RESEARCH ARTICLE

Porous silica synthesis out of coal fly ash with no residue generation and complete silicon separation

  • Tongyao Ju ,
  • Siyu Han ,
  • Fanzhi Meng ,
  • Li Lin ,
  • Jinglin Li ,
  • Kailun Chen ,
  • Jianguo Jiang
Expand
  • School of Environment, Tsinghua University, Beijing 100084, China
jianguoj@tsinghua.edu.cn

Received date: 29 Jan 2023

Revised date: 16 Mar 2023

Accepted date: 16 Mar 2023

Copyright

2023 Higher Education Press

Highlights

● Both amorphous and crystalline silicon are completely separated from coal fly ash.

● Porous silica is synthesized out of coal fly ash.

● No residues is produced during the whole synthesis process.

● The one-step method to synthesize silica don’t need long-time reaction and aging.

Abstract

Ordered mesoporous silica materials exhibit enormous potential in industrial production. Since coal fly ash (CFA) is abundant in Si, it has become a green and promising way to utilize CFA by synthesizing porous silica materials. However, the stable crystalline structure of CFA limits the extraction of Si, and the residue is generated during the process of extracting Si. In this work, we proposed a no-residue method to synthesize ordered mesoporous silica out of CFA. Sodium carbonate (Na2CO3) was used to reconstruct the crystals of the CFA, and the calcined mixture then directly reacted with the precipitators. This method combined the process of Si extraction and porous material synthesis. In this method, no residue was generated and the silicon in both amorphous and crystalline phases of CFA was fully utilized. By this method, the extraction efficiency of Si was increased from 31.75% to nearly 100%. The as-synthesized mesoporous silica had a highly-ordered pore structure with a space group of la-3d, a surface area of 663.87 m2/g, a pore volume of 0.41 cm3/g, and an average pore diameter of 2.73 nm. The mechanism of crystalline transformation and material structure formation were systematically studied. This method provides a new idea to dispose of CFA and synthesize porous silica materials.

Cite this article

Tongyao Ju , Siyu Han , Fanzhi Meng , Li Lin , Jinglin Li , Kailun Chen , Jianguo Jiang . Porous silica synthesis out of coal fly ash with no residue generation and complete silicon separation[J]. Frontiers of Environmental Science & Engineering, 2023 , 17(9) : 112 . DOI: 10.1007/s11783-023-1712-2

Acknowledgements

We are thankful to the financial support by the National Natural Science Foundation of China (No. 22176108).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-023-1712-2 and is accessible for authorized users.
1
Akpotu S O , Moodley B . (2018). MCM-48 encapsulated with reduced graphene oxide/graphene oxide and as-synthesised MCM-48 application in remediation of pharmaceuticals from aqueous system. Journal of Molecular Liquids, 261: 540–549

DOI

2
Ameh A E , Musyoka N M , Oyekola O , Louis B , Petrik L F . (2021). Acylation of anisole with benzoyl chloride over rapidly synthesized fly ash-based HBEA zeolite. Frontiers in Chemistry, 9: 683125

DOI

3
Azizi D , Ibsaine F , Dionne J , Pasquier L C , Coudert L , Blais J F . (2021). Microporous and macroporous materials state-of-the-art of the technologies in zeolitization of aluminosilicate bearing residues from mining and metallurgical industries: a comprehensive review. Microporous and Mesoporous Materials, 318: 111029

DOI

4
Basumatary A K , Kumar R V , Ghoshal A K , Pugazhenthi G . (2016). Removal of FeCl3 from aqueous solution by ultrafiltration using ordered mesoporous MCM-48 ceramic composite membrane. Separation Science and Technology, 51(12): 2038–2046

DOI

5
Boycheva S , Marinov I , Miteva S , Zgureva D . (2020). Conversion of coal fly ash into nanozeolite Na-X by applying ultrasound assisted hydrothermal and fusion-hydrothermal alkaline activation. Sustainable Chemistry and Pharmacy, 15: 100217

DOI

6
Boycheva S , Zgureva D , Vaclavikova M , Kalvachev Y , Lazarova H , Popova M . (2019). Studies on non-modified and copper-modified coal ash zeolites as heterogeneous catalysts for VOCs oxidation. Journal of Hazardous Materials, 361: 374–382

DOI

7
Carvalho G C , Marena G D , Karnopp J C F , Jorge J , Sabio R M , Martines M A U , Bauab T M , Chorilli M . (2022). Cetyltrimethylammonium bromide in the synthesis of mesoporous silica nanoparticles: general aspects and in vitro toxicity. Advances in Colloid and Interface Science, 307: 102746

