A review of biomass-derived graphene and graphene-like carbons for electrochemical energy storage and conversion
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摘要: 石墨烯和类石墨烯炭材料（G炭）具有高比表面积、优异的导电性和导热性等性质，很多原料可以被用来制备石墨烯和类石墨烯炭材料。该文介绍了近年来多种自然资源作为碳前体合成高质量G炭的方法，包括高温处理、基底上生长、模板辅助合成、无模板的自生催化、g-C3N4衍生、等离子体辅助合成、激光诱导等，分析了生物质合成石墨烯量子点的特点，讨论了G炭在电化学储存与转化、灵敏传感器等领域中的应用。这篇综述将有助于研究人员理解生物质高效利用并制备G炭，有利于大规模工业化生产的研究。Abstract: Graphene and graphene-like carbons (G-carbons) have many excellent properties, such as a high specific surface area, and good electrical and thermal conductivities. Recent advances in the synthesis of large amounts of G-carbons from biomass are discussed, including the types of biomass materials used as the precursors and the various synthesis routes. The latter include high-temperature graphitization, growth on substrates, template-assisted synthesis, template-free catalysis, a g-C3N4-derived approach, plasma-assisted synthesis, and laser-induced synthesis. The uses of G-carbons in electrochemical energy storage and conversion, and sensing are also discussed.
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Key words:
- Graphene /
- Graphene-like carbon /
- G-carbon /
- Sustainable biomass /
- Electrochemical energy storage and conversion
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Figure 2. (a) XRD spectra of pyrolyzed chitosan beads used as a graphene precursor, (b) Raman spectrum of exfoliated pyrolyzed chitosan beads after exfoliation and spin casting on a glass substrate, (c) SEM image of pyrolyzed chitosan beads and (d) TEM image of the graphene-based residue deposited from an aqueous suspension[52]. Reprinted with permission.
Figure 3. (a) Preparation of phosphorus-doped graphene (PDG), (b) Raman spectrum of PDG-2 recorded using a 514-nm excitation wavelength, (c) comparison of the ultraviolet–visible spectra of graphene products and (d) TEM image of PDG-2[55]. Reprinted with permission.
Figure 4. (a) Schematic of graphene synthesis from leaves, (b) corresponding Raman spectrum and (c) Raman shifts after modification via π–π interactions.[61]. Reprinted with permission.
Figure 5. Raman spectra of the following: (a) Hydrothermal carbon, 500–1500 /cm and (b) Coconut, 500–1500 /cm[64]. Reprinted with permission.
Figure 7. (a) Schematic of graphene synthesis, supported on a fibrous clay sepiolite, from natural resources, as follows from (b) sucrose and (c) gelatin[44]. Reprinted with permission.
Figure 8. (a) Formation of porous graphic carbon sheets from cornstalks, (b) XRD patterns for samples derived from a cornstalk-[Fe(CN)6]4− composite, synthesized over a carbonization temperature range of 700 °C to 1100 °C, (c) Raman spectra for the porous graphic carbon sheet samples synthesized under various conditions, labeled in accordance with the catalyst concentration and carbonization temperature, (d) TEM image of the overall structure of the porous graphic carbon sheet samples and (e) TEM image of the enlarged structures of the selected area[95]. Reprinted with permission.
Figure 9. (a) General synthetic route to lower symmetric HBCs[101], (b) preparation of porous flake-like carbon/Fe3O4 composites from chitosan[105], (c) XRD patterns for graphene-like carbons from glucose[104], (d) Raman spectra for graphene-like carbons from glucose[104], (e) XRD patterns of porous graphene NS-3 materials[106] and (f) Raman spectrum of a porous graphene NS-3-900 material[106]. Reprinted with permission.
Figure 10. (a) Proposed synthetic protocol for free-standing graphene (Bottom: Repetition motifs of an ideal g-C3N4 plane (middle) and of graphene (right); C, black or gray; N, blue) and (b) synthesis of N-graphene sheets grafted to a carbon fiber from the mixture of urea and cotton[114]. Reprinted with permission.
Figure 11. (a) Schematic for converting cheese precursors into vertical graphene NSs[120], (b) typical SEM image from a processed cheese precursor, (c) typical SEM image from a cream cheese precursor, (d) Raman spectrum of the product formed from a processed cheese precursor and (e) Raman spectrum of the product formed from a cream cheese precursor. Reprinted with permission.
