Log in

Hydrothermal synthesis of high crystallinity ZSM-5 zeolite from coal gasification coarse slag and mother liquor circulation for efficient coal chemical wastewater purification

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

Abstract

A hydrothermal synthesis method was developed to produce high crystallinity ZSM-5 zeolite using coal gasification coarse slag (CGCS) as the raw material. Instead of the expensive NaOH(s.), Na2SiO3(s.) was utilized to activate, depolymerize, and recombine Si and Al elements in the CGCS. The mother liquor circulation technology was employed to recover and reuse raw materials and residual reagents (Na2SiO3(aq.) and TPABr), reducing waste emissions and enhancing resource utilization efficiency. The synthesized ZSM-5 had a specific surface area of 455.675 m2 g−1, pore volume of 0.284 cm3 g−1, and pore diameter of 2.496 nm. The influence of various factors on the morphology and crystallinity of ZSM-5 was investigated, resulting in the production of ZSM-5 with higher specific surface area and pore volume. Adsorption experiments showed that WU-ZSM-5 exhibited a removal efficiency of 85% for ammonia nitrogen (NH4+-N(aq.)), validating its effectiveness in coal chemical wastewater purification. The mother liquor recycling technology enabled zero-emission utilization of solid waste resources and improved the utilization rate of alkali and template to 90%. These results demonstrate the potential application of the developed method in the efficient treatment of coal chemical wastewater.

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

Access this article

Subscribe and save

Springer+ Basic
EUR 32.99 /Month
  • Get 10 units per month
  • Download Article/Chapter or Ebook
  • 1 Unit = 1 Article or 1 Chapter
  • Cancel anytime
Subscribe now

Buy Now

Price includes VAT (Germany)

Instant access to the full article PDF.

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

Similar content being viewed by others

Data Availability

Raw data and materials are available.

References

  • Belviso C (2018) State-of-the-art applications of fly ash from coal and biomass: a focus on zeolite synthesis processes and issues. Prog Energ Combust 65:109–135

    Google Scholar 

  • Bensafi B, Chouat N, Djafri F (2023) The universal zeolite ZSM-5: Structure and synthesis strategies. A review. Coordin Chem Rev. 496:215

    Google Scholar 

  • Bukhari SS, Behin J, Kazemian H, Rohani S (2015) Conversion of coal fly ash to zeolite utilizing microwave and ultrasound energies: a review. Fuel 140:250–266

    CAS  Google Scholar 

  • Chen CT, Iyoki K, Hu P, Yamada H, Ohara K, Sukenaga S, Ando M, Shibata H, Okubo T, Wakihara T (2021) Reaction kinetics regulated formation of short-range order in an amorphous matrix during zeolite crystallization. J Am Chem Soc 143:10986–10997

    CAS  Google Scholar 

  • Dallenes J, Wuyts J, Van Velthoven N, Krajnc A, Mali G, Usoltsev OA, Bugaev AL, De Vos D (2023) Zeolites as equilibrium-shifting agents in shuttle catalysis. Nat Catal 6:495–505

    CAS  Google Scholar 

  • Demikhova NR, Rubtsova MI, Kireev GA, Cherednichenko KA, Vinokurov VA, Glotov AP (2023) Micro-mesoporous catalysts based on ZSM-5 zeolite synthesized from natural clay nanotubes: preparation and application in the isomerization of C-8 aromatic fraction. Chem Eng J 453:139581

    CAS  Google Scholar 

  • Du J, Liu Z, Christodoulatos C, Conway M, Bao Y, Meng W (2022) Utilization of off-specification fly ash in preparing ultra-high-performance concrete (UHPC): mixture design, characterization, and life-cycle assessment. Resour Conserv Recy 180:106136

    Google Scholar 

  • Du M, Advincula PA, Ding X, Tour JM, **ang C (2023) Coal-based carbon nanomaterials: en route to clean coal conversion toward net zero CO2. Adv Mater 35(25):2300129

