Skip to main content
Log in

Synthesis and characterization of aluminum citrate compounds and evaluation of their influence on the formation of hydrogels based on polyacrylamide

  • Original Research
  • Published:
Iranian Polymer Journal Aims and scope Submit manuscript

Abstract

Aluminum citrate is used as a conformance control agent to improve oil production and excess water production. This paper discusses the formation of mono and polynuclear aluminum species from the synthesis of aluminum citrate and evaluates these compounds as crosslinkers in hydrogels for conformance control. The products obtained from the synthesis were characterized by Fourier-transform infrared spectrometry (FTIR), elemental analysis (CHN), scanning electron microscopy (SEM), and inductively coupled plasma–optical emission spectrometry (ICP-OES). The FTIR analyses indicated the presence of mononuclear aluminum citrate complexes at pH 3 and polynuclear species starting at pH 4. These results were corroborated by CHN and ICP-OES techniques, which revealed the variation of carbon, oxygen, hydrogen, and alumina precipitate levels as functions of pH variation. The focus of the study was to assess how these crosslinking agents perform in hydrogel formation under reservoir conditions. Rheological analysis showed that the values of tan (delta) of the hydrogel synthesized with aluminum citrate at pH 6 were lower than 0.1, indicating strong gels, while at pH 9, the values were above 0.1, indicating weak gels. These results are in agreement with those obtained by FTIR, which showed that at pH 6, the structures of the aluminum citrate complex were probably in the form [Al3(C6H5O7)3(OH)4(H2O)]4−. This structure appears to allow easier access to the aluminum orbital for the crosslinking process compared to the gel composed of aluminum citrate synthesized at pH 9 [Al3(C6H6O7)3(OH)4(H2O)5]4−.

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

Access this article

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

Similar content being viewed by others

References

  1. Chamberlain D (2007) Anion mediation of aluminium-catalysed degradation of paper. Polym Degrad Stabil 92:1417–1420

    Article  CAS  Google Scholar 

  2. Xu LQ, Neoh K, Kang E (2018) Natural polyphenols as versatile platforms for material engineering and surface functionalization. Prog Polym Sci 87:165–196

    Article  CAS  Google Scholar 

  3. Zhu G, Cui X, Zhang Y, Chen S, Dong M, Liu H, Shao Q, Ding T, Shide W, Guo Z (2019) Poly (vinyl butyral)/graphene oxide/poly (methylhydrosiloxane) nanocomposite coating for improved aluminum alloy anticorrosion. Polymer 172:415–422

    Article  CAS  Google Scholar 

  4. Li F, Koopal L, Tan W (2018) Effect of citrate on the species and levels of Al impurities in ferrihydrite. Colloid Surf A 539:140–147

    Article  CAS  Google Scholar 

  5. Rajalakshmi K, Siknam Y, Selvaraj M, Lee Y, Lee K (2018) Metal free bioimaging reagent for intracellular citrate in prostate cancer cells using aryl boronate derivative. Sens Actuators B Chem 259:90–96

    Article  CAS  Google Scholar 

  6. Ranjbar M, Salavati-Niasari M, Hosseinpour-Mashkani SM (2012) Microwave synthesis and characterization of spinel-type zinc aluminate nanoparticles. J Inorg Organomet Polym Mater 22:1093–1100

    Article  CAS  Google Scholar 

  7. Song P, Chen G, Wel Z, Chang Y, Zhang W, Liang J (2012) Rapid crystallization of poly(l-lactic acid) induced by a nanoscaled zinc citrate complex as nucleating agent. Polymer 53:4300–4309

    Article  CAS  Google Scholar 

  8. Mirzajani F, Rafati H, Atyabi F (2010) Fabrication of biodegradable poly(d, l-lactide-co-glycolide) nanoparticles containing tamoxifen citrate. Iran Polym J 19:437–446

