2018) Electrochemical exfoliation of graphene-like two-dimensional nanomaterials. Nanoscale 11:16–33. https://doi.org/10.1039/c8nr08227h10.1039/c8nr08227h ↗
25. Sahoo SK, Behera AK, Chandran R, Mallik A (2020) Industrial scale synthesis of few-layer graphene nanosheets (flgnss): an exploration of electrochemical exfoliation approach. J Appl Electrochem 50:673–688. https://doi.org/10.1007/s10800-020-01422-310.1007/s10800-020-01422-3 ↗
26. Lei Y, Ossonon BD, Chen J, Perreault J, Tavares AC (2021) Electrochemical characterization of graphene-type materials obtained by electrochemical exfoliation of graphite. J Electroanal Chem 887:115084. https://doi.org/10.1016/j.jelechem.2021.11508410.1016/j.jelechem.2021.115084 ↗
27. Najafabadi AT, Gyenge E (2015) Synergistic production of graphene microsheets by simultaneous anodic and cathodic electro-exfoliation of graphitic electrodes in aprotic ionic liquids. Carbon 84:449–459. https://doi.org/10.1016/j.carbon.2014.12.04110.1016/j.carbon.2014.12.041 ↗
28. Jeon I, Yoon B, He M, Swager TM (2018) Hyperstage graphite: electrochemical synthesis and spontaneous reactive exfoliation. Adv Mater. https://doi.org/10.1002/adma.20170453810.1002/adma.201704538 ↗
29. Chen D, Wang F, Li Y, Wang WW, Huang TX, Li JF, Novoselov KS, Tian ZQ, Zhan D (2019) Programmed electrochemical exfoliation of graphite to high quality graphene. Chem Commun 55:3379–3382. https://doi.org/10.1039/c9cc00393b10.1039/c9cc00393b ↗
30. Zhang Y, Xu Y, Liu R (2021) Regulating cations and solvents of the electrolyte for ultra-efficient electrochemical production of high-quality graphene. Carbon 176:157–167. https://doi.org/10.1016/j.carbon.2021.01.10910.1016/j.carbon.2021.01.109 ↗
31. Zhang P, He P, Yu Q, Wang G, Huang T, Yang S, Liu Z, Xie X, Ding G (2022) Delocalized electrochemical exfoliation toward high-throughput fabrication of high-quality graphene. Chem Eng J 428:131122. https://doi.org/10.1016/j.cej.2021.13112210.1016/j.cej.2021.131122 ↗
32. Phiri J, Gane P, Maloney TC (2017) General overview of graphene: production, properties and application in polymer composites. Mater Sci Eng, B 215:9–28. https://doi.org/10.1016/j.mseb.2016.10.00410.1016/j.mseb.2016.10.004 ↗
33. Backes C, Higgins TM, Kelly A, Boland C, Harvey A, Hanlon D, Coleman JN (2017) Guidelines for exfoliation, characterization and processing of layered materials produced by liquid exfoliation. Chem Mater 29:243–255. https://doi.org/10.1021/acs.chemmater.6b0333510.1021/acs.chemmater.6b03335 ↗
34. Qiu Z, Liu Z, Miao J, Zheng F, Jiang J, Li Y, Wu Q, Huang Y, Wang H, Li Q (2023) Scalable production of electrochemically exfoliated graphene by an extensible electrochemical reactor with encapsulated anode and dual cathodes. Appl Surf Sci 608:155211. https://doi.org/10.1016/j.apsusc.2022.15521110.1016/j.apsusc.2022.155211 ↗
35. Abdelkader AM, Cooper AJ, Dryfe RAW, Kinloch IA (2015) How to get between the sheets: a review of recent works on the electrochemical exfoliation of graphene materials from bulk graphite. Nanoscale 7:6944–6956. https://doi.org/10.1039/c4nr06942k10.1039/c4nr06942k ↗
36. Liu J, Poh CK, Zhan D, Lai L, Lim SH, Wang L, Liu X, Sahoo NG, Li C, Shen Z, Lin J (2013) Improved synthesis of graphene flakes from the multiple electrochemical exfoliation of graphite rod. Nano Energy 2:377–386. https://doi.org/10.1016/j.nanoen.2012.11.00310.1016/j.nanoen.2012.11.003 ↗
37. Coroş M, Pogăcean F, Roşu M-C, Socaci C, Borodi G, Mageruşan L, Biriş AR, Pruneanu S (2016) Simple and cost-effective synthesis of graphene by electrochemical exfoliation of graphite rods. RSC Adv 6:2651–2661. https://doi.org/10.1039/c5ra19277c10.1039/c5ra19277c ↗
38. Munuera JM, Paredes JI, Villar Rodil S, Ayán Varela M, Pagán A, Aznar Cervantes SD, Cenis JL, Martínez Alonso A, Tascón JMD (2015) High quality, low oxygen content and biocompatible graphene nanosheets obtained by anodic exfoliation of different graphite types. Carbon 94:729–739. https://doi.org/10.1016/j.carbon.2015.07.05310.1016/j.carbon.2015.07.053 ↗
