Preparation of graphene-MoS2 hybrid aerogels as multifunctional sorbents for water remediation

基于石墨烯-二硫化钼复合气凝胶的多功能吸附材料的制备及其在水污染处理方面的应用

Abstract

The increasing demand of clean water and effective way to recycle industrial wastewater has offered a new application for carbon-based three-dimensional (3D) porous networks as sorbents due to their superior sorption abilities. Through the surface modification and hybridization with functional materials, the physical and chemical properties of the 3D carbon-based materials can be engineered. In this work, graphene-MoS2 aerogels (GMAs) with bulky shape are synthesized via a one-pot hydrothermal method. The obtained GMAs show quick sorption rate and high sorption capacity towards a wide variety of contaminants. The sorption covers not only organic solvents or organic dyes, but also toxic heavy metals ions such as Hg2+ and Pb2+. More importantly, the sorption capacity towards metal ions can be optimized by simply changing the loading amount of MoS2.

摘要

三维碳基多孔材料因其独特的结掏和超高的吸附性能, 已成为最有水污染处理应用前景的吸附材料之一. 本文通过有效的调控, 合成了多种具有不同孔道结掏和成分组成的石墨烯-二硫化钼复合气凝胶材料. 这种材料在吸附重金属离子, 有机染料, 油及有机溶剂方面都有很多优异的表现. 通过调控二硫化钼的比例, 可以有效改善材料的吸附性能. 得益于此, 其吸附重金属汞离子的效率可以达到 1245mg g−1.

References

  1. 1

    Titirici MM, White RJ, Brun N, et al. Sustainable carbon materials. Chem Soc Rev, 2014, 44: 250–290

    Article  Google Scholar 

  2. 2

    Liang HW, Guan QF, Chen LF, et al. Macroscopic-scale template synthesis of robust carbonaceous nanofiber hydrogels and aerogels and their applications. Angew Chem Int Ed, 2012, 51: 5101–5105

    Article  Google Scholar 

  3. 3

    Bi H, Yin Z, Cao X, et al. Carbon fiber aerogel made from raw cotton: a novel, efficient and recyclable sorbent for oils and organic solvents. Adv Mater, 2013, 25: 5916–5921

    Article  Google Scholar 

  4. 4

    Chen B, Ma Q, Tan C, et al. Carbon-based sorbents with threedimensional architectures for water remediation. Small, 2015, 11: 3319–3336

    Article  Google Scholar 

  5. 5

    Zhao H, Jiao T, Zhang L, et al. Preparation and adsorption capacity evaluation of graphene oxide-chitosan composite hydrogels. Sci China Mater, 2015, 58: 811–818

    Article  Google Scholar 

  6. 6

    Ma Q, Yu Y, Sindoro M, et al. Carbon-based functional materials derived from waste for water remediation and energy storage. Adv Mater, 2017, 29: 1605361

    Article  Google Scholar 

  7. 7

    Chen N, Pan Q. Versatile fabrication of ultralight magnetic foams and application for oil–water separation. ACS Nano, 2013, 7: 6875–6883

    Article  Google Scholar 

  8. 8

    Dong X, Chen J, Ma Y, et al. Superhydrophobic and superoleophilic hybrid foam of graphene and carbon nanotube for selective removal of oils or organic solvents from the surface of water. Chem Commun, 2012, 48: 10660–10662

    Article  Google Scholar 

  9. 9

    Gui X, Wei J, Wang K, et al. Carbon nanotube sponges. Adv Mater, 2010, 22: 617–621

    Article  Google Scholar 

  10. 10

    Wu X, Wu D, Fu R. Studies on the adsorption of reactive brilliant red X-3B dye on organic and carbon aerogels. J Hazard Mater, 2007, 147: 1028–1036

    Article  Google Scholar 

  11. 11

    Mi X, Huang G, Xie W, et al. Preparation of graphene oxide aerogel and its adsorption for Cu2+ ions. Carbon, 2012, 50: 4856–4864

