Synthesis of phillipsite from perlite utilizing mother waters from wet gel EMT preparation and study of the obtained zeolitic material as ion exchanger

Abstract

In the present paper, a supplementary method was elaborated for synthesis of phillipsite from perlite utilizing mother waters from wet gel EMT preparation. The method is reproducible and cheap—synthesis was performed at mild conditions at 90 °C. One of the obtained phillipsite samples was tested as ion exchanger with solutions containing K+, Cs+ and Sr2+ for simulated radioactive fixation of these ions. The kinetics of ion exchange was adequately described by pseudo-second-order kinetic model equations. The obtained parameters for the ion exchange properties of the synthesized phillipsite show that this material could be used in the Cs+ and Sr2+ removal in decontamination processes. Cation-exchange effectiveness was also tested for Cs+ and Sr2+ solutions, contaminated with model nonionic surfactant Pluronic 123, which may appear as a municiple pollutant.

Introduction

According to verified syntheses of zeolitic materials (Robson 2001), phillipsite could be synthesized from mixed potassium/sodium systems, applying sodium silicate or silica sol as silica source and sodium aluminate as aluminum source. At 100 °C and sodium silicate as silica source, the time needed for hydrothermal crystallization with stirring is 6–7 h. If silica sol without agitation is elaborated the time needed for crystallization is up to 7 days (Robson 2001).

Zeolites could be prepared applying commercial reagents and also various natural, industrial and waste Si and Al-containing materials (Yoldi et al. 2019). Very recently, phillipsite, zeolite P and zeolite X were synthesized from perlite by-product (Osacký et al. 2020). It was found that the concentration of NaOH solution had significant impact on the type of synthesized zeolites, whereas reaction temperature and time influenced mainly the quantity of the synthesized zeolite species.

Phillipsite, like some other zeolites has been tested as material for uptake of contaminants in urban and industrial waste waters and radionuclides Cs+ and Sr2+ from wastes of nuclear power plants.

Phillipsite exhibits similar ion exchange behaviour as clinoptilolite for example. However, either natural or synthesized phillipsites are less studied and characterized in respect to their kinetic and equilibrium behaviour. The testing of phillipsite as sorption material began with the investigation on the use of Italian natural zeolites in wastewater treatment in the middle of 1960s. In the review of Caputo and Pepe (2007), there are numerous cited articles, in which a systematic study of phillipsite concerning mainly evaluation of selectivity and cation exchange capacities with different cations is presented. In particular, the equilibrium reactions between the Na-exchanged form of phillipsite and aqueous solutions containing Cs+ and Sr2+ were studied by Adabbo et al. (1999) and Collela et al. (2001).

Adabo et al. (1999) investigated the ion exchange of Cs+ and Sr2+ for Na+ by two naturally occurring and one synthetic phillipsites with different Si/Al ratios. The authors found that samples, with higher Si/Al ratio display good selectivity for Cs+ and moderate selectivity for Sr2+. More aluminous phillipsite displays a lower selectivity for Cs+ and a higher selectivity for Sr2+. This is in accordance with the observation that ion exchange selectivity depends on the anionic electric field strength of the zeolites. Higher siliceous zeolites with low electric field strength prefer larger cations, i.e. Cs+, characterized by a lower charge density, whereas aluminous zeolites are more selective for cations with a high charge density, e.g., Sr2+ (Barrer and Klinowski 1972). Additionally, in the review of Caputo and Pepe (2007), values of equilibrium constant (Ka) and standard Gibbs free energy (∆G0) at 25 °C for ion exchange equilibria involving Italian natural phillipsites of sedimentary origin were summarized.