    CAS  Google Scholar 

  • Faizan M, Song H (2023) Critical review on catalytic biomass gasification: state-of-art progress, technical challenges, and perspectives in future development. J Clean Prod 408:137224

    CAS  Google Scholar 

  • Felvey N, Guo J, Rana R, Xu L, Bare SR, Gates BC, Katz A, Kulkarni AR, Runnebaum RC, Kronawitter CX (2022) Interconversion of atomically dispersed platinum cations and platinum clusters in zeolite ZSM-5 and formation of platinum gem-dicarbonyls. J Am Chem Soc 144:13874–13887

    CAS  Google Scholar 

  • Gai H, Liu X, Feng B, Gai C, Huang T, **ao M, Song H (2021) An alternative scheme of biological removal of ammonia nitrogen from wastewater–highly dispersed Ru cluster @mesoporous TiO2 for the catalytic wet air oxidation of low-concentration ammonia. Chem Eng J 407:127082

    CAS  Google Scholar 

  • Iqbal A, Sattar H, Haider R, Munir S (2019) Synthesis and characterization of pure phase zeolite 4A from coal fly ash. J Clean Prod 219:258–267

    CAS  Google Scholar 

  • Ji W, Zhang S, Zhao P, Zhang S, Feng N, Lan L, Zhang X, Sun Y, Li Y, Ma Y (2020) Green synthesis method and application of NaP zeolite prepared by coal gasification coarse slag from Ningdong, China. Appl Sci 10:082694

    Google Scholar 

  • Jia W, Guo Y, Guo F, Li H, Li Y, Zhang Y, Wu J, Si C (2023) Co-combustion of carbon-rich fraction from coal gasification fine slag and biochar: gas emission, ash sintering, heavy metals evolutions and environmental risk evaluation. Chem Eng J 471:144312

    CAS  Google Scholar 

  • Jonscher C, Seifert M, Kretzschmar N, Marschall MS, Le Anh M, Doert T, Busse O, Weigand JJ (2022) Origin of morphology change and effect of crystallization time and si/al ratio during synthesis of zeolite ZSM-5. ChemCatChem 14:e202101248

    CAS  Google Scholar 

  • Kim S, Park G, Woo MH, Kwak G, Kim SK (2019) Control of hierarchical structure and framework-Al distribution of ZSM-5 via adjusting crystallization temperature and their effects on methanol conversion. Acs Catal 9:2880–2892

    CAS  Google Scholar 

  • Kohse-Hoinghaus K (2023) Combustion, chemistry, and carbon neutrality. Chem Rev 123:5139–5219

    Google Scholar 

  • Le TT, Qin W, Agarwal A, Nikolopoulos N, Fu D, Patton MD, Weiland C, Bare SR, Palmer JC, Weckhuysen BM, Rimer JD (2023) Elemental zoning enhances mass transport in zeolite catalysts for methanol to hydrocarbons. Nat Catal 6:254–265

    CAS  Google Scholar 

  • Lim LH, Tan P, Chan WP, Veksha A, Lim T-T, Lisak G, Liu W (2023) A techno-economic assessment of the reutilisation of municipal solid waste incineration ash for CO2 capture from incineration flue gases by calcium loo**. Chem Eng J 464:142567

    CAS  Google Scholar 

  • Liu X, Tu Y, Liu S, Liu K, Zhang L, Li G, Xu Z (2021) Adsorption of ammonia nitrogen and phenol onto the lignite surface: an experimental and molecular dynamics simulation study. J Hazard Mater 416:125966

    CAS  Google Scholar 

  • Liu Y, Wang Z, Zhao W, Hou J, Cui L, Zou L, Li C, Li H, Wu Y, Xu R, Zhu Y (2023) Hierarchical porous nanosilica derived from coal gasification fly ash with excellent CO2 adsorption performance. Chem Eng J 455:140622