    Article  Google Scholar 

  12. 12

    Niu Z, Liu L, Zhang L, et al. Porous graphene materials for water remediation. Small, 2014, 10: 3434–3441

    Article  Google Scholar 

  13. 13

    Ma Y, Zhang B, Ma H, et al. Polyethylenimine nanofibrous adsorbent for highly effective removal of anionic dyes from aqueous solution. Sci China Mater, 2016, 59: 38–50

    Article  Google Scholar 

  14. 14

    Ge J, Zhao HY, Zhu HW, et al. Advanced sorbents for oil-spill cleanup: recent advances and future perspectives. Adv Mater, 2016, 28: 10459–10490

    Article  Google Scholar 

  15. 15

    Ma Q, Cheng H, Fane AG, et al. Recent development of advanced materials with special wettability for selective oil/water separation. Small, 2016, 12: 2186–2202

    Article  Google Scholar 

  16. 16

    Wen Q, Di J, Jiang L, et al. Zeolite-coated mesh film for efficient oil–water separation. Chem Sci, 2013, 4: 591–595

    Article  Google Scholar 

  17. 17

    Zhang LH, Sun Q, Yang C, et al. Synthesis of magnetic hollow carbon nanospheres with superior microporosity for efficient adsorption of hexavalent chromium ions. Sci China Mater, 2015, 58: 611–620

    Article  Google Scholar 

  18. 18

    Zhuang YT, Gao W, Yu YL, et al. A three-dimensional magnetic carbon framework derived from Prussian blue and amylopectin impregnated polyurethane sponge for lead removal. Carbon, 2016, 108: 190–198

    Article  Google Scholar 

  19. 19

    Komarneni M, Sand A, Burghaus U. Adsorption of thiophene on inorganic MoS2 fullerene-like nanoparticles. Catal Lett, 2009, 129: 66–70

    Article  Google Scholar 

  20. 20

    Ai K, Ruan C, Shen M, et al. MoS2 nanosheets with widened interlayer spacing for high-efficiency removal of mercury in aquatic systems. Adv Funct Mater, 2016, 26: 5542–5549

    Article  Google Scholar 

  21. 21

    Dervin S, Dionysiou DD, Pillai SC. 2D nanostructures for water purification: graphene and beyond. Nanoscale, 2016, 8: 15115–15131

    Article  Google Scholar 

  22. 22

    Chao Y, Zhu W, Wu X, et al. Application of graphene-like layered molybdenum disulfide and its excellent adsorption behavior for doxycycline antibiotic. Chem Eng J, 2014, 243: 60–67

    Article  Google Scholar 

  23. 23

    Zhou W, Yin Z, Du Y, et al. Synthesis of few-layer MoS2 nanosheet- coated TiO2 nanobelt heterostructures for enhanced photocatalytic activities. Small, 2013, 9: 140–147

    Article  Google Scholar 

  24. 24

    Bi H, Xie X, Yin K, et al. Spongy graphene as a highly efficient and recyclable sorbent for oils and organic solvents. Adv Funct Mater, 2012, 22: 4421–4425

    Article  Google Scholar 

  25. 25

    Wang J, Liu J, Chao D, et al. Self-assembly of honeycomb-like MoS2 nanoarchitectures anchored into graphene foam for enhanced lithium-ion storage. Adv Mater, 2014, 26: 7162–7169

    Article  Google Scholar 

  26. 26

    Yang D, Velamakanni A, Bozoklu G, et al. Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and Micro-Raman spectroscopy. Carbon, 2009, 47: 145–152

    Article  Google Scholar 

  27. 27

    Kibsgaard J, Chen Z, Reinecke BN, et al. Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis. Nat Mater, 2012, 11: 963–969

    Article  Google Scholar 

  28. 28

    Ma CB, Qi X, Chen B, et al. MoS2 nanoflower-decorated reduced graphene oxide paper for high-performance hydrogen evolution reaction. Nanoscale, 2014, 6: 5624–5629

