Skip to main content
SpringerLink
Log in

Single-step synthesis of N, S co-doped waste-derived nanoporous carbon sorbent for mercury vapor removal

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

As well known, mercury is a toxic trace element due to its bioaccumulation and volatility which results in severe effects in health of ecosystems and humans’ life. Herein, for the first time, the synthesis of a N and S dual-doped waste-derived graphene-like nanoporous carbon via a facile and single-step route is presented and its capability in mercury vapor removal from gas streams is investigated. To prepare a modified adsorbent, thiourea was utilized as the doping agent to induce nitrogen and sulfur dopants into the nanoporous carbon structure derived from pyrolysis of cabbage (Capitat. var. Brassica oleracea) waste from Brassicaceae family as an inherently S, N-containing precursor, which is produced in noticeable amounts annually. The prepared adsorbents were characterized through FTIR, XRD, BET, SEM, TEM, and CHNOS techniques to get an insight into the structure, morphology, and chemical characteristics of the adsorbents. The structural characterization revealed the successful synthesis of a graphene-like nanoporous carbon sheet which was doped with nitrogen and sulfur atoms. The S, N dual-doped graphene-like carbon nanosheets showed an enhanced activity toward mercury vapor adsorption. For this end, two different dopant to carbon source ratios were considered and it was found that the higher dopant amount results in a better performance. From the adsorption experiments, it was revealed that the pristine graphene–like carbon had a less performance in mercury removal (71%) compared with doped samples (more than 90%) which shows the necessity of reinforcement and surface modification of as mentioned cabbage base graphene. However, the best sample which was prepared with the dopant to carbon ratio of 10 had a performance of 94.5% removal (2100 μg/g) compared with 89% (1980 μg/g) for mercury removal by the sulfur-impregnated commercial activated carbon.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

Data availability

Hereby, we confirm that all data and materials can be provided upon request by reviewers, editors, or readers.

References

  • Cao Y, Huang J, Li Y, Qiu S, Liu J, Khasanov A, Khan MA, Young DP, Peng F, Cao D (2016) One-pot melamine derived nitrogen doped magnetic carbon nanoadsorbents with enhanced chromium removal. Carbon 109:640–649

    Article  CAS  Google Scholar 

  • Chalkidis A, Jampaiah D, Hartley PG, Sabri YM, Bhargava SK (2020) Mercury in natural gas streams: a review of materials and processes for abatement and remediation. J Hazard Mater 382:121036

    Article  CAS  Google Scholar 

  • Couling DJ, Nguyen HV, Green WH (2012) Screening of metal oxides and metal sulfides as sorbents for elemental mercury at elevated temperatures. Fuel 97:783–795

    Article  CAS  Google Scholar 

  • Ding F, Zhao Y, Mi L, Li H, Li Y, Zhang J (2012) Removal of gas-phase elemental mercury in flue gas by inorganic chemically promoted natural mineral sorbents. Ind Eng Chem Res 51(7):3039–3047

    Article  CAS  Google Scholar 

  • Dong J, Xu Z, Kuznicki SM (2009) Mercury removal from flue gases by novel regenerable magnetic nanocomposite sorbents. Environ Sci Technol 43(9):3266–3271

    Article  CAS  Google Scholar 

  • Ghasemy E, Motejadded HB, Hamzehlouyan T, Yousefian Z (2018) N-doped CNT nanocatalyst prepared from camphor and urea for gas phase desulfurization: experimental and DFT study. J Taiwan Inst Chem Eng 85:121–131

    Article  CAS  Google Scholar 

  • Ghasemy E, Emrooz HBM, Rashidi A, Hamzehlouyan T (2020) Highly uniform molybdenum oxide loaded N-CNT as a remarkably active and selective nanocatalyst for H2S selective oxidation. Sci Total Environ 711:134819

