Skip to main content
SpringerLink
Log in

Novel strategy to enhance the biological treatment of coal chemical wastewater by nano-zero valent iron loaded fly ash-based activated carbon assisted activated sludge process

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

Abstract

Industrial waste as novel conductive mediator was applied for wastewater treatment as a novel strategy for both waste recycling and sustainable development of wastewater treatment. In this study, nanoscale zero valent iron-loaded fly ash-based activated carbon (nZVI@FABAC) was prepared and applied to enhancing activated sludge (AS) process for coal chemical wastewater (CCW) treatment. The results demonstrated that the removal efficiencies of COD and total phenols (TPh) in nZVI@FABAC/AS process reached about 83.96 and 85.17%, which increased 52.51 and 31.52% compared with the single AS process, respectively. And the acute toxic unit value of CCW was reduced by 88.24% after nZVI@FABAC/AS process treatment. The various functional bacteria including phenol-degrading bacteria (Comamonas and Acinetobacter), electroactive bacteria (Geobacter), and iron reduction bacteria (Geothrix) were enriched in the nZVI@FABAC/AS process, which provided various electron transfer pathways to improve the degradation of toxic organics in CCW. Accordingly, nZVI@FABAC/AS process provided a promising and sustainable way for industrial wastewater treatment.

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

Similar content being viewed by others

Data availability

Not applicable.

Abbreviations

AS:

Activated sludge

CCW:

Coal chemical wastewater

3E:

Engineering, economic, environmental

FABAC:

Fly ash-based activated carbon

nZVI:

Nanoscale zero valent iron

nZVI@FABAC:

nZVI-loaded FABAC

nZVI@FABAC/AS:

nZVI@FABAC-enhanced AS process

SEM:

Scanning electron microscope

TPh:

Total phenols

T. thermophila :

Tetrahymena thermophila

TU:

Toxic unit

XRD:

X-ray diffraction

References

  • Chen KF, Kao CM, Sung WP, Lin CC, Yeh TY (2011) Enhanced in-situ anaerobic bioremediation of TCE-contaminated groundwater using nanoscale zero-valent iron (nZVI). Mater Sci Forum 694:3–7

    Article  Google Scholar 

  • Gao C, Wang A, Wu WM, Yin Y, Zhao YG (2014) Enrichment of anodic biofilm inoculated with anaerobic or aerobic sludge in single chambered air-cathode microbial fuel cells. Bioresour Technol 167:124–132

    Article  CAS  Google Scholar 

  • Ghauch A, Tuqan A, Assi HA (2009) Antibiotic removal from water: elimination of amoxicillin and ampicillin by microscale and nanoscale iron particles. Environ Pollut 157(5):1626–1635

    Article  CAS  Google Scholar 

  • Greenberg AE, Clesceri LS, Eaton AD (1998) Standard methods for the examination of water and wastewater. APHA, Washington, DC

  • Guo T, Ji Y, Zhao J, Horn H, Li J (2020) Coupling of Fe-C and aerobic granular sludge to treat refractory wastewater from a membrane manufacturer in a pilot-scale system. Water Res 186(14):116331

    Article  CAS  Google Scholar 

  • Huang Y, Hou X, Liu S, Ni J (2016) Correspondence analysis of bio-refractory compounds degradation and microbiological community distribution in anaerobic filter for coking wastewater treatment. Chem Eng J 304:864–872

    Article  CAS  Google Scholar 

  • Ji QH, Tabassum S, Hena S, Silva CG, Yu GX, Zhang ZJ (2016) A review on the coal gasification wastewater treatment technologies: past, present and future outlook. J Clean Prod 126:38–55

    Article  CAS  Google Scholar 

  • Krehula S, Musi S (2006) Influence of ruthenium ions on the precipitation of α-FeOOH, α-Fe2O3 and Fe3O4 in highly alkaline media. J Alloy Compd 416(1–2):284–290