    Article  Google Scholar 

  29. 29

    Nguyen DD, Tai NH, Lee SB, et al. Superhydrophobic and superoleophilic properties of graphene-based sponges fabricated using a facile dip coating method. Energ Environ Sci, 2012, 5: 7908–7912

    Article  Google Scholar 

  30. 30

    Bi H, Xie X, Yin K, et al. Highly enhanced performance of spongy graphene as an oil sorbent. J Mater Chem A, 2014, 2: 1652–1656

    Article  Google Scholar 

  31. 31

    Sun H, Xu Z, Gao C. Multifunctional, ultra-flyweight, synergistically assembled carbon aerogels. Adv Mater, 2013, 25: 2554–2560

    Article  Google Scholar 

  32. 32

    Kyzas GZ, Travlou NA, Deliyanni EA. The role of chitosan as nanofiller of graphite oxide for the removal of toxic mercury ions. Colloids Surfs B-Biointerfaces, 2014, 113: 467–476

    Article  Google Scholar 

  33. 33

    Zhao J, Ren W, Cheng HM. Graphene sponge for efficient and repeatable adsorption and desorption of water contaminations. J Mater Chem, 2012, 22: 20197

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by Ministry of Education (Singapore) under AcRF Tier 2 (ARC 19/15, MOE2014-T2-2-093, MOE2015-T2-2-057 and MOE2016-T2-2-103) and AcRF Tier 1 (2016-T1-001-147 and 2016-T1-002-051), NTU under Start-Up Grant (M4081296.070.500000), and NOL Fellowship Programme Research Grant in Singapore. This research grant is supported by the Singapore National Research Foundation under its Environmental & Water Technologies Strategic Research Programme and administered by the Environment & Water Industry Programme Office (EWI) of the PUB (project No.: 1301-IRIS-47). This research is supported by the National Research Foundation, Prime Minister’s Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. We would like to acknowledge the Facility for Analysis, Characterization, Testing and Simulation, Nanyang Technological University, Singapore, for use of their electron microscopy facilities.

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Correspondence to Hua Zhang.

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Bo Chen received his BSc degree and MSc degrees from Lanzhou University (in 2009) and Shandong University (in 2012), respectively, and completed his PhD with Prof. Hua Zhang at Nanyang Technological University (in 2017). Currently, he is a Postdoctoral Fellow at School of Materials Science and Engineering, Nanyang Technological University in Prof. Hua Zhang’s group. His research work focuses on the preparation of novel functional materials, especially twodimensional nanomaterials and carbon-based nanomaterials, for water remediation and water splitting.

Hua Zhang obtained his BSc and MSc degrees at Nanjing University in 1992 and 1995, respectively, and completed his PhD with Prof. Zhongfan Liu at Peking University in 1998. As a Postdoctoral Fellow, he joined Prof. Frans C. De Schryver’s group at Katholieke Universiteit Leuven (Belgium) in 1999, and then moved to Prof. Chad A. Mirkin’s group at Northwestern University in 2001. After he worked at NanoInk Inc. (USA) and Institute of Bioengineering and Nanotechnology (Singapore), he joined Nanyang Technological University in July 2006. His current research interests focus on the synthesis of ultrathin two-dimensional nanomaterials (e.g., metal nanosheets, graphene, metal dichalcogenides, metalorganic frameworks, covalent organic frameworks, etc.) and their hybrid composites for applications in nano- and biosensors, clean energy, (opto-)electronic devices, catalysis, and water remediation; etc.

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Chen, B., Bi, H., Ma, Q. et al. Preparation of graphene-MoS2 hybrid aerogels as multifunctional sorbents for water remediation. Sci. China Mater. 60, 1102–1108 (2017). https://doi.org/10.1007/s40843-017-9150-7

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Keywords

  • Graphene
  • MoS2
  • aerogels
  • multifunctional sorbents
  • water remediation