    Article  CAS  Google Scholar 

  • Ghenaatian HR, Shakourian-Fard M, Kamath G (2019) The effect of sulfur and nitrogen/sulfur co-doping in graphene surface on the adsorption of toxic heavy metals (Cd, Hg, Pb). J Mater Sci 54(20):13175–13189

    Article  CAS  Google Scholar 

  • Hu C, Zhou J, He S, Luo Z, Cen K (2009) Effect of chemical activation of an activated carbon using zinc chloride on elemental mercury adsorption. Fuel Process Technol 90(6):812–817

    Article  CAS  Google Scholar 

  • Jurng J, Lee TG, Lee GW, Lee S-J, Kim BH, Seier J (2002) Mercury removal from incineration flue gas by organic and inorganic adsorbents. Chemosphere 47(9):907–913

    Article  CAS  Google Scholar 

  • Kabiri S, Tran DNH, Cole MA, Losic D (2016) Functionalized three-dimensional (3D) graphene composite for high efficiency removal of mercury. Environ Sci: Water Res Technol 2(2):390–402

    CAS  Google Scholar 

  • Lazar P, Mach R, Otyepka M (2019) Spectroscopic fingerprints of graphitic, pyrrolic, pyridinic, and chemisorbed nitrogen in N-doped graphene. J Phys Chem C 123(16):10695–10702

    Article  CAS  Google Scholar 

  • Liu D, Li C, Wu J, Liu Y (2019) Novel carbon-based sorbents for elemental mercury removal from gas streams: a review. Chem Eng J 123514

  • Liu H, Chang L, Liu W, Xiong Z, Zhao Y, Zhang J (2020) Advances in mercury removal from coal-fired flue gas by mineral adsorbents. Chem Eng J 379:122263

    Article  CAS  Google Scholar 

  • Luo Z, Lim S, Tian Z, Shang J, Lai L, MacDonald B, Fu C, Shen Z, Yu T, Lin J (2011) Pyridinic N doped graphene: synthesis, electronic structure, and electrocatalytic property. J Mater Chem 21(22):8038–8044

    Article  CAS  Google Scholar 

  • Marczak M, Budzyń S, Szczurowski J, Kogut K, Burmistrz P (2019) Active methods of mercury removal from flue gases. Environ Sci Pollut Res 26(9):8383–8392

    Article  CAS  Google Scholar 

  • Meeprasert J, Junkaew A, Rungnim C, Kunaseth M, Kungwan N, Promarak V, Namuangruk S (2016) Capability of defective graphene-supported Pd13 and Ag13 particles for mercury adsorption. Appl Surf Sci 364:166–175

    Article  CAS  Google Scholar 

  • Naushad M, Ahamad T, Al-Maswari BM, Alqadami AA, Alshehri SM (2017) Nickel ferrite bearing nitrogen-doped mesoporous carbon as efficient adsorbent for the removal of highly toxic metal ion from aqueous medium. Chem Eng J 330:1351–1360

    Article  CAS  Google Scholar 

  • Seema H, Kemp KC, Le NH, Park S-W, Chandra V, Lee JW, Kim KS (2014) Highly selective CO2 capture by S-doped microporous carbon materials. Carbon 66:320–326

    Article  CAS  Google Scholar 

  • Simões EF, Leitão JM, da Silva JCE (2017) Sulfur and nitrogen co-doped carbon dots sensors for nitric oxide fluorescence quantification. Anal Chim Acta 960:117–122

    Article  Google Scholar 

  • Sun D, Ban R, Zhang P-H, Wu G-H, Zhang J-R, Zhu J-J (2013) Hair fiber as a precursor for synthesizing of sulfur-and nitrogen-co-doped carbon dots with tunable luminescence properties. Carbon 64:424–434

    Article  CAS  Google Scholar 

  • Sun H, Zhao S, Ma Y, Wu J, Liang P, Yang D, Zhang H (2018) Effective and regenerable Ag/4A zeolite nanocomposite for Hg0 removal from natural gas. J Alloys Compd 762:520–527

