Layered Double Hydroxides as Rising-Star Adsorbents for Water Purification: A Brief Discussion
Abstract
:1. General Background
- (1)
- Physical adsorption. LDHs can have a high specific surface area, and hence present high adsorption capacities due to the presence and availability of active adsorption sites. Furthermore, the specific surface area of LDHs can be increased through calcinating or modifying/depositing on supports with three-dimensional structures.
- (2)
- Ion exchange. Strongly negative molecules can be easily changed for the original anions in LDHs. In addition, positive ions can also be exchanged in the intermediate layer of LDHs, if pre-interleaved by some chelators.
- (3)
- Interleaving. This starts from a preparation process, such as co-precipitation. Furthermore, the capture of molecules via the intercalation process is faster and more complete than ion exchange.
2. LDHs Physicochemical Characteristics
- (i)
- Direct methods: The preparation of LDHs occurs via direct precipitation from the addition of tri- and divalent cations, in a solution in alkaline pH with the main methods of coprecipitation, salt–oxide, sol–gel, induced hydrolysis, and hydrothermal synthesis.
- (ii)
- Indirect methods: involve replacing an interlamellar anion from a previously produced precursor LDH. Examples of this substitution method are ion exchange in solution, ion exchange in acidic medium, double phase replacement, and regeneration through the delaminate precursor [35,36,37]. Therefore, the supramolecular structure, the facile manipulation of adsorption sites at the atomic scale, the versatility of compositions, in addition to the possibility of morphological manipulation create the possibility of tuning the amount and accessibility of the active adsorption sites, and hence the adsorption kinetics, as well as the efficiency for a specifically targeted pollutant [34]. As in any case, LDHs have some specific characteristics that can complicate their use as adsorbents. The low mechanical resistance is a problem for continuous water treatment units and in certain regeneration processes, as LDHs can be exfoliated. Therefore, there is a series of studies in the literature proposing to support LDHs in larger and recalcitrant particles [38,39,40]. In addition, in acidic media, the removal capacity of LDHs is compromised due to low structural stability at low pH [26]. In Table 2, we collected characteristics of methods of synthesis which can be followed for the preparation of pure LDHs, as well as their composites and hybrids [18,25,41,42].
3. LDHs as Adsorbents
4. Discussion
5. Future Prospects
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Conflicts of Interest
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Advantages | Disadvantages |
---|---|
Low cost | Few studies regarding their toxicity in the environment |
Sustainable nature | Current methods limit the amount of LDHs produced |
Can be engineered for specific purposes | Few studies on its application in real wastewater |
Excellent thermal stability | Functional groups preferences for anionic dyes |
High removal efficiency | Can be exfoliated during synthesis |
Extensive specific surface area | Cannot be easily regenerated/reused |
High number of active sites | |
Easy to prepare | |
Memory effect | |
High anion exchange capacities | |
Chemical stability |
Methods of Synthesis | Characteristics |
---|---|
Coprecipitation | This method is based on the controlled and slow addition of a base (such as sodium hydroxide and/or bicarbonate, sodium carbonate or ammonium hydroxide) to a solution containing simultaneous divalent and trivalent metal cations. Since more than two cations can precipitate simultaneously, the process must be carried out under supersaturation conditions. It is recommended that the pH of the reaction medium be kept constant in the range of 7–10. Subsequently, the suspension is subjected to hydrothermal treatment to increase the yield or crystallinity. |
Salt-oxide | This method was developed by Boehm in 1977 to prepare zinc and chromium LDHs, using an aqueous suspension of ZnO to react with excess CrCl3 in an aqueous solution. The salt–oxide method, in short, is a solid–liquid reaction in which the aqueous solution of the excess trivalent ion chloride salt is treated with an aqueous suspension of the divalent metal oxide. |