Phillipsite, clinoptilolite, and mordenite natural zeolitic tuffs, as well as synthetic zeolite samples, were tested (Komarneni 1985) in simulated nuclear waste water decontamination. It was found that phillipsite-rich tuff performs better, reaching 13.5–23.7% exchange of Cs+ present in simulated alkaline waste, containing 0.00025 M CsCl in 5.5 M NaC1–NaOH solution, than mordenite-rich tuff which exchanged less than 12.7%. The author makes a conclusion “that phillipsite is probably the best natural zeolite for exchange and fixation of Cs because of its very high cation-exchange selectivity and capacity for Cs”. In addition, Komarneni (1985) states that immobilization or fixation of Cs+ in phillipsite, unlike other zeolites, can be achieved by heating the zeolite at 600 °C for 4 h and after treatment at 800–1000 °C of the Cs-exchanged phillipsite tuft the result was pollucite, CsA1Si2O6, which “locks in” the Cs+ ions in its structure. It should be emphasized that the same fixation strategy applied for Cs-exchanged clinoptilolite-rich rock (Brundu and Cerri 2015) showed transformation into the orthorhombic phase CsAlSi5O12 at 1145 °C.

Recently, on the outer surface of a porous α-alumina tubular support, K-phillipsite membrane was synthesized (Hou et al. 2013). In simulated seawater experiments, it was found a preferential selectivity for K+ ion exchange relative to Na+ ion and this membrane was proposed as potential inorganic membrane for potassium extraction from seawater (Hou et al. 2013).

A new route for preparation of zeolites such as beta, RUB-13, and ZSM-12 via seed-assisted, organic template-free synthesis recently has been demonstrated (Itabashi et al. 2012; Kamimura et al. 2012). The idea proposed by the authors was, instead of using organic structure directing agents (OSDA) usually applied in conventional hydrothermal preparation recipes, to use seeds of the same zeolite, or other ones that share common building units with the target zeolite. Thus, application of seeds helps avoiding the use of expensive OSDA and makes the process environmentally friendly. Additionally, besides directing to certain target product/s, application of seeds in zeolite synthesis, could also drastically improve the yield and kinetics of the process, thus diminishing the time and energy consumption needed for crystallization.

As far as perlite, raw material is mined and manufactured for products of various applications, it is important to elaborate approaches for new utilization possibilities via synthesis of microporous materials based on this precursor.

In the present paper, we are elaborating phillipsite preparation based on the above-mentioned ideas. Cheap natural source of silica like perlite and relatively low temperature (90 °C) for crystallization were applied. These conditions offer the possibility to use plastic vessels, avoiding expensive non-corrosive metal autoclaves, usually applied in hydrothermal zeolite synthesis. Additional aim is to inspect the ion exchange properties and selectivity of the synthesized phillipsite towards Cs+, Sr2+ and K+ polluting cations.

Experimental

Materials and methods

Three perlite samples were used in the present study. Two of them are from the Numinbah and Chillagoe deposits (Queensland, Australia) and the third is from Blue Pacific deposit (Nord Island, New Zeeland). The Numinbah perlite appears black and after been milled in agate mortar becomes gray. The whitest one is the Blue Pacific sample and the Chillagoe deposit sample is a nuance of gray, darker than Blue Pacific, but whiter than Numinbah. The chemical composition of Blue Pacific perlite, according to producer in wt% is: 74.92 SiO2, 10.56 Al2O3, 2.86 Na2O, 5.19 K2O, 0.6 CaO, 1.41 Fe2O3, 0.1 MgO, 0.13 TiO2 and ignition losses i.e. adsorbed and chemically bonded water about 7.3. For hydrothermal transformation in microporous materials, the samples of perlite were used as received, not dried and expanded by calcination.

Powder XRD experiments were performed on D2 Phaser, Bruker diffractometer, using Ni-filtered CuKα radiation (1.54056 Å), working at 10 mA and 30 mV. The XRD measurements were done in the 2θ range 4–40°, with 0.05° step and scanning time 1 s/step. The phase analyses were done using the PDF data base (PDF-4, JCPDS-ICDD, 2016).

FTIR spectra of the starting perlite and ion-exchanged samples were taken on Bruker Tensor 37, applying KBr pellet technique at 4 cm−1 spectral resolution and 32 scans.