    Article  CAS  Google Scholar 

  • Suresh Kumar Reddy K, Al Shoaibi A, Srinivasakannan C (2014) Elemental mercury adsorption on sulfur-impregnated porous carbon–a review. Environ Technol 35(1):18–26

    Article  CAS  Google Scholar 

  • Vidic RD, Siler DP (2001) Vapor-phase elemental mercury adsorption by activated carbon impregnated with chloride and chelating agents. Carbon 39(1):3–14

    Article  CAS  Google Scholar 

  • Wdowin M, Wiatros-Motyka MM, Panek R, Stevens LA, Franus W, Snape CE (2014) Experimental study of mercury removal from exhaust gases. Fuel 128:451–457

    Article  CAS  Google Scholar 

  • Wdowin M, Macherzyński M, Panek R, Górecki J, Franus W, Christidis G (2015) Investigation of the sorption of mercury vapour from exhaust gas by an Ag-X zeolite. Clay Miner 50(1):31–40

    Article  CAS  Google Scholar 

  • Wu H, Jiang J, Gu X, Tong C (2017) Nitrogen and sulfur co-doped carbon quantum dots for highly selective and sensitive fluorescent detection of Fe (III) ions and L-cysteine. Microchim Acta 184(7):2291–2298

    Article  CAS  Google Scholar 

  • Xie J, Qu Z, Yan N, Yang S, Chen W, Hu L, Huang W, Liu P (2013) Novel regenerable sorbent based on Zr–Mn binary metal oxides for flue gas mercury retention and recovery. J Hazard Mater 261:206–213

    Article  CAS  Google Scholar 

  • Xie J, Xu H, Qu Z, Huang W, Chen W, Ma Y, Zhao S, Liu P, Yan N (2014) Sn–Mn binary metal oxides as non-carbon sorbent for mercury removal in a wide-temperature window. J Colloid Interface Sci 428:121–127

    Article  CAS  Google Scholar 

  • Xu H, Qu Z, Zhao S, Mei J, Quan F, Yan N (2015a) Different crystal-forms of one-dimensional MnO2 nanomaterials for the catalytic oxidation and adsorption of elemental mercury. J Hazard Mater 299:86–93

    Article  CAS  Google Scholar 

  • Xu Q, Pu P, Zhao J, Dong C, Gao C, Chen Y, Chen J, Liu Y, Zhou H (2015b) Preparation of highly photoluminescent sulfur-doped carbon dots for Fe (III) detection. J Mater Chem A 3(2):542–546

    Article  CAS  Google Scholar 

  • Xu Y, Zhong Q, Liu X (2015c) Elemental mercury oxidation and adsorption on magnesite powder modified by Mn at low temperature. J Hazard Mater 283:252–259

    Article  CAS  Google Scholar 

  • Yao Y, Velpari V, Economy J (2014) Design of sulfur treated activated carbon fibers for gas phase elemental mercury removal. Fuel 116:560–565

    Article  CAS  Google Scholar 

  • Yu Z, Bai Y, Wang Y, Liu Y, Zhao Y, Liu Y, Sun K (2017) One-step synthesis of three-dimensional nitrogen and sulfur co-doped graphene networks as low cost metal-free counter electrodes for dye-sensitized solar cells. Chem Eng J 311:302–309

    Article  CAS  Google Scholar 

  • Yuan X, An N, Zhu Z, Sun H, Zheng J, Jia M, Lu C, Zhang W, Liu N (2018) Hierarchically porous nitrogen-doped carbon materials as efficient adsorbents for removal of heavy metal ions. Process Saf Environ Prot 119:320–329

    Article  CAS  Google Scholar 

  • Yun YS, Le V-D, Kim H, Chang S-J, Baek SJ, Park S, Kim BH, Kim Y-H, Kang K, Jin H-J (2014) Effects of sulfur doping on graphene-based nanosheets for use as anode materials in lithium-ion batteries. J Power Sources 262:79–85