DOI

8
Chen Y , Cong S , Wang Q , Han H , Lu J , Kang Y , Kang W , Wang H , Han S , Song H , Zhang J . (2018). Optimization of crystal growth of sub-micron ZSM-5 zeolite prepared by using Al(OH)3 extracted from fly ash as an aluminum source. Journal of Hazardous Materials, 349: 18–26

DOI

9
Costa J A S , de Jesus R A , Santos D O , Mano J F , Romão L P C , Paranhos C M . (2020). Recent progresses in the adsorption of organic, inorganic, and gas compounds by MCM-41-based mesoporous materials. Microporous and Mesoporous Materials, 291: 109698

DOI

10
Costa J A S , Paranhos C M . (2020). Mitigation of silica-rich wastes: an alternative to the synthesis eco-friendly silica-based mesoporous materials. Microporous and Mesoporous Materials, 309: 110570

DOI

11
de Oliveira F F , Moura K O , Costa L S , Vidal C B , Loiola A R , Do Nascimento R F . (2020). Reactive adsorption of parabens on synthesized micro- and mesoporous silica from coal fly ash: pH effect on the modification process. ACS Omega, 5(7): 3346–3357

DOI

12
Faghihian H , Nasri Nasrabadi S , Khonsari S . (2014). Removal of Sr(II) from aqueous solutions by aminosilane functionalized MCM-48. Separation Science and Technology, 49(13): 2031–2038

DOI

13
Guo Y , Li Y , Cheng F , Wang M , Wang X . (2013). Role of additives in improved thermal activation of coal fly ash for alumina extraction. Fuel Processing Technology, 110: 114–121

DOI

14
Guo Y , Zhao Z , Zhao Q , Cheng F . (2017). Novel process of alumina extraction from coal fly ash by pre-desilicating–Na2CO3 activation–acid leaching technique. Hydrometallurgy, 169: 418–425

DOI

15
Gupta P K , Mahato A , Oraon P , Gupta G K , Maity S . (2020). Coal fly ash-derived mesoporous SBA-15 as support material for production of liquid hydrocarbon through Fischer–Tropsch route. Asia-Pacific Journal of Chemical Engineering, 15(4): e2471

DOI

16
Han Y , Han S , Kim S , Jung M , Jeon H S , Choi S Q , Kim K , Kim Y . (2021). Mesoporous silica derived from municipal solid waste incinerator (MSWI) ash slag: synthesis, characterization and use as supports for Au(III) recovery. Materials (Basel), 14(22): 6894

DOI

17
He Y , Zhang L , An X , Han C , Luo Y . (2019). Microwave assistant rapid synthesis MCM-41–NH2 from fly ash and Cr(VI) removal performance. Environmental Science and Pollution Research International, 26(30): 31463–31477

DOI

18
Heo Y J , Le M U T. , Park S J . (2016). Investigation of carbon dioxide adsorption by nitrogen-doped carbons synthesized from cubic MCM-48 mesoporous silica. Carbon letters, 18: 62–66

DOI

19
Hossini Asl S M , Masomi M , Tajbakhsh M . (2020). Hybrid adaptive neuro-fuzzy inference systems for forecasting benzene, toluene & m-xylene removal from aqueous solutions by HZSM-5 nano-zeolite synthesized from coal fly ash. Journal of Cleaner Production, 258: 120688

DOI

20
Jin Z , Xu Y , Lin S , Sheng J . (2016). Cubic mesoporous silica material as a highly efficient solid phase extraction sorbent for bisphenol A, tert-nonylphenol from water. Journal of Nanoscience and Nanotechnology, 16(6): 5833–5838

DOI

21
Ju T , Han S , Meng Y , Jiang J . (2021a). High-end reclamation of coal fly ash focusing on elemental extraction and synthesis of porous materials. ACS Sustainable Chemistry & Engineering, 9(20): 6894–6911

DOI

22
Ju T , Jiang J , Meng Y , Yan F , Xu Y , Gao Y , Aihemaiti A . (2020). An investigation of the effect of ultrasonic waves on the efficiency of silicon extraction from coal fly ash. Ultrasonics Sonochemistry, 60: 104765

DOI

23
Ju T , Meng Y , Han S , Lin L , Jiang J . (2021b). On the state of the art of crystalline structure reconstruction of coal fly ash: a focus on zeolites. Chemosphere, 283: 131010

DOI

24
Lázaro A L , Rodríguez-Valadez F J , López J J M , Espejel-Ayala F . (2020). SBA-15 synthesis from sodium silicate prepared with sand and sodium hydroxide. Materials Research Express, 7(4): 045503

