Research Progress on the Hydrolysis-Polymerization Forms and Mechanisms of Aluminum

doi:10.19894/j.issn.1000-0518.240377

Chinese Journal of Applied Chemistry ›› 2025, Vol. 42 ›› Issue (4): 466-479.DOI: 10.19894/j.issn.1000-0518.240377

• Review • Previous Articles

Research Progress on the Hydrolysis-Polymerization Forms and Mechanisms of Aluminum

Hui LI, Zhi-Zhong XIE(), Ji FENG

School of Chemistry，Chemical Engineering and Life Sciences，Wuhan University of Technology，Wuhan 430070，China

Received:2024-11-20 Accepted:2025-03-10 Published:2025-04-01 Online:2025-05-14
Contact: Zhi-Zhong XIE
Supported by:
the Special Fund for Basic Scientific Research for Central Universities(2020IB027)

Abstract

Abstract:

The study of aluminum hydrolysis and polymerization forms has long been at the forefront of research in numerous fields， including analytical chemistry， materials science， geochemistry， environmental science and biotoxicology. Aluminum species are primarily categorized into three forms： monomeric hydroxyl species， polymeric hydroxyl species， and sol or gel species. Currently， the mainstream analytical methods for studying aluminum species include the Al-Ferron timed complexation colorimetric spectrophotometry， ²⁷Al nuclear magnetic resonance spectroscopy （²⁷Al NMR）， and electrospray ionization mass spectrometry （ESI-MS）. Among the polymeric aluminum species， the Keggin-structured polyaluminum chloride （Al₁₃） and polyaluminum （Al₃₀） species are particularly notable for their high positive charge density and stability， which hold significant importance for the development of inorganic polymer coagulants. This paper provides an overview of the distribution of aluminum hydrolysis species， the primary analytical methods for aluminum species， and the mechanisms of aluminum hydrolysis and polymerization. It also summarizes the formation mechanisms and research progress in the applications of Al₁₃ and Al₃₀ species， while offering insights into future research directions in aluminum hydrolysis and polymerization.

Key words: Aluminum hydrolysis-polymerization, Aluminum form analysis, Al₁₃, Al₃₀

CLC Number:

O635

Hui LI, Zhi-Zhong XIE, Ji FENG. Research Progress on the Hydrolysis-Polymerization Forms and Mechanisms of Aluminum[J]. Chinese Journal of Applied Chemistry, 2025, 42(4): 466-479.

Figures/Tables 13

Table 1 Aluminum ion hydrolysis acid dissociation constant［16］

Balanced reaction	pK_a
Al³⁺+H₂O=Al（OH）²⁺+H⁺	5.0
Al（OH）²⁺+H₂O=Al（OH） $_{2}^{+}$ +H⁺	5.5
Al（OH） $_{2}^{+}$ +H₂O=Al（OH）₃+H⁺	6.0
Al（OH）₃+H₂O=Al（OH） $_{4}^{-}$ +H⁺	8.5

Table 1 Aluminum ion hydrolysis acid dissociation constant［16］

Balanced reaction	pK_a
Al³⁺+H₂O=Al（OH）²⁺+H⁺	5.0
Al（OH）²⁺+H₂O=Al（OH） $_{2}^{+}$ +H⁺	5.5
Al（OH） $_{2}^{+}$ +H₂O=Al（OH）₃+H⁺	6.0
Al（OH）₃+H₂O=Al（OH） $_{4}^{-}$ +H⁺	8.5

Fig.1 Hydroxyl group morphology distribution of aluminum monomer at different pH values［17］

Fig.2 Al-Ferron reaction kinetic curve［28］

Fig.3 Representative 27Al NMR spectrum for PAC［45］

Table 2 The aluminum species and their corresponding ion peaks in the ESI-MS spectra of aluminum hydrolysis in PAC solutions［53］

Aluminum species	Molecular formula	Ion peak （m/z）
Al₁	Al（OH） $_{2}^{+}$ （H₂O） _n_=1、2	79，97
Al₂	Al₂O₂（OH）⁺（H₂O）_1-6	103，121，139，157，175，193，211，229，247
Al₃	Al₃O $_{4}^{+}$ （H₂O）_0-6	163，181，199，217，235，253，271
Al $_{13}^{3 +}$	Al₁₃O₁₈（OH） $_{0,2, 4 \dots, 20}^{3 +}$	213，219，225，231，237，243，249，255，261，267，279
Al $_{13}^{2 +}$	Al₁₃O₁₈（OH） $_{1,3, 5 \dots 19}^{2 +}$	328，337，346，355，364，373，382，391，400，409

Table 2 The aluminum species and their corresponding ion peaks in the ESI-MS spectra of aluminum hydrolysis in PAC solutions［53］

Aluminum species	Molecular formula	Ion peak （m/z）
Al₁	Al（OH） $_{2}^{+}$ （H₂O） _n_=1、2	79，97
Al₂	Al₂O₂（OH）⁺（H₂O）_1-6	103，121，139，157，175，193，211，229，247
Al₃	Al₃O $_{4}^{+}$ （H₂O）_0-6	163，181，199，217，235，253，271
Al $_{13}^{3 +}$	Al₁₃O₁₈（OH） $_{0,2, 4 \dots, 20}^{3 +}$	213，219，225，231，237，243，249，255，261，267，279
Al $_{13}^{2 +}$	Al₁₃O₁₈（OH） $_{1,3, 5 \dots 19}^{2 +}$	328，337，346，355，364，373，382，391，400，409

Table 3 Comparison of three analytical methods for aluminum species

Analytical methods	Advantage	Malpractices
Al-Ferron colorimetry^{［44，57］}	It can detect the aluminum form at low aluminum concentration； Low cost； The aluminum form can be distinguished by the reaction rate of the reagent.	It is not possible to accurately and qualitatively identify the type of aluminum.
²⁷Al NMR^［58-59］	It can quantitatively detect the form of aluminum； Fast， non-destructive， and accurate， suitable for solid and liquid samples.	At low Al_b concentrations， Al₁₃ could not be detected. Larger aluminum polymers are difficult to detect.
ESI-MS^［60］	At low concentrations， it can qualitatively and quantitatively detect a variety of aluminum forms.	The solution cannot be reacted in situ form.

Fig.4 The polymerization reaction model for Al3+ six-membered ring［13］

Fig.5 The structural model of Keggin-Al13［67］

Fig.6 The structural model for dimeric cation Al2（OH）2（H2O）84+［68］

Fig.7 Medium-rate base titration curve （c（AlCl3）=5×10-3 mol/L， c（NaOH）=0.01 mol/L， c（ion）=2×10-2 mol/L）［69］

Fig.8 The “Continuous” model of morphological changes under aluminum hydrolysis-polymerization［69］

Fig.9 The structural model for Al13 and the aggregation model of Al30［89］

Fig.10 The two formation mechanisms of Al30［78］

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Research Progress on the Hydrolysis-Polymerization Forms and Mechanisms of Aluminum

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