Magnetic motive, ordered mesoporous carbons with partially graphitized framework and controllable surface wettability: preparation, characterization and their selective adsorption of organic pollutants in water

Abstract

Magnetically active, ordered and stable mesoporous carbons with partially graphitized networks and controllable surface wettability (PR-Fe-P123-800 and PR-Ni-P123-800) have been synthesized through direct carbonization of Fe or Ni functionalized, and ordered mesoporous polymers at 800°C, which could be synthesized from self assembly of resol (phenol/formaldehyde) with block copolymer template (P123) in presence of Fe³⁺ or Ni²⁺, and hydrothermal treatment at 200°C. PR-Fe-P123-800 and PR-Ni-P123-800 possess ordered and uniform mesopores, large BET surface areas, good stabilities, controllable surface wettability and partially graphitized framework. The above structural characteristics result in their enhanced selective adsorption property and good reusability for organic pollutants such as RhB, p-nitrophenol and n-heptane in water, which could be easily regenerated through separation under constant magnetic fields and washing with ethanol solvent. The unique magnetically active and adsorptive property found in PR-Fe-P123-800 and PR-Ni-P123-800 will be very important for them to be used as efficient absorbents for removal of various organic pollutants in water.

Keywords

magnetic separation / mesoporous carbon / graphitization / adsorption / high temperature synthesis

References

[1] Ryoo R, Joo S H, Jun S. Synthesis of highly ordered carbon molecular sieves via template-mediated structural transformation. Journal of Physical Chemistry B, 1999, 103(37): 7743–7746

[2] Wickramaratne N P, Perera V S, Park B W, . Graphitic mesoporous carbons with embedded prussian blue-derived iron oxide nanoparticles synthesized by soft templating and low-temperature graphitization. Chemistry of Materials, 2013, 25(14): 2803–2811

[3] Zhai Y, Dou Y, Zhao D, . Carbon materials for chemical capacitive energy storage. Advanced Materials, 2011, 23(42): 4828–4850

[4] Meng Y, Gu D, Zhang F Q, . Ordered mesoporous polymers and homologous carbon frameworks: amphiphilic surfactant templating and direct transformation. Angewandte Chemie International Edition, 2005, 44(43): 7053–7059

[5] Almeida V C, Silva R, Acerce M, . N-doped ordered mesoporous carbons with improved charge storage capacity by tailoring N-dopant density with solvent-assisted synthesis. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2014, 2(36): 15181–15190

[6] Liang C, Dai S. Synthesis of mesoporous carbon materials via enhanced hydrogen-bonding interaction. Journal of the American Chemical Society, 2006, 128(16): 5316–5317

[7] Liu F J, Li C J, Ren L M, . High-temperature synthesis of stable and ordered mesoporous polymer monoliths with low dielectric constants. Journal of Materials Chemistry, 2009, 19(42): 7921–7928

[8] Wang X, Liang C, Dai S. Facile synthesis of ordered mesoporous carbons with high thermal stability by self-assembly of resorcinol-formaldehyde and block copolymers under highly acidic conditions. Langmuir, 2008, 24(14): 7500–7505

[9] Lee K T, Ji X L, Rault M, . Simple synthesis of graphitic ordered mesoporous carbon materials by a solid-state method using metal phthalocyanines. Angewandte Chemie International Edition, 2009, 48(31): 5661–5665

[10] Su P, Jiang L, Zhao J, . Mesoporous graphitic carbon nanodisks fabricated via catalytic carbonization of coordination polymers. Chemical Communications, 2012, 48(70): 8769–8771

[11] Kim J, Lee J, Choi Y, . Synthesis of hierarchical linearly assembled graphitic carbon nanoparticles via catalytic graphitization in SBA-15. Carbon, 2014, 75(8): 95–103

[12] Jensen M P, Mehn M P, Que L. Intramolecular aromatic amination through iron-mediated nitrene transfer. Angewandte Chemie International Edition, 2003, 42(36): 4357–4360

[13] Wu Z, Li W, Webley P A, . General and controllable synthesis of novel mesoporous magnetic iron oxide@carbon encapsulates for efficient arsenic removal. Advanced Materials, 2012, 24(4): 485–491