SEM and EDX analyses were performed on Jeol Scanning Electron Microscope JSM-6390.

BET surface analyses were performed on Qantachrome NOVA 1200e apparatus. Before measurements, the samples were evacuated 16 h at 200 °C. Nitrogen adsorption–desorption isotherms were measured at liquid nitrogen temperature.

Perlite transformation to phillipsite

Recently (Ng et al. 2012), ultra-small EMT zeolite crystals were prepared for about 30 h in highly basic (Na2O/SiO2 molar ratio of about 3.5) and template-free system at about 30 °C. In the present paper, this method was modified to prepare ultra-small EMT zeolite crystals in wet gel transformation conditions. Thus, after preparation and its ageing of appropriate time, the gel was separated by centrifugation at 7000 rpm for 10 min from mother waters and these waters were used further in perlite transformation to phillipsite.

Amount of 3.4 g of Blue Pacific perlite as a powder (fraction with dimensions less than 0.125 mm) was mixed in a plastic bottle with 0.2 g sodium aluminate (Riedel de Haien) and 4.0 g mother waters, separated from the EMT synthesis. The mixture is hold for 48–72 h in an oven at 90 °C, periodically shaken and then separated by filtration.

It is known that mother waters from EMT zeolite synthesis are highly basic and it is expected that they contain substantial amounts of reagents, including primary and secondary building units that are forming EMT zeolite, including double hexagonal rings and sodalite cages.

At the same time, one of the building units of phillipsite is a ribbon of connected 4-member rings. Therefore, it could be hypothesized that at highly basic conditions of EMT zeolite synthesis, the double hexagonal rings could be hydrolyzed, forming a ribbon of five connected 4-member rings, terminated with ≡Si–ONa groups. These ribbons, interacting with other building units, obtained upon perlite dissolution in existing basic conditions, lead to phillipsite crystallization.

Hence, as an overall result of the idea is to prepare two types of zeolites (EMT and PHY).

In this way, the reagents used for EMT synthesis are better utilized. They are not disposed upon filtration in nature as mother and washing waters and, additionally, a cheap natural product perlite, is transformed in a value-added microporous zeolite, phillipsite. Recently, mother waters from wet gel Ge-EMT preparation were utilized for Ge-FAU zeolite synthesis (Chakarova et al. 2016).

Ion exchange experiments

Cation exchange was studied at 298 °K by a batch-exchange mode. To a weighed amount of phillipsite (0.05 g) prepared from Blue Pacific sample, placed in a screw capped polypropylene flask were added 10 ml of solution with appropriate concentration and the flasks were transferred into thermostatic shaker. The liquid/solid [mL/g] ratio was kept in all experiments at 200:1. The removal of K+, Cs+ and Sr2+ cations was followed at 2, 4, 6, 22 and 48 h contact time. After defined time, the mixture was separated by centrifugation at 4000 rpm and the remaining cation concentration was determined in the supernatant solutions with Atomic Absorption Spectrometry (Perkin Elmer 3030 spectrophotometer). Each experiment was carried out in duplicate.

The ion-exchange effectiveness (E %) was calculated using the equation:

$$E,\% \, = { 1}00\,m_{{\text{s}}} /\left( {V \, C_{{\text{o}}} } \right),$$
(1)

where ms [mg] is the mass of ions immobilized on zeolite, V [L] is the solution volume used in the experiment and Co [mg/L] is the initial concentration of ions (K+, Cs+ and Sr2+).

Additionally, for the same cations, distribution coefficients Kd [mL/g] were calculated according to Eq. (2):

$$K_{{\text{d}}} = \, q_{{\text{e}}} /C_{{\text{e}}} = \, (C_{0} {-} \, C_{{\text{e}}} ) \cdot V/C_{{\text{e}}} \cdot m,$$
(2)

where qe is the content of fixed cation on phillipsite [meq/g] at equilibrium, C0 is the initial concentration of cation in the solution [mg/L], Ce is the equilibrium concentration of the exchanged cation in supernatant solution after ion exchange [mg/L], V is the volume of the used starting ion-exchange solution [mL], and m—the mass [g] of the ion exchanger, applied in the experiment.