Sol-gel | This synthetic protocol is widely used for the preparation of a plethora of metal oxides due to the possible high efficiency and purity of the final material. One important advantage of this method is the variety of compositions obtained through temperature adjustment. This process consists of the constant agitation of the component that transforms sol to gel. This sol–gel transformation occurs during the strong acid hydrolysis of metallic precursors, predominately using a strong acid such chloric acid or nitric acid. After the formation of the gel, the material is filtered and washed with distilled water, and later with ethanol. |
Hydrothermal | The hydrothermal method is generally used when low-affinity anions need to be intercalated into the intermediate layers. This method uses gibbsite and brucite, double-layered hydroxide–deoxycholate intercalation compounds, which are not feasible to obtain easily via other syntheses. An aqueous suspension consists of two oxides, one trivalent metal ion and the other bivalent, which are placed in a pressurized container and subjected to hydrothermal treatment at high temperature for a few days. During this process, the hydrated amorphous precursor crystallizes in the presence of reactive basic oxide. |
Ion exchange | This is an indirect method usually applied to pre-synthesized LDHs. This method is used when the anions or the divalent/trivalent metal cations are unstable in the alkaline solution, or when the LDHs have a greater affinity for the guest anions than for the intercalated anions of a pre-synthesized LDH. An aqueous suspension of the LDH precursors/pre-synthesized is mixed with a large excess of the salt of the anion to be intercalated. The reaction is carried out under an inert atmosphere to avoid excess carbonate in the intermediate layers. It is recommended the reaction not occur at pH lower than 4, due to the anion interaction in the LDH layers being weaker and presenting a high temperature in this pH range. |
Regeneration/“memory effect” | One of the main properties of LDH is its ability to restructure. After being subjected to heat treatment or calcination (400 to 500 °C), the layered structure of LDH changes to mixed metallic oxides (water, anion, and hydroxyl groups are highlighted). When calcined LDH is placed in a solution containing guest anions, they can recover their original layered structure and form a new LDH phase. This procedure of retrieving its original form (rehydration) is called the “memory effect”, and must be carried out in an inert atmosphere, mostly comprised of nitrogen. |
Pollutant | LDH | Synthesis Method | qmax (mg·g−1) | Reference |
---|---|---|---|---|
Dye methyl orange | Mg-Al-Ds | Coprecipitation | 185.06 | [45] |
Mg-Al-CO3 | 97.50 | |||
Dye RB19 | MgCoAl-CO3-LDH | Coprecipitation | 367.93 | [18] |
Dye Congo red | Mg/Fe-LDHs | Precipitation | 9127.08 | [4] |
Pb2+ | Ca/Fe LDH-Cit(NC10%) | Precipitation | 110.00 | [48] |
Ca/Fe LDH-Cit(NC5%) | 56.00 | |||
Cr6+ | ZnNiCr-LDHs | Hydrothermal | 28.20 | [29] |
Cd2+ | MgAl-LDH (SA-LDH) | Coprecipitation | 60.00 | [16] |
Pb2+ | 243.66 | |||
Cu2+ | 95.55 | |||
Phosphate | Zr-LDH | Coprecipitation | 99.35 | [51] |
Zr-LDO | 80.33 | |||
Arsenate (mono) | Mg-Al LDHs-FHC | Hydrothermal | 56.30 | [17] |
Arsenate (mult) | 16.22 | |||
Phosphate (mono) | 33.21 | |||
Phosphate (mult) | 20.26 | |||
Nitrate | FeMgMn-LDH | Co-precipitation | 10.56 | [50] |
Diclofenac | ZnTiAl | Co-precipitation | 0.07 | [53] |
Salicylic acid | 0.01 | |||
Diclofenac | Zn-Al-LDH.xBi2O3 | Hydrothermal | 574.71 | [11] |
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Gama, B.M.V.d.; Selvasembian, R.; Giannakoudakis, D.A.; Triantafyllidis, K.S.; McKay, G.; Meili, L. Layered Double Hydroxides as Rising-Star Adsorbents for Water Purification: A Brief Discussion. Molecules 2022, 27, 4900. https://doi.org/10.3390/molecules27154900
Gama BMVd, Selvasembian R, Giannakoudakis DA, Triantafyllidis KS, McKay G, Meili L. Layered Double Hydroxides as Rising-Star Adsorbents for Water Purification: A Brief Discussion. Molecules. 2022; 27(15):4900. https://doi.org/10.3390/molecules27154900
Chicago/Turabian StyleGama, Brígida Maria Villar da, Rangabhashiyam Selvasembian, Dimitrios A. Giannakoudakis, Konstantinos S. Triantafyllidis, Gordon McKay, and Lucas Meili. 2022. "Layered Double Hydroxides as Rising-Star Adsorbents for Water Purification: A Brief Discussion" Molecules 27, no. 15: 4900. https://doi.org/10.3390/molecules27154900