Synthesis of mesoporous carbon materials from renewable plant polyphenols for environmental and energy applications
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摘要: 介孔炭材料具有高比表面积、可调的组成和孔结构、良好的化学稳定性和导电性，被广泛用于环境、催化、能源等领域。碳源是介孔炭合成的关键。植物多酚，作为一种生物质碳源，具有低价、无毒、可再生的优点。且植物多酚具有黏附性和金属络合能力，被广泛用于合成介孔炭复合材料。尽管该领域已取得巨大进展，但关于植物多酚衍生介孔炭的综述还很少。本文综述了以植物多酚为原料制备的各种介孔炭材料，包括多孔炭泡沫、有序介孔炭、介孔炭球、杂原子掺杂炭和金属/介孔炭复合材料。总结了上述炭材料在环境和能源等领域的应用。该综述将为植物多酚化学和纳米多孔炭材料的研究建立桥梁，促进更多的研究者利用植物多酚作为碳源制备功能介孔炭材料。Abstract: Mesoporous carbon materials have a high specific surface area, tunable surface chemistry and pore structure, and good chemical stability and conductivity. They have attracted great attention for use in environmental remediation, industrial catalysis, energy conversion and storage. The carbon precursor is important for the synthesis of mesoporous carbons with different properties. Plant polyphenols are a kind of universal biomass with low cost, nontoxicity and sustainability that can be used as a carbon source. Most importantly, their good adhesion and metal chelating ability make them suitable for the synthesis of mesoporous carbon composites. Methods for the synthesis of different forms of mesoporous carbon from plant polyphenols are provided, including porous carbon foams, ordered mesoporous carbons, mesoporous carbon spheres, heteroatom-doped mesoporous carbons, and composites of mesoporous carbon with metals. Their uses in environmental and energy studies are summarized.
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Key words:
- Plant polyphenol /
- Mesoporous carbon /
- Adsorption /
- Catalysis /
- Energy storage
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Figure 2. Mesoporous carbon materials derived from plant polyphenols and their applications.
Figure 3. (a) The synthesis of tannin-based carbon foam. (b) SEM images of tannin-based carbon foam with low magnification. (c) SEM images of tannin-based carbon foam with high magnification (Reproduced with permission, Copyright 2009, Elsevier)[83].
Figure 4. (a) Synthesis of ordered mesoporous carbon materials. (b) TEM images of ordered mesoporous carbon materials. (c) N2 adsorption-desorption isotherms of different mesoporous carbon samples pyrolyzed at three temperatures (Reproduced with permission, Copyright 2016, Royal Society of Chemistry)[72].
Figure 5. (a) Synthesis of ordered mesoporous carbon material. (b) TEM images of OMC@F1270.8-800 sample (ratio of tannins and Pluronic F127 of 0.8, pyrolysis temperature of 800 °C). (c) TEM images of Ni-OMC@F1270.8-600 (ratio of tannins and F127 of 0.8, pyrolysis temperature of 600 °C) (Reproduced with permission, Copyright 2016, Nature)[40].
Figure 6. (a) Synthesis of RF resin spheres via the extended Stöber method. (b) TEM images of carbon spheres carbonized by the RF colloidal spheres. (c) Dynamic light scattering plot of carbon spheres carbonized by the RF colloidal spheres (Reproduced with permission, Copyright 2011, WILEY)[34].
Figure 7. (a) Synthesis of Co-TA crystals derived Co/N-doped carbon. (b) SEM images of Co/N-doped carbon (Reproduced with permission, Copyright 2016, WILEY)[38]. (c) Synthesis of zinc-ellagic acid mesocrystals and derived hierarchically porous carbon. (d) SEM image of EAZn2_2d_C carbon ( molar ratio for EA/Zn of 1∶2) (Reproduced with permission, Copyright 2015, American Chemical Society)[41].
Figure 8. (a) Synthesis of metal-phenolic coordination spheres. (b) SEM image of CoII-FeIII-TA spheres. (c) The coordination units of metal-TA with different kinds metal ions. (d) Reaction for the metal-TA coordination under acid conditions and the possible covalent connection for the Co-TA sphere after hydrothermal treatment (Reproduced with permission, Copyright 2018, WILEY)[39].
Figure 9. (a) Snthesis of nanoporous carbon spheres carbonized from zinc-phenolic coordination polymers. (b) TEM image for Zn-TA-40% carbonized at 900 °C. (c) TEM image for Zn-TA-40% carbonized at 900 °C under high magnification. (d) N2 sorption isotherms for Zn-TA-40%-900, Zn-TA-50%-900 and Zn-TA-60%-900, respectively (Reproduced with permission, Copyright 2019, Elsevier)[62].