    Article  CAS  Google Scholar 

  • Zeng X, Xu Y, Zhang B, Luo G, Sun P, Zou R, Yao H (2017) Elemental mercury adsorption and regeneration performance of sorbents FeMnOx enhanced via non-thermal plasma. Chem Eng J 309:503–512

    Article  CAS  Google Scholar 

  • Zhang J, Duan Y, Zhou Q, Zhu C, She M, Ding W (2016a) Adsorptive removal of gas-phase mercury by oxygen non-thermal plasma modified activated carbon. Chem Eng J 294:281–289

    Article  CAS  Google Scholar 

  • Zhang J, Yang Z, Qiu J, Lee H-W (2016b) Design and synthesis of nitrogen and sulfur co-doped porous carbon via two-dimensional interlayer confinement for a high-performance anode material for lithium-ion batteries. J Mater Chem A 4(16):5802–5809

    Article  CAS  Google Scholar 

  • Zhang G, Wang P, Lu W-T, Wang C-Y, Li Y-K, Ding C, Gu J, Zheng X-S, Cao F-F (2017) Co nanoparticles/Co, N, S tri-doped graphene templated from in-situ-formed Co, S co-doped g-C3N4 as an active bifunctional electrocatalyst for overall water splitting. ACS Appl Mater Interfaces 9(34):28566–28576

    Article  CAS  Google Scholar 

  • Zhou Q, Duan Y-F, Hong Y-G, Zhu C, She M, Zhang J, Wei H-Q (2015) Experimental and kinetic studies of gas-phase mercury adsorption by raw and bromine modified activated carbon. Fuel Process Technol 134:325–332

    Article  CAS  Google Scholar 

  • Zhou Z, Liu X, Li C, Cao XE, Xu M (2020) Seawater-assisted synthesis of MnCe/zeolite-13X for removing elemental mercury from coal-fired flue gas. Fuel 262:116605

    Article  CAS  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Department of environmental science, Faculty of natural resources and environment, Science and research branch, Islamic Azad University, Tehran, Iran

    Forouzan Vakili & Lobat Taghavi

  2. Nanotechnology Research Center, Research Institute of Petroleum Industry (RIPI), West Entrance Blvd., Olympic Village, P.O. Box 14857-33111, Tehran, Iran

    Alimorad Rashidi

  3. Department of environmental Engineering, Faculty of natural resources and environment, Science and research branch, Islamic Azad University, Tehran, Iran

    Nabiollah Mansouri

Authors
  1. Forouzan Vakili
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Alimorad Rashidi
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Lobat Taghavi
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Nabiollah Mansouri
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Forouzan Vakili: investigation, data curation, writing—original draft preparation. Alimorad Rashidi: supervision, conceptualization, methodology, validation, writing—reviewing and editing; Lobat Taghavi: advisor, validation, writing—reviewing. Nabiollah Mansouri: advisor, validation, writing—reviewing.

Corresponding author

Correspondence to Alimorad Rashidi.

Ethics declarations

Conflict of interest

The authors declare that there is no conflict of interest.

Ethical approval

Hereby, we confirm that we consent to all ethical standards of the journal.

Consent to participate

Hereby, we confirm that the presented research work does not include any data regarding the humans’ health or any investigation on humans or animals.

Consent to publish

Hereby, we confirm that we consent to publish the work according to the guidelines of the journal.

Additional information

Responsible Editor: Tito Roberto Cadaval Jr

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Vakili, F., Rashidi, A., Taghavi, L. et al. Single-step synthesis of N, S co-doped waste-derived nanoporous carbon sorbent for mercury vapor removal. Environ Sci Pollut Res 28, 17265–17274 (2021). https://doi.org/10.1007/s11356-020-12075-2

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-020-12075-2

Keywords

Search

Navigation