    CAS  Google Scholar 

  • Long Y, Yang P, Wang C, Wu W, Chen X, Liu W, Cao Z, Zhan X, Liu D, Huang W (2023) Peroxymonosulfate activation by iron-carbon composite derived from coal gasification slag for sulfamethoxazole removal: performance evaluation and mechanism insight. Chem Eng J 456:140996

    CAS  Google Scholar 

  • Lv B, Deng X, Jiao F, Dong B, Fang C, **ng B (2023) Enrichment and utilization of residual carbon from coal gasification slag: a review. Process Saf Environ 171:859–873

    CAS  Google Scholar 

  • Magnuson JK, Weiksnar KD, Patel AD, Clavier KA, Ferraro CC, Townsend TG (2023) Processing municipal solid waste incineration bottom ash for integration into cement product manufacture. Resour Conserv Recy 198:107139

    Google Scholar 

  • Miao Z, Wu J, Niu Y, Guo Z, Guo F, Zhang Y (2022) Development of a novel type hierarchical porous composite from coal gasification fine slag for CO2 capture. Chem Eng J 435:134909

    CAS  Google Scholar 

  • Mirshafiee F, Khoshbin R, Karimzadeh R (2022) A green approach for template free synthesis of beta zeolite incorporated in ZSM-5 zeolite to enhance catalytic activity in MTG reaction: effect of seed nature and temperature. J Clean Prod 361:132159

    CAS  Google Scholar 

  • Mohamed HO, Parsapur RK, Hita I, Cerrillo JL, Ramírez A, Huang K-W, Gascon J, Castaño P (2022) Stable and reusable hierarchical ZSM-5 zeolite with superior performance for olefin oligomerization when partially coked. Appl Catal B Environ 316:121582

    CAS  Google Scholar 

  • Qiao Q, Zhou H, Guo F, Shu R, Liu S, Xu L, Dong K, Bai Y (2022) Facile and scalable synthesis of mesoporous composite materials from coal gasification fine slag for enhanced adsorption of malachite green. J Clean Prod 379:134739

    CAS  Google Scholar 

  • Ren L, Ding L, Guo Q, Gong Y, Yu G, Wang F (2023) Characterization, carbon-ash separation and resource utilization of coal gasification fine slag: a comprehensive review. J Clean Prod 398:136554

    CAS  Google Scholar 

  • Salem KS, Clayson K, Salas M, Haque N, Rao R, Agate S, Singh A, Levis JW, Mittal A, Yarbrough JM, Venditti R, Jameel H, Lucia L, Pal L (2023) A critical review of existing and emerging technologies and systems to optimize solid waste management for feedstocks and energy conversion. Matter 6:3348–3377

    Google Scholar 

  • Shi D, Zhang J, Hou X, Li S, Li H, He F, Zhu G (2022) Occurrence mode and molecular structure model of unburned carbon in coal gasification fine slags. Fuel 323:124364

    CAS  Google Scholar 

  • Sun X, Yi Y (2022) Utilization of incineration bottom ash, waste marine clay, and ground granulated blast-furnace slag as a construction material. Resour Conserv Recy 182:106292

    CAS  Google Scholar 

  • Tang Y, Guo X, **e Q, Finkelman RB, Han S, Huan B, Pan X (2018) Petrological characteristics and trace element partitioning of gasification residues from slagging entrained-flow gasifiers in Ningdong, China. Energ Fuel 32:3052–3067

    CAS  Google Scholar 

  • Tian X, Chen Z, Hou J, Li Z (2022) Sustainable utilization method of using coal gasification fine ash to prepare activated carbon for supercapacitor. J Clean Prod 363:132524

    CAS  Google Scholar 

  • Wang B, Zhang X, Liu Y, Li D, Lin Y (2022) Basic intensity regulation of layered double oxide for CO2 adsorption process at medium temperature in coal gasification. Chem Eng J 446:136842