Figure 10. (a) Synthesis of magnetic mesoporous carbon nanospheres. (b) TEM image of magnetic mesoporous carbon nanospheres. (c) STEM and elemental mapping of magnetic mesoporous carbon nanospheres (Reproduced with permission, Copyright 2021, Elsevier)[53].
Figure 11. (a) Synthesis of PSTA-Co-1000 hollow carbon nanospheres. (b) TEM image of PSTA-Co-1000 nanospheres. (c) HAADF-STEM image of PSTA-Co-1000. Single cobalt atoms were marked with red circles (Reproduced with permission, Copyright 2020, WILEY)[42].
Figure 12. (a) Procedures for the preparation of iron carbide/Fe-N-carbon catalysts. (b) Optical photograph and SEM image of FP-Fe-TA-N-850 (Fe-TA coating on filter paper and carbonized at 850 °C). (c) TEM images of FP-Fe-TA-N-850. (d) N2 sorption isotherms for FP-Fe-TA-N-850 and FP-Fe-N-850 (Reproduced with permission, Copyright 2016, Wiley)[37].
Figure 13. (a) Synthesis of N, S co-doped porous carbon with Fe single atom nanoclusters (named N, S co-doped CPANI-TA-Fe Fe-SA-NC catalysts). (b) Cnnection of PANI and TA-Fe3+ in the 3D hydrogel. (c) N, S co-doped porous carbon inlaid with Fe-SA-NCs. (d) SEM image of N, S co-doped CPANI-TA-Fe Fe-SA-NC catalysts. (e) Low magnification TEM of N, S co-doped CPANI-TA-Fe Fe-SA-NC catalysts. (f) High magnification TEM of N, S co-doped CPANI-TA-Fe Fe-SA-NC catalysts (Reproduced with permission, Copyright 2020, Royal Society of Chemistry)[110].
Figure 14. (a) Ultraviolet and visible spectrophotometry of Rhodamine B (RhB) solutions with various products (inset is an optical photograph of Rhodamine B) (Reproduced with permission, Copyright 2015, American Chemical Society)[41]. (b) CO2 and N2 adsorption isotherms for tannin-based carbon with the Toth model (Reproduced with permission, Copyright 2020, Elsevier)[52]. (c) Adsorption kinetic plots of magnetic mesoporous carbon nanospheres. (d) Selectivity of adsorption capacity (Reproduced with permission, Copyright 2021, Elsevier)[53].
Figure 15. (a) LSV of commercial Pt/C, CoTA-700, Co-TA-800, Co-TA-900 and Fe-TA-800 for ORR. (b) LSV curves of Co-TA-800 under different rotating speeds. (c) Electron transfer numbers of Co-TA-800 (inset is the corresponding K-L plots). (d) LSV curves of Co-TA-800 for OER (inset is the corresponding Tafel plots). (Reproduced with permission, Copyright 2016, Wiley)[38].
Figure 16. Selective hydrogenation of alkene by Ni-based catalysts (Reproduced with permission, Copyright 2016, Nature)[40].
Figure 17. (a) Mechanism of BPA removal by Cu-Fe oxides loaded mesoporous carbon framework. (b) Removal of BPA by different catalysts. (c) Different dosages of Cu-Fe-TA-400 to BPA degradation (Reproduced with permission, Copyright 2021, Elsevier)[115].
Figure 18. (a) High electrochemical performance of highly N-, O-doped carbons. (b) Ragone plot calculated in the current density interval of 0.1-12 A g−1 with a two-electrode system in 1 mol L−1 H2SO4 electrolyte. (c) Cycling stability determined from galvanostatic charge-discharge tests at 0.5 A g−1 until 5000 cycles. (d) Nyquist plot of highly N-, O-doped carbons. (e) Frequency response plot of highly N-, O-doped carbons (Reproduced with permission, Copyright 2017, Royal Society of Chemistry)[57].
Table 1. Mesoporous carbon materials derived from plant polyphenols.