    CAS  Google Scholar 

  9. Amir M, Baykal A, Güner S, Sertkol M, Sözeri H, Toprak M (2012) Synthesis and Characterization of CoxZn1−xAlFeO4 Nanoparticles. J Inorg Organomet Polm Mater 25:747–754

    Article  Google Scholar 

  10. Feng L, Bian X, Li G, Chen Z, Cui Y, Chen X (2013) Determination of ultra-low glass transition temperature via differential scanning calorimetry. Polym Test 32:1368–1372

    Article  CAS  Google Scholar 

  11. Feng IL, Gurian PL, Healy MD, Barron AR (1990) Aluminum citrate: isolation and structural characterization of a stable trinuclear complex. Inorg Chem 29:408–411

    Article  CAS  Google Scholar 

  12. Wang J, Liu S, Mu Y, Yang L, Yang J, Feng S, Shi M, Yang W, Fu W, Yang H (2018) Sodium citrate complexing agent-dependent growth of n- and p-type CdTe thin films for applications in CdTe/CdS based photovoltaic devices. J Alloy Compd 748:515–521

    Article  CAS  Google Scholar 

  13. Raju U, Warkar SG, Kuma A (2017) Green synthesis of multi metal-citrate complexes and their characterization. J Mol Struct 1133:90–94

    Article  CAS  Google Scholar 

  14. Staal PW (1984) Method for the preparation of liquid aluminum citrate US4447364

  15. Stavlanda A, Carlsenh H (1996) New insight into aluminium citrate/polyacrylamide gels for fluid control. SPE. https://doi.org/10.2118/35381-MS

    Article  Google Scholar 

  16. Matzapetakis M, Raptopoulou CP, Terzis A, Lakatos A, Kiss T, Salifoglou A (1999) Synthesis, pH-dependent structural characterization, and solution behavior of aqueous aluminum and gallium citrate complexes. Inorg Chem 38:618–619

    Article  CAS  Google Scholar 

  17. Silva AF, Aguiar MSS, Carvalho OS, Santana LNS, Leal WG (2013) Hippocampal neuronal loss, decreased GFAP immunoreactivity and cognitive impairment following experimental intoxication of rats with aluminum citrate. Brain Res J 1491:23–33

    Article  CAS  Google Scholar 

  18. Ren X, Hu X, Xue D, Li Y, Shao Z, Dong H, Cheng W, Zhao Y, Xin L, Lu W (2019) Novel sodium silicate/polymer composite gels for the prevention of spontaneous combustion of coal. J Hazar Mater 371:643–654

    Article  CAS  Google Scholar 

  19. Karimi S, Kazemi S, Kazemi N (2016) Syneresis measurement of the HPAM-Cr (III) gel polymer at different conditions: an experimental investigation. J Nat Gas Sci Eng 34:1027–1033

    Article  CAS  Google Scholar 

  20. Bai Y, Xiong C, Wei F, Li J, Shu Y, Liu D (2015) Gelation study on a hydrophobically associating polymer/polyethylenimine gel system for water shut-off treatment. Energy Fuel 29:447–458

    Article  CAS  Google Scholar 

  21. Qiu L, Shen Y, Wang C, Yang X (2018) Scanning electron microscopy analysis of guar gum in the dissolution, gelation and gel-breaking process. Polym Test 68:95–99

    Article  CAS  Google Scholar 

  22. Ren X, Hu X, Cheng W, Bian S, Zhao Y, Wu M, Xue D, Li Y, Lu W, Wang P (2020) Study of resource utilization and fire prevention characteristics of a novel gel formulated from coal mine sludge (MS). Fuel 267:117261. https://doi.org/10.1016/j.fuel.2020.117261

    Article  CAS  Google Scholar 

  23. Smith JE (1997) Permeability modifying composition for use in oil recovery.US 5654261 A

  24. Moradi-Araghi A (2000) A review of thermally stable gels for fluid diversion in petroleum production. J Petrol Sci Eng 26:1–10