The time of interaction was set 48 h at room temperature, initial concentration C0 of the cations was 0.001 N and constant shaking of the vessel during the experiment.

To monitor the effect of presence of nonionic surfactant in the solution, additional ion-exchange experiments were conducted. BASF made triblock copolymer Pluronic P-123 was used, based on poly(ethylene glycol)-poly(propylene glycol)-poly(ethylene glycol) with chemical formula HO(CH2CH2O)20(CH2CH(CH3)O)70(CH2CH2O)20H and molecular mass about 5800 g/mol. The surfactant concentration 0.02 × 10–4 mol/L in solutions of Cs+ and Sr2+ was well below the one of critical micelle concentration – 0.1 × 10–4 mol/L (Singh et al. 2013). The experiments were carried out with single cation solutions with concentrations of Cs+ ions – 4.58 and Sr2+ – 13.28 meq/L, respectively.

Results and discussion

Characterization of the initial perlite and the synthesized phillipsite

Phase composition of starting perlite samples and the synthesized phillipsite was investigated by powder XRD analysis. As it is seen from Fig. 1a, the perlite from Numinbah is completely amorphous and the one from Blue Pacific deposit (Fig. 1c) contains, amorphous glass matrix and trace amounts of α-quartz (< 5%) and plagioclase (< 3%). The phase analysis for Chillagoe (Fig. 1b) gives as a major component amorphous material and traces of quartz (< 2%) and plagioclase (< 3%).

Fig. 1
figure1

Powder XRD pattern of perlite from Numinbah (a), Chillagoe (b) and Blue Pacific (c), deposits

According to the presented on Fig. 2 powder XRD patterns of synthesized zeolites, amorphous halo is not observed and the prepared phillipsite samples are highly crystalline. The observed XRD reflections are narrow, sharp and with good intensity. Minor additional phases such as NaP and sodalite were found in some experiments. The above results prove the applied method for synthesis is reproducible and cheap.

Fig. 2
figure2

Powder XRD analysis of phillipsite, obtained from Blue Pacific, Chillagoe and Numinbah perlite deposits after 72 h of hydrothermal transformation at 90 °C

On Fig. 3a, b, c are presented FTIR spectra of the perlite samples in the silicate short-to-medium-range structural unit vibrations. The band located at about 467 cm−1 is assigned to rocking motion of the bridging oxygen atoms perpendicular to the Si–O–Si plane (Lucovsky et al. 1983).

Fig. 3
figure3

a, b FTIR spectra of quartz and initial perlite samples. c FTIR spectra of starting sodium form of phillipsite, synthesized from Blue Pacific perlite deposits and Cs+ and Sr+2 ion-exchanged samples

At about 789 cm−1, the band is attributed to bending motion of the oxygen atom along the bisector of the Si–O–Si bridging group. The spectra exhibit a broad band at 1046–1073 cm−1 which could be deconvoluted to at least three components at about 960–980, 1000 and 1190–2000 cm−1. The band appearing at 960–980 cm−1 could be attributed to stretching vibrations of the Si–OH groups in the silanol defect nests, as well as to perturbated Si–O vibrations in the vicinity of titanium or other element incorporated in the silicate framework.

The high-frequency band at 1046 for Blue pacific and 1050, 1073 cm−1, respectively, for Chillagoe and Numinbah perlite samples, is assigned to antisymmetric stretching mode of Si–O–Si(Al) bonds involving mainly oxygen motion (Lucovsky et al. 1983). It is known that the band at about 1000–1100 cm−1, assigned to antisymmetric stretching mode of Si–O–Si(Al) bonds vibrations is sensitive to Si/Al ratio and shifts to higher frequencies with increasing of the Si/Al ratio in the silicate frameworks (Flanigen 1976). Therefore, in accordance with FTIR data, the studied perlite samples are in the following order of Si/Al ratio: Blue Pacific < Chillagoe < Numinbah.