    Article  CAS  Google Scholar 

  • Li Y, Tabassum S, Chu C, Zhang Z (2018) Inhibitory effect of high phenol concentration in treating coal gasification wastewater in anaerobic biofilter. J Environ Sci 64:207–215

    Article  CAS  Google Scholar 

  • Li Y, Liu L, Wang Q, Wu J, Huang T (2020) Enhanced anaerobic co-metabolism of coal gasification wastewater via the assistance of zero-valent iron. J Water Process Eng 40(8):101817

    Google Scholar 

  • Ling XF, Li JS, Zhu W, Zhu YY, Sun XY, Shen JY, Han WQ, Wang LJ (2012) Synthesis of nanoscale zero-valent iron/ordered mesoporous carbon for adsorption and synergistic reduction of nitrobenzene. Chemosphere 7(8):655–600

    Article  Google Scholar 

  • Liu F, Rotaru AE, Shrestha PM, Malvankar NS, Nevin KP, Lovley DR (2012) Promoting direct interspecies electron transfer with activated carbon. Energy Environ Sci 10:118–123

    Google Scholar 

  • Lonergan DJ, Lovley DR, Davis M, Stolz JF, McInerney MJ (1994) Geobacter sulfurreducens sp. nov., a hydrogen- and acetate-oxidizing dissimilatory metal-reducing microorganism. Appl Environ Microb 628:12428

    Google Scholar 

  • Lovley D, Rooneyvarga J, Anderson RT, Fraga JL, Ringelberg D (1999) Microbial communities associated with anaerobic benzene degradation in a petroleum-contaminated aquifer. Appl Environ Microb 65(7):3056–3063

    Article  Google Scholar 

  • Ma Q, Qu Y, Shen W, Zhang Z, Wang J, Liu Z, Li D, Li H, Zhou J (2015) Bacterial community compositions of coking wastewater treatment plants in steel industry revealed by Illumina high-throughput sequencing. Bioresour Technol 179:436–443

    Article  CAS  Google Scholar 

  • Ma ZY, Yang Y, Jiang YH, Xi BD, Yang TX, Peng X, Lian XY, Yan K, Liu HL (2017) Enhanced degradation of 2,4-dinitrotoluene in groundwater by persulfate activated using iron–carbon micro-electrolysis. Chem Eng J 311:183–190

    Article  CAS  Google Scholar 

  • Ma WW, Han YX, Xu CY, Han HJ, Wc Ma, Zhu H (2018a) Enhanced degradation of phenolic compounds in coal gasification wastewater by a novel integration of micro-electrolysis with biological reactor (MEBR) under the micro-oxygen condition. Bioresour Technol 251:303–310

    Article  CAS  Google Scholar 

  • Ma WW, Han YX, Xu CY, Han HJ, Zhong D, Zhu H, Li K (2018b) The mechanism of synergistic effect between iron-carbon microelectrolysis and biodegradation for strengthening phenols removal in coal gasification wastewater treatment. Bioresour Technol 271:84–90

    Article  Google Scholar 

  • Ma WW, Han YX, Xu CY, Han HJ, Zhu H, Li K, Zheng MQ (2018c) Biotoxicity assessment and toxicity mechanism on coal gasification wastewater (CGW): A comparative analysis of effluent from different treatment processes. Sci Total Environ 637–638(1):1–8

    Article  Google Scholar 

  • Ma WC, Li JX, Zhong D, Ge XL, Li KF, Dai CL, Gao YH (2020) New insights into enhanced anaerobic degradation of coal gasification wastewater (CGW) with the assistance of magnetite nanoparticles. Chemosphere 262:127872

    Article  Google Scholar 

  • Majchrzak-Kucba I, Nowak W, Sciubidlo A (2009) Studies on the properties of mesoporous materials derived from polish fly ashes. International Pittsburgh Coal Conference, Pittsburgh, pp 1542–1545

  • Nevin KP, Lovley DR (2002) Mechanisms for accessing insoluble Fe(III) oxide during dissimilatory Fe(III) reduction by geothrix fermentans. Appl Environ Microb 68(5):2294–2299