    Article  CAS  Google Scholar 

  25. Smith JE, Liu H, Guo ZD (2000) Laboratory studies of in-depth colloidal dispersion gel technology for daqing oil field. SPE. https://doi.org/10.2118/62610-MS

    Article  Google Scholar 

  26. Aksoy G, Gomaa AM, Nasr-El-Din HA, Wang X, Boles JL, Cawiezel KE (2011) Evaluation of a new liquid breaker for polymer based in situ gelled acids. SPE. https://doi.org/10.2118/143447-MS

    Article  Google Scholar 

  27. Jia H, Chen H (2018) Using DSC technique to investigate the non-isothermal gelation kinetics of the multi-crosslinked Chromium acetate (Cr3+)-polyethyleneimine (PEI)-polymer gel sealant. J Petrol Sci Eng 165:105–113

    Article  CAS  Google Scholar 

  28. Bjϕrsvik M, Høiland H, Skauge A (2008) Formation of colloidal dispersion gels from aqueous polyacrylamide solutions. Colloid Surf A 317:504–511

    Article  Google Scholar 

  29. Bodor A, Bányai L, Zélánk L, Tóth I (2002) Slow dynamics of aluminum-citrate complexes studied by 1H- and 13C-NMR spectroscopy. Coord Chem Rev 28:163–173

    Article  Google Scholar 

  30. Hacht B (2008) Speciation studies of aluminium(III)–acetate complexes under physiological conditions. Chem Spec Bioavailab 20:2047–6523

    Article  Google Scholar 

  31. Groen H, Ronerts KJ (2001) Nucleation, growth, and pseudo-polymorphic behavior of citric acid as monitored in situ by attenuated total reflection Fourier transform infrared spectroscopy. J Phys Chem B 105:10723–10730

    Article  CAS  Google Scholar 

  32. Clausen M, Ohman L, Persson P (2005) Spectroscopic studies of aqueous gallium(III) and aluminum(III) citrate complexes. J Inorg Biochem 99:716–726

    Article  CAS  Google Scholar 

  33. Peukert A, Seubert A (2009) Characterization of an aluminium(III)-citrate species by means of ion chromatography with inductively coupled plasma-atomic emission spectrometry detection. J Chromatogr A 45:1216

    Google Scholar 

  34. Ross-Marphy SB (1994) Rheological characterization of polymer gels and networks. Polym Gels Netw 2:229–237

    Article  Google Scholar 

  35. Wang S, Tang H, Guo J, Wang K (2016) Effect of pH on the rheological properties of borate crosslinked hydroxypropyl guar gum hydrogel and hydroxypropyl guar gum. Carbohyd Polym 147:455–463

    Article  CAS  Google Scholar 

  36. Tessarolli FGC, Queirós YGC, Mansur CRE (2014) Evaluation of pH-sensitive hydrogels to control the permeability anisotropy of oil reservoirs. J Appl Polym Sci. https://doi.org/10.1002/app.40665

    Article  Google Scholar 

  37. Oliveira PF, Costa JÁ, Oliveira LFS, Mota LS, Oliveira LA, Mansur CRE (2019) Hydrolysis and thermal stability of partially hydrolyzed polyacrylamide in high-salinity environments. J Appl Polym. https://doi.org/10.1002/app.47793

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPQ), Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)-Financie Code 001, Fundação Carlos Chagas Filho de Amparo à Pesquisa do Estado do Rio de Janeiro (FAPERJ), and Petrobras.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Claudia R. E. Mansur.

Ethics declarations

Conflict of interest

The authors declare no conflicts of interest.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Fraga, A.K., Oliveira, P.F., das Dores, F.G.L. et al. Synthesis and characterization of aluminum citrate compounds and evaluation of their influence on the formation of hydrogels based on polyacrylamide. Iran Polym J 29, 649–657 (2020). https://doi.org/10.1007/s13726-020-00825-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s13726-020-00825-5

Keywords

Navigation