39. Chuang C-H, Su C-Y, Hsu K-T, Chen C-H, Huang C-H, Chu C-W, Liu W-R (2015) A green, simple and cost-effective approach to synthesize high quality graphene by electrochemical exfoliation via process optimization. RSC Adv 5:54762–54768. https://doi.org/10.1039/c5ra07710a10.1039/c5ra07710a ↗
40. Parvez K, Wu ZS, Li R, Liu X, Graf R, Feng X, Muellen 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 ↗
41. Parviz D, Irin F, Shah SA, Das S, Sweeney CB, Green MJ (2016) Challenges in liquid-phase exfoliation, processing, and assembly of pristine graphene. Adv Mater 28:8796–8818. https://doi.org/10.1002/adma.20160188910.1002/adma.201601889 ↗
42. Chen J, Perez-Page M, Ji Z, Zhang Z, Guo Z, Holmes S (2021) One step electrochemical exfoliation of natural graphite flakes into graphene oxide for polybenzimidazole composite membranes giving enhanced performance in high temperature fuel cells. J Power Sources. https://doi.org/10.1016/j.jpowsour.2021.22955010.1016/j.jpowsour.2021.229550 ↗
43. Achee TC, Sun W, Hope JT, Quitzau SG, Sweeney CB, Shah SA, Habib T, Green MJ (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 ↗
44. Lee H, Choi JI, Park J, Jang SS, Lee SW (2020) Role of anions on electrochemical exfoliation of graphite into graphene in aqueous acids. Carbon 167:816–825. https://doi.org/10.1016/j.carbon.2020.06.04410.1016/j.carbon.2020.06.044 ↗
45. Abdollahifar M, Doose S, Cavers H, Kwade A (2022) Graphite recycling from end-of-life lithium-ion batteries: processes and applications. Mater Technol, Adv. https://doi.org/10.1002/admt.20220036810.1002/admt.202200368 ↗
46. Niu B, Xiao J, Xu Z (2022) Advances and challenges in anode graphite recycling from spent lithium-ion batteries. J Hazard Mater 439:129678. https://doi.org/10.1016/j.jhazmat.2022.12967810.1016/j.jhazmat.2022.129678 ↗
47. Natarajan S, Divya ML, Aravindan V (2022) Should we recycle the graphite from spent lithium-ion batteries? The untold story of graphite with the importance of recycling. J Energy Chem 71:351–369. https://doi.org/10.1016/j.jechem.2022.04.01210.1016/j.jechem.2022.04.012 ↗
48. Liu J, Shi H, Hu X, Geng Y, Yang L, Shao P, Luo X (2021) Critical strategies for recycling process of graphite from spent lithium-ion batteries: a review. Sci Total Environ 816:151621. https://doi.org/10.1016/j.scitotenv.2021.15162110.1016/j.scitotenv.2021.151621 ↗
49. Hashimoto H, Muramatsu Y, Nishina Y, Asoh H (2019) Bipolar anodic electrochemical exfoliation of graphite powders. Electrochem Commun. https://doi.org/10.1016/j.elecom.2019.06.00110.1016/j.elecom.2019.06.001 ↗
50. Mei J, Qiu Z, Gao T, Wu Q, Zheng F, Jiang J, Liu K, Huang Y, Wang H, Li Q (2023) Insights into the conductive network of electrochemical exfoliation with graphite powder as starting raw material for graphene production. Langmuir. https://doi.org/10.1021/acs.langmuir.3c0004610.1021/acs.langmuir.3c00046 ↗
51. Paredes JI, Munuera JM (2017) Recent advances and energy-related applications of high quality/chemically doped graphenes obtained by electrochemical exfoliation methods. J Mater Chem A 5:7228–7242. https://doi.org/10.1039/c7ta01711a10.1039/c7ta01711a ↗
52. Munuera JM, Paredes JI, Villar-Rodil S, Castro-Muñiz A, Martínez-Alonso A, Tascón JMD (2018) High quality, low-oxidized graphene via anodic exfoliation with table salt as an efficient oxidation-preventing co-electrolyte for water/oil remediation and capacitive energy storage applications. Appl Mater Today 11:246–254. https://doi.org/10.1016/j.apmt.2018.03.00210.1016/j.apmt.2018.03.002 ↗
53. Kumar MKP, Srivastava C (2016) Synthesis of graphene from a used battery electrode. JOM 68:383. https://doi.org/10.1007/s11837-015-1657-410.1007/s11837-015-1657-4 ↗