Samples Synthesis
methodMorphology Component
(except
carbon)Specific
surface
area (m2 g−1)Pore
size
(nm)Type of
plant
polyphenolApplication Refs. FP-Fe-TA-N-850 Coating method - Fe-N-C 16 - Tannic acid Catalysts for oxygen-reduction reaction [37] Co-TA-800 Direct carbonization of mesocrystals A core-shell Co@C structure Co-N-C 180 4.8 Tannic acid Catalyst for the oxygen reduction and evolution reactions [38] Co-Fe-TA-C800 Direct carbonization of mesocrystals - Fe-Co-N-C 449 4.8 Tannic acid Catalysts for oxygen-reduction reaction [39] Ni-OMC Solid-state synthesis Hexagonal cylindrical structures Ni 1057 7.8 - The selective hydrogenation of large biomolecules [40] EAZn2_7d Direct carbonization of mesocrystals Hierarchically porous carbon particles Zn 842 4 Ellagic acid CO2 and Rhodamine B adsorption [41] PSTA-Co-1000 Directly pyrolyzed to afford mesoporous hollow carbon nanospheres Nanospheres Co-N-P 411.60 0.7 Tannic acid Catalysts for the oxygen reduction reaction [42] Pd@MC catalysts Soft templating strategy Worm-like Pd 330 12 Wattle tannin Catalyst for ligand-free Suzuki-Miyaura couplings [47] Co@OMC Solid-state synthesis Hexagonal cylindrical structures Co 700 4.4 Mimosa tannin all-in-one deoxygenation of ketone into alkylbenzene [48] CP-Fe-N Coating method A random pore structure Fe-N - - Tannic acid Highly reactive Fenton-like catalysts [49] N0.8A80F50 Soft templating strategy Worm-like N 315 16.3 Chestnut tannin CO2 adsorption [50] TG-C700-4K Soft templating strategy Irregularly-shaped particles of various sizes K 1192 - Mimosa tannin CO2 adsorption [51] MC-Tyrosine-0.1 A mechanochemical assembly through coordination polymerization - N 657 0.76 - CO2 adsorption and high capacity for light hydrocarbon and priority for alkyne molecule [52] Magnetic mesoporous carbon nanospheres Direct carbonization of mesocrystals Nanospheres Fe 512.2 6.7 Tannic acid Cr(VI) adsorption [53] PNDC-2 Microwave method Similar graphitic flakes N-P 479 3.29 - Supercapacitor [54] SiPDC-2 Microwave method Irregular rock like structures Si-P 641.51 20.17 Quebracho tannin Supercapacitor [55] X11 Hydrothermally treated Typical granular structure of carbon gels N 102 3.84 Mimosa tannin Supercapacitor [56] TW Hydrothermal carbonisation Quasi-spherical particles N-O 729 - Pine tannin Supercapacitor [57] GaC Hard-templating route Hexagonal cylindrical structures O 1045 9.16 Gallic acid Supercapacitor [58] CT2P0W0_60 Solid-state synthesis Hexagonal cylindrical structures - 829 - Mimosa tannin CO2 adsorption and supercapacitor [59] C3/30 Soft templating strategy Hexagonal cylindrical structures - 1152 11.93 Mimosa tannin Supercapacitor [60] A120-CTPW Solid-state synthesis Hexagonal cylindrical structures - 1215 1.6 Mimosa tannin Supercapacitor [61] Zn-TA-40%-900 Direct carbonization of mesocrystals Nanoporous carbons spheres Zn 2221 5.3 Tannic acid Biosensor [62] DM2C Solid-state synthesis A thick and homogeneous layer - 382 0.65 Mimosa tannin Biosensor [63] A1-C Pyrolysis Particles - 420 9.6 Wattle tannin - [64] SFG6 Solid-state synthesis Carbon foams - - - Mimosa tannin Seasonal thermal storage applications [65] TBC-K3.6 Pyrolysis Disordered structure K 2554 1.26 Pine tannin Supercapacitor [66] CH0S100T180_u Hydrothermal conditions Spherical particles - 904 - Mimosa tannin Supercapacitor [67] Tannin-based carbon xerogels Sol gel method Cluster S - - Wattle tannin - [68] CH-AT1 Hydrothermal carbonization Carbon gel structure N 547 - Mimosa tannin Supercapacitor [69] CH100T180_4Ag Hydrothermal carbonization Microspheres Ag 618 - Mimosa tannin - [70] CH-EAT Hydrothermal carbonization Spherical particles N 400 - Mimosa tannin - [71] PTW_2_900°C Pyrolysis - - 718 5.8 Mimosa tannin - [72] ASFT5.5 Sol gel method Filamentous structure - 407 30 Wattle tannin The insulating properties [73] IS2M-1-400 A self-assembly approach Hexagonal cylindrical structures - 534 9.4 Wattle tannin - [74] Carbon meringues Whipping Foams - 400 - Mimosa tannin Thermal insulators [75] CarboHIPE Emulsion-templating Spherical - 400 - Mimosa tannin Thermal insulators [76] OMC Surfactant-water-assisted mechanochemical mesostructuration Hexagonal cylindrical structures - 487 6 Mimosa tannin The selective separation of di-branched C6 isomers [77] NCM Hydrothermal carbonization Spherical particles N 500 - Wattle tannin - [78] OMC Soft templating strategy Hexagonal cylindrical structures - 792 0.6 Mimosa tannin Tetracycline (TC) adsorption [79] CFAT-C - - - 723 0.7 - Catalysts for oxygen-reduction reaction [80] 
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