DOI

25
Li C C , Qiao X C . (2016). A new approach to prepare mesoporous silica using coal fly ash. Chemical Engineering Journal, 302: 388–394

DOI

26
Li L , Shi Q , Huang L , Yan C , Wu Y . (2021). Green synthesis of faujasite-La0.6Sr0.4Co0.2Fe0.8O3-δ mineral nanocomposite membrane for low temperature advanced fuel cells. International Journal of Hydrogen Energy, 46(15): 9826–9834

DOI

27
Liu L , Zhu G , Liu Z , Gao C . (2016). Effect of MCM-48 nanoparticles on the performance of thin film nanocomposite membranes for reverse osmosis application. Desalination, 394: 72–82

DOI

28
Machado S W M , Santana J C , Pedrosa A M G , Souza M J B , Coriolano A C F , Morais E K L , Araujo A S . (2018). Catalytic cracking of isopropylbenzene over hybrid HZSM-12/M41S (M41S = MCM-41 or MCM-48) micro-mesoporous materials. Petroleum Science and Technology, 36(13): 923–929

DOI

29
Miao C , Liang L , Zhang F , Chen S , Shang K , Jiang J , Zhang Y , Ouyang J . (2022). Review of the fabrication and application of porous materials from silicon-rich industrial solid waste. International Journal of Minerals Metallurgy and Materials, 29(3): 424–438

DOI

30
Miricioiu M G , Niculescu V C . (2020). Fly ash, from recycling to potential raw material for mesoporous silica synthesis. Nanomaterials (Basel, Switzerland), 10(3): 474–487

DOI

31
Miricioiu M G , Niculescu V C , Filote C , Raboaca M S , Nechifor G . (2021). Coal fly ash derived silica nanomaterial for MMMs-application in CO2/CH4 separation. Membranes (Basel), 11(2): 78

DOI

32
Muir B , Sobczyk M , Bajda T . (2021). Fundamental features of mesoporous functional materials influencing the efficiency of removal of VOCs from aqueous systems: a review. Science of the Total Environment, 784: 147121

DOI

33
Peng X . (2019). Dynamic hydrothermal synthesis of xonotlite fibers by alkali silica extraction of fly ash. Journal of Engineered Fibers and Fabrics, 14: 1–5

DOI

34
Peron D V , Zholobenko V L , De Melo J H S , Capron M , Nuns N , De Souza M O , Feris L A , Marcilio N R , Ordomsky V V , Khodakov A Y . (2019). External surface phenomena in dealumination and desilication of large single crystals of ZSM-5 zeolite synthesized from a sustainable source. Microporous and Mesoporous Materials, 286: 57–64

DOI

35
Qian Y , Zhang H , Li L , Duan Y . (2020). Optimization of crystal growth of hierarchical porosity ZSM-5 zeolite based on coal fly ash “waste utilization”. Materialwissenschaft und Werkstofftechnik, 51(9): 1295–1303

DOI

36
Rehman W U , Wang H , Manj R Z A , Luo W , Yang J . (2021). When silicon materials meet natural sources: opportunities and challenges for low-cost lithium storage. Small, 17(9): e1904508

DOI

37
Sayehi M , Tounsi H , Garbarino G , Riani P , Busca G . (2020). Reutilization of silicon- and aluminum- containing wastes in the perspective of the preparation of SiO2-Al2O3 based porous materials for adsorbents and catalysts. Waste Management (New York, N.Y.), 103: 146–158

DOI

38
Shaban M , Hamd A , Amin R R , Abukhadra M R , Khalek A A , Khan A A P , Asiri A M . (2020). Preparation and characterization of MCM-48/nickel oxide composite as an efficient and reusable catalyst for the assessment of photocatalytic activity. Environmental Science and Pollution Research International, 27(26): 32670–32682

DOI

39
Sikarwar P , Kumar U K A , Gosu V , Subbaramaiah V . (2018). Catalytic oxidative desulfurization of DBT using green catalyst (Mo/MCM-41) derived from coal fly ash. Journal of Environmental Chemical Engineering, 6(2): 1736–1744

DOI

40
Taggart R K , Hower J C , Hsu-Kim H . (2018). Effects of roasting additives and leaching parameters on the extraction of rare earth elements from coal fly ash. International Journal of Coal Geology, 196: 106–114

DOI

41
Tang M , Zhou C , Pan J , Zhang N , Liu C , Cao S , Hu T , Ji W . (2019a). Study on extraction of rare earth elements from coal fly ash through alkali fusion – acid leaching. Minerals Engineering, 136: 36–42