    CAS  Google Scholar 

  • Wang Y, Zhang Z, Li L, Guo X, Wei D, Kong J, Du H, Wang H, Zhuang Y, **ng P (2023) A novel process to recycle coal gasification fine slag by preparing Si-Fe-Al-Ca alloy. J Environ Manage 337:117681

    CAS  Google Scholar 

  • Wu S, Huang S, Ji L, Wu Y, Gao J (2014) Structure characteristics and gasification activity of residual carbon from entrained-flow coal gasification slag. Fuel 122:67–75

    CAS  Google Scholar 

  • Xu L, Dong K, Guo F, Liu S, Qiao Q, Mao S, Qian L, Bai Y (2023) Synthesis of zeolite-based porous catalysts from coal gasification fine slag for steam reforming of toluene. Energy 274:127294

    CAS  Google Scholar 

  • Xue Z, Yang C, Dong L, Bao W, Wang J, Fan P (2023) Recent advances and conceptualizations in process intensification of coal gasification fine slag flotation. Sep Purif Technol 304:122394

    CAS  Google Scholar 

  • Yang D, Li S, He S, Zheng Y (2022) Can conversion of CO2 into fuels via electrochemical or thermochemical reduction be energy efficient and reduce emissions? Energ Convers Manag 273:116425

    CAS  Google Scholar 

  • Yuan N, Tan K, Zhang X, Zhao A, Guo R (2022) Synthesis and adsorption performance of ultra-low silica-to-alumina ratio and hierarchical porous ZSM-5 zeolites prepared from coal gasification fine slag. Chemosphere 303:134839

    CAS  Google Scholar 

  • Yue Q, Liu C, Zhao H, Liu H, Ruterana P, Zhao J, Qin Z, Mintova S (2023) Urea-assisted morphological engineering of MFI nanosheets with tunable b-thickness. Nano Res 16:12196–12206

    CAS  Google Scholar 

  • Zagorščak R, Metcalfe R, Limer L, Thomas H, An N, Bond A, Watson S (2022) Risk assessment methodology for underground coal gasification technology. J Clean Prod 370:133493

    Google Scholar 

  • Zhang C, Li S, Bao S (2018) Sustainable synthesis of ZSM-5 zeolite from rice husk ash without addition of solvents. Waste Biomass Valori 10:2825–2835

    Google Scholar 

  • Zhou Y, Deng Q, Deng D, Liu W, Zhai M, Wang Z, Han L, Zhu K (2023) Multiscale structural control of MFI zeolite using poly-quaternary ammonium cation. J Mater Chem A 11:15702–15716

    CAS  Google Scholar 

Download references

Funding

This study is supported by the Natural Science Foundation of Ningxia Province, China (2023AAC02008) and the National Natural Science Foundation of China (22366031).

Author information

Authors and Affiliations

Authors

Contributions

Lu Ma: Conceptualization, data curation, writing—original draft. Kangning Li: Visualization, software, investigation. Yi **ao: Writing—review and editing. Keren Shi: Software, formal analysis. Yulin Ma: Resources, validation. Mei Yang: Investigation, software. Yifei Yang: Resources, visualization. Yuanyuan Li: Supervision, writing—review and editing. Yulong Ma: Writing—review and editing. Yonggang Sun: Writing—review and editing. Wenxin Ji: Methodology, supervision, writing—review and editing.

Corresponding author

Correspondence to Wenxin Ji.

Ethics declarations

Ethics approval and consent to participate

This article does not contain any studies involving animals or human participants performed by any of the authors. We confirm the ethics approval. All the authors and contributors have consented for this article.

Consent for publication

All authors and contributors have consent to publish in this journal.

Competing interests

The authors declare no competing interests.

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.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 24 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, L., Li, K., **ao, Y. et al. Hydrothermal synthesis of high crystallinity ZSM-5 zeolite from coal gasification coarse slag and mother liquor circulation for efficient coal chemical wastewater purification. Environ Sci Pollut Res 31, 36849–36860 (2024). https://doi.org/10.1007/s11356-024-33264-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-024-33264-3

Keywords

Navigation