    Article  CAS  Google Scholar 

  • Nouha K (2016) Characterization of extracellular polymeric substances (Eps) produced by Cloacibacterium normanense isolated from wastewater sludge for sludge settling and dewatering. J Civil Environ Eng 5(6):1–8

    Article  Google Scholar 

  • Persoone G, Marsalek B, Blinova I, Törökne A, Zarina D, Manusadzianas L, Nalecz-Jawecki G, Tofan L, Stepanova N, Tothova L, Kolar B (2003) A practical and user-friendly toxicity classification system with microbiotests for natural waters and wastewaters. Environ toxicol 18(6):395–401

    Article  CAS  Google Scholar 

  • Ren X, Yue C, Liang G, She Z, Gao M, Zhao Y, Shao M (2018) The influence of Fe2+, Fe3+ and magnet powder (Fe3O4) on aerobic granulation and their mechanisms. Ecotoxicol Environ Saf 164:1–11

    Article  CAS  Google Scholar 

  • Shawabkeh RA, Aslam Z, Hussien IA (2015) Thermochemical treatment of fly ash for synthesis of mesoporous activated carbon. J Therm Anal Calorim 122:1191–1196

    Article  CAS  Google Scholar 

  • Shi JX, Han YX, Xu CY, Han HJ (2018) Biological coupling process for treatment of toxic and refractory compounds in coal gasification wastewater. Rev Environ Sci Bio 17(4):765–790

    Article  CAS  Google Scholar 

  • Shi JX, Han YX, Xu CY, Han HJ (2019) Enhanced anaerobic degradation of selected nitrogen heterocyclic compounds with the assistance of carboxymethyl cellulose. Sci Total Environ 689(1):781–788

    Article  CAS  Google Scholar 

  • Wang Y, Kern SE, Newman DK (2010) Endogenous phenazine antibiotics promote anaerobic survival of Pseudomonas aeruginosa via extracellular electron transfer. J Bacter 192(1):365–369

    Article  CAS  Google Scholar 

  • Wang ZX, Xu XC, Gong Z, Yang FL (2012) Removal of COD, phenols and ammonium from Lurgi coal gasification wastewater using A2O-MBR system. J Hazard Mater 235–236:78–84

    Article  Google Scholar 

  • Wu B, Wang J, Hu Z, Yuan S, Wang W (2020) Anaerobic biotransformation and potential impact of quinoline in an anaerobic methanogenic reactor treating synthetic coal gasification wastewater and response of microbial community. J Hazard Mater 384:67–85

    Article  Google Scholar 

  • Xiao J, Gao B, Yue Q, Sun Y, Qian L (2015) Characterization of nanoscale zero-valent iron supported on granular activated carbon and its application in removal of acrylonitrile from aqueous solution. J Taiwan Inst Chem Eng 55:152–158

    Article  CAS  Google Scholar 

  • Yang JW, Hou ZK, Chen ZR, Ma ZY, Li SH, Wang YL, Gao J, Cui PZ (2021) Comprehensive analysis of diverse biochemical treatment technologies of fixed-bed coal gasification wastewater from the perspective of different weight dimensions. Sep Purif Technol 257:117889

    Article  CAS  Google Scholar 

  • Zhao Q, Liu Y (2016) State of the art of biological processes for coal gasification wastewater treatment. Biotech Adv 34(6):1064–1072

    Article  CAS  Google Scholar 

  • Zheng MQ, Han YX, Xu CY, Han HJ, Zhang ZW (2018) Discrimination of typical cyclic compounds and selection of toxicity evaluation bioassays for coal gasification wastewater (CGW) based on toxicity mechanism of actions (MOAs). Sci Total Environ 644(10):324–334