DOI

42
Tang M , Zhou C , Zhang N , Pan J , Cao S , Hu T , Ji W , Wen Z , Nie T . (2019b). Extraction of rare earth elements from coal fly ash by alkali fusion–acid leaching: mechanism analysis. International Journal of Coal Preparation and Utilization, 42(3): 536–555

DOI

43
Wang B , Zhou Y , Li L , Wang Y . (2018a). Preparation of amidoxime-functionalized mesoporous silica nanospheres (ami-MSN) from coal fly ash for the removal of U(VI). Science of the Total Environment, 626: 219–227

DOI

44
Wang B , Zhou Y , Li L , Xu H , Sun Y , Du Y , Wang Y . (2018b). In situ synthesis of TiO2-doped mesoporous silica from coal fly ash for the photocatalytic degradation of dyes. Industrial & Engineering Chemistry Research, 57(46): 15632–15637

DOI

45
Wang B , Zhou Y , Li L , Xu H , Sun Y , Wang Y . (2018c). Novel synthesis of cyano-functionalized mesoporous silica nanospheres (MSN) from coal fly ash for removal of toxic metals from wastewater. Journal of Hazardous Materials, 345: 76–86

DOI

46
Wu Y H , Ma Y L , Sun Y G , Xue K , Ma Q L , Ma T , Ji W X . (2020). Graded synthesis of highly ordered MCM-41 and carbon/zeolite composite from coal gasification fine residue for crystal violet removal. Journal of Cleaner Production, 277: 123186

DOI

47
Yadav V K , Fulekar M H . (2020). Advances in methods for recovery of ferrous, alumina, and silica nanoparticles from fly ash waste. Ceramics, 3(3): 384–420

DOI

48
Yan F , Jiang J , Tian S , Liu Z , Shi J , Li K , Chen X , Xu Y . (2016). A green and facile synthesis of ordered mesoporous nanosilica using coal fly ash. ACS Sustainable Chemistry & Engineering, 4(9): 4654–4661

DOI

49
Yang G , Ren Q , Xu J , Lyu Q . (2021). Co-melting properties and mineral transformation behavior of mixtures by MSWI fly ash and coal ash. Journal of the Energy Institute, 96: 148–157

DOI

50
Yang T , Han C , Liu H , Yang L , Liu D , Tang J , Luo Y . (2019a). Synthesis of Na-X zeolite from low aluminum coal fly ash: characterization and high efficient As(V) removal. Advanced Powder Technology, 30(1): 199–206

DOI

51
Yang X , Tang W , Liu X , Du H , Wu Y , Zhang J . (2019b). Synthesis of mesoporous silica from coal slag and CO2 for phenol removal. Journal of Cleaner Production, 208: 1255–1264

DOI

52
Yao Z T , Xia M S , Sarker P K , Chen T . (2014). A review of the alumina recovery from coal fly ash, with a focus in China. Fuel, 120: 74–85

DOI

53
Yu Y , Li X , Zou X , Zhu X . (2014). Effect of seawater salinity on the synthesis of zeolite from coal fly ash. Frontiers of Environmental Science & Engineering, 8(1): 54–61

DOI

54
Yuan N, Cai H, Liu T, Huang Q, Zhang X (2019). Adsorptive removal of methylene blue from aqueous solution using coal fly ash-derived mesoporous silica material. Adsorption Science and Technology, 37(3–4): 333–348

DOI

55
Zhang M , Chen C , Wang X , Li A . (2021a). Extraction of aluminum from coal fly ash sintering-acid leaching process. Chinese Journal of Envrionmental Engineering, 15(7): 2389–2397

DOI

56
Zhang X , Du T , Jia H . (2021b). Efficient activation of coal fly ash for silica and alumina leaches and the dependence of Pb(II) removal capacity on the crystallization conditions of Al-MCM-41. International Journal of Molecular Sciences, 22(12): 6540

DOI

57
Zhou B , Zhou J , Hu T , Yang L , Lin G , Zhang L . (2018). Phase transformation mechanism in activation of high-alumina fly ash with Na2CO3. Materials Research Express, 6(1): 015502

DOI

58
Zhou T , Liu Y , Xiao X , Xu X , Dou J . (2022). Synthesis of NaHS zeolite using microwave assisted alkali activation of coal fly ash: preparation, mechanism, application. Energy Sources. Part A, Recovery, Utilization, and Environmental Effects, 44(4): 10506–10517

DOI

Outlines

/