Figure 12. (a) In-house plasma reactor system employed for graphene growth, (b) proposed graphene growth pathway under plasma: (i) C—O, C＝O, and C—H bonds breaks due to thermal energy, (ii) H atoms generated by plasma adsorb on the Cu substrate, etch the surface, and reduce more stable C—O and C＝O bonds, whereas Ar atoms act as carriers, (iii) carbon atoms form nucleation islands on the substrate surface and migrate on the surface, (iv) graphene layer formed by the bond between the nucleation islands, whereas the excess carbon atoms start forming another layer on top and (v) the top layers etch, attributable to the hydrogen atoms generated by the plasma, to form a single-layered graphene at long plasma exposure times, (c) TEM image of graphene under plasma treatment for 30 min and (d) ratio of ID/IG and ID/I2G under various plasma treatment times[124]. Reprinted with permission.
Figure 14. (a) TEM image of RH-graphene QDs, (b) higher magnification image of the type shown in part (a), (c) atomic force micrograph and height profiles of RH-GQDs synthesized at 200 °C and (d) SEM micrograph of RH-GQDs[46]. Reprinted with permission.
Table 1. Summary of graphene synthesized at high temperatures.
Biomass materials Products ID/IG Ref. Wood char powders Graphene - [43] Biochar materials from woods Graphene - [48] Chitosan NDG 1/1.15 [52] Chitosan NDG - [53] Alginate Graphene 1/1.13 [54] Alginate PDG - [55] Alginate BDG - [56] Alginate CeOx/G - [57] Wheat straw Graphene 1/1.37 [45] Soybean shells NDG 1.13 [58] Silk cocoons NDG 0.87 [59] Camphor leaves Graphene 0.99 [61] Coconut coir dust Graphene - [64] Oil palm empty fruit bunches Graphene 1/1.25 [60] Cucumbers Graphene 1.07 [65] 
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Table 2. Summary of graphene grown on various substrates.
Biomass materials Products ID/IG I2D/IG Ref. Cookies Graphene - - [71] Chocolate Graphene - - [71] Grass Graphene - - [71] Plastic Graphene - - [71] Dog feces Graphene - - [71] Roaches Graphene - - [71] Chicken fat Graphene - 3.0 [72] Soybean oil Graphene 1.50 [73] Sodium alginate Graphene - - [76] Alginate and chitosan BNG - - [77] Rice husk ash Graphene 1.34 - [78] Sucrose Graphene - - [83] Chitosan NDG - - [84]
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Table 3. Summary of template-assisted graphene growth.
Biomass materials Products ID/IG Ref. Sucrose Graphene - [44] Gelatin Graphene 1/1.2 [44] Rice Graphene - [88] Seaweed Magnetic graphene 1.00 [89] Shrimp shells Graphene-like carbon 1/1.06 [86] Larch wood chips Graphene-like carbon 0.9 [87] Salvai splendens petals GPCNs 1.13 [90] Clover precursor Graphene-like carbon - [91] CMCC-Na JS-CK2NS 0.93 [92] Cornstalk Graphene-like carbon - [93]
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Table 4. Summary of graphene synthesized by self-generating, template-free catalysis.
Biomass materials Products ID/IG Ref. Cornstalk Graphitic carbon 1/1.6 [95] Milk powder Graphene - [98] Bamboo Graphene-like carbon 0.62 [99] Disposable paper cups Graphene - [100] Seven kinds of biomass feedstocks GO, rGO - [103] Glucose Graphene-like carbon - [104] Coconut shells Graphene-like carbon 1/3.98 [106] Chitosan Magnetic graphene-like carbon - [105] Peanut shell Graphene-like nanosheets 1.01 [107] Ginger root Graphene-like carbon - [108]
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Table 6. Summary of plasma-assisted graphene synthesis.
Biomass materials Products ID/IG I2D/IG Ref. Processed cheese Graphene 0.7 1.2 [120] Cream cheese Graphene 1.4 0.95 [120] Butter Graphene 1.1 - [122] Honey Graphene 0.45 0.59 [123] Table sugar Graphene 0.7 0.47 [123] Butter Graphene 0.6 0.6 [123] Condensed milk Graphene 0.51 0.55 [123] Methane Graphene 0.71 0.49 [123] Mango peels Graphene 0.7–2.8 0.4–2.78 [124]
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