    Article  CAS  Google Scholar 

  • Zheng MQ, Han YX, Han HJ, Xu CY, Zhang ZW, Ma WW (2019) Synergistic degradation on phenolic compounds of coal pyrolysis wastewater (CPW) by lignite activated coke-active sludge (LAC-AS) process: Insights into succession of microbial community under selective pressure. BioresourTechnol 281:126–134

    Article  CAS  Google Scholar 

  • Zheng MQ, Shi JX, Xu CY, Ma WC, Han HJ (2020a) Ecological and functional research into microbiomes for targeted phenolic removal in anoxic carbon-based fluidized bed reactor (CBFBR) treating coal pyrolysis wastewater (CPW). Bioresour Technol 308:123308

    Article  CAS  Google Scholar 

  • Zheng MQ, Shi JX, Xu CY, Han YX, Zhang ZW, Han HJ (2020b) Insights into electroactive biofilms for enhanced phenolic degradation of coal pyrolysis wastewater (CPW) by magnetic activated coke (MAC): metagenomic analysis in attached biofilm and suspended sludge. J Hazard Mater 395:122688

    Article  CAS  Google Scholar 

  • Zheng MQ, Han HJ, Shi JX, Zhang ZW, Xu CY (2021) Metagenomic analysis of aromatic ring-cleavage mechanism in nano-Fe3O4@activated coke enhanced bio-system for coal pyrolysis wastewater treatment. J Hazard Mater 414(8):125387

    Article  CAS  Google Scholar 

  • Zhu H, Han YX, Ma WC, Han HJ, Ma WW (2018a) New insights into enhanced anaerobic degradation of coal gasification wastewater (CGW) with the assistance of graphene. Bioresour Technol 262:302–309

    Article  CAS  Google Scholar 

  • Zhu H, Han YX, Xu CY, Han HJ, Ma WW (2018b) Overview of the state of the art of processes and technical bottlenecks for coal gasification wastewater treatment. Sci Total Environ 637:1108–1126

    Article  Google Scholar 

Download references

Funding

This work was supported by Natural Science Foundation of Shandong Province (No. ZR2021QE227), Open Project of State Key Laboratory of Urban Water Resource and Environment (No. ES202120), Taishan Scholars Program of Shandong Province, China (No. tsqn201812091).

Author information

Authors and Affiliations

  1. School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao, 266520, China

    Weiwei Ma, Xiaoqi Zhang, Xueqing Shi, Qiaoping Kong, Tong Yu & Fei Zhao

  2. State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, 150090, China

    Hongjun Han

Authors
  1. Weiwei Ma
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Xiaoqi Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Hongjun Han
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Xueqing Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Qiaoping Kong
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Tong Yu
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Fei Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

WM: conceptualization, methodology, investigation, and writing original draft; XZ: experimental design and data curation; HH: supervision and funding acquisition; XS: review, editing, supervision, and funding acquisition; QK: resources, editing, and project administration; FZ: resources and review; TY: resources and editing.

Corresponding author

Correspondence to Xueqing Shi.

Ethics declarations

Ethical approval

Not applicable.

Consent to participate

Not applicable.

Consent for publication

Not applicable.

Conflict of interest

The authors declare no competing interests.

Additional information

Responsible Editor: Weiming Zhang

Publisher's Note

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

Highlights

1. Novel conductive mediator of nZVI@FABAC was prepared.

2. nZVI@FABAC/AS process effectively enhanced the removal of toxic organics in CCW.

3. Biotoxicity of CCW was significantly reduced after nZVI@FABAC/AS process treatment.

4. nZVI@FABAC greatly facilitated the enrichment of various functional bacteria.

5. nZVI@FABAC/AS process has a promising application from the 3E perspective.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 52 KB)

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Ma, W., Zhang, X., Han, H. et al. Novel strategy to enhance the biological treatment of coal chemical wastewater by nano-zero valent iron loaded fly ash-based activated carbon assisted activated sludge process. Environ Sci Pollut Res 30, 110550–110561 (2023). https://doi.org/10.1007/s11356-023-29904-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-023-29904-9

Keywords

Search

Navigation