[14] Inagaki S, Yokoo Y, Miki T, . Improvement of electric double-layer capacitance of ordered mesoporous carbon CMK-3 by partial graphitization using metal oxide catalysts. Microporous and Mesoporous Materials, 2013, 179(10): 136–143

[15] Sun Z H, Wang L F, Liu P P, . Magnetically motive porous sphere composite and its excellent properties for the removal of pollutants in water by adsorption and desorption cycles. Advanced Materials, 2006, 18(15): 1968–1971

[16] Thompson E, Danks A E, Bourgeois L, . Iron-catalyzed graphitization of biomass. Green Chemistry, 2015, 17(1): 551–556

[17] Gao W J, Wan Y, Dou Y Q, . Synthesis of partially graphitic ordered mesoporous carbons with high surface areas. Advanced Energy Materials, 2011, 1(1): 115–123

[18] Sevilla M, Fuertes A B. Fabrication of porous carbon monoliths with a graphitic framework. Carbon, 2013, 56(6): 155–166

[19] Karthik M, Faik A, Doppiu S, . A simple approach for fabrication of interconnected graphitized macroporous carbon foam with uniform mesopore walls by using hydrothermal method. Carbon, 2015, 87: 434–443

[20] Yao J Y, Li L X, Song H H, . Synthesis of magnetically separable ordered mesoporous carbons from F127/[Ni(H₂O)₆](NO₃)₂/resorcinol-formaldehyde composites. Carbon, 2009, 47(2): 436–444

[21] Liu F J, Zhang H, Zhu L F, . High-temperature hydrothermal synthesis of magnetically active, ordered mesoporous resin and carbon monoliths with reusable adsorption for organic dye. Adsorption, 2013, 19(1): 39–47

[22] Wu Z X, Li W, Xia Y Y, . Ordered mesoporous graphitized pyrolytic carbon materials: synthesis, graphitization, and electrochemical properties. Journal of Materials Chemistry, 2012, 22(18): 8835–8845

[23] Lu A H, Salabas E L, Schüth F. Magnetic nanoparticles: synthesis, protection, functionalization, and application. Angewandte Chemie International Edition, 2007, 46(8): 1222–1244

[24] Lu A H, Li W C, Kiefer A, . Fabrication of magnetically separable mesostructured silica with an open pore system. Journal of the American Chemical Society, 2004, 126(28): 8616–8617

[25] Lu A H, Schmidt W, Matoussevitch N, . Nanoengineering of a magnetically separable hydrogenation catalyst. Angewandte Chemie International Edition, 2004, 43(33): 4303–4306

[26] Fuertes A B, Sevilla M, Álvarez S, . Templated synthesis of mesoporous superparamagnetic polymers. Advanced Functional Materials, 2007, 17(14): 2321–2327

[27] Liu F J, Kong W P, Qi C Z, . Design and synthesis of mesoporous polymer-based solid acid catalysts with excellent hydrophobicity and extraordinary catalytic activity. ACS Catalysis, 2012, 2(4): 565–572

[28] Liu F, Wang L, Sun Q, . Transesterification catalyzed by ionic liquids on superhydrophobic mesoporous polymers: heterogeneous catalysts that are faster than homogeneous catalysts. Journal of the American Chemical Society, 2012, 134(41): 16948–16950

[29] Liu F J, Feng G F, Lin M Y, . Superoleophilic nanoporous polymeric ionic liquids loaded with palladium acetate: Reactants enrichment and efficient heterogeneous catalysts for Suzuki–Miyaura coupling reaction. Journal of Colloid and Interface Science, 2014, 435: 83–90

[30] Liu F, Li W, Sun Q, . Transesterification to biodiesel with superhydrophobic porous solid base catalysts. ChemSusChem, 2011, 4(8): 1059–1062

Acknowledgements

This work was supported by the Foundation of Science Technology Department of Zhejiang Province (Grant No. 2013C31030), the Natural Science Foundation of Zhejiang Province (LY15B030002), and the Foundation of Shaoxing University (Grant No. 20145018).

RIGHTS & PERMISSIONS

2014 Higher Education Press and Springer-Verlag Berlin Heidelberg