As it is seen from the FTIR spectra on Fig. 3, the antisymmetric stretching Si–O–Si(Al) band moves from 1046 to lower (1026 cm−1) frequency for the starting Blue Pacific and respective phillipsite sample, obtained from this perlite. This could be explained with incorporation of aluminum in the silicate framework from the sodium aluminate added during the hydrothermal synthesis. As additional sodium aluminate was delivered in the starting synthesis composition, the Si/Al ratio in the obtained phillipsite has to diminish in comparison to the starting silicate framework. It is known that the ion-exchange capability is roughly proportional to the number of [AlO4]¯ tetrahedra in zeolite framework. Therefore, the respective ion-exchange capability in alumina-enriched phillipsite is expected to be enhanced.

On Fig. 4 are presented panoramic view and more detailed picture of the obtained phillipsite crystal aggregations with some well faceted crystals with dimensions of about 2–4 μm. EDX analysis on several spots gives average SiO2/Al2O3 = 5.4 molar ratio for the hydrothermally transformed material. This ratio is in the margins 4.07–6.27 for the phillipsite samples, prepared according to verified synthesis of zeolitic materials (Robson 2001).

Fig. 4
figure4

SEM picture of the phillipsite product, obtained from hydrothermally transformed Blue Pacific perlite

Nitrogen adsorption–desorption isotherm at liquid nitrogen temperature for the phillipsite sample, prepared from Blue Pacific perlite is presented on Fig. 5.

Fig. 5
figure5

Nitrogen adsorption–desorption isotherm for phillipsite sample, prepared from Blue Pacific perlite

The measured BET specific surface area is 13 m2/g and the total pore volume, estimated at relative pressure p/p0 = 0.98, is 0.02 cm3/g. The obtained BET surface area is comparable to the one of natural phillipsite tuff (Notario et al. 1995) and the value determined for total pore volume is close to the one, obtained for natural phillipsite treated with 1 N phosphoric acid. Also, as reported earlier (Osacký et al. 2020) phillipsite, prepared from perlite by-product material, shows SBET 11 m2/g and total pore volume 0.023 cm3/g, very close to the values obtained in the present work. Further ion-exchange experiments were performed with this sample.

Ion exchange of Cs+, Sr2+ and K+ by the synthesized phillipsite

The kinetics of ion exchange on the synthesized phillipsite was studied. The extents of Cs+, Sr2+ and K+ removal with time from single cation solutions are shown on Fig. 6a. During the first 2 h of interaction for the studied Cs+ concentration 609 mg/L, the effectiveness of Cs+ removal is about 93% and for the next contact time up to 48 h, it increases a little with 1.5%. For Sr2+ it took almost 24 h to reach equilibrium with about 47% effectiveness of fixation. The uptake profile for K+ shows that equilibrium is achieved within 24 h. By this time, the effectiveness of K+ removal for the studied concentration – 354 mg/L is 55.32% and then increases to 58.74% for the next 24 h.

Fig. 6
figure6

a Extent of Cs+, Sr2+ and K+ removal with time, from single cation solutions. b Pseudo-second-order kinetic model (Eq. 4) fitted to experimental data for the uptake of Cs+, K+, and Sr2+ by phillipsite

From the results of the kinetic study (Fig. 6a), it can be concluded that the interaction is more rapid in the first time period (30 min for Cs+ and about 5 h for Sr2+ and K+) when about 80–90% of totally sorbed amount is achieved for the studied experimental conditions. The equilibrium ions concentrations are achieved for about 4 h for Cs+, while 22–24 h are needed for K+ and Sr2+.

The kinetics of cation uptake by phillipsite was described by applying pseudo-first (Eq. 3) and pseudo-second (Eq. 4) order kinetic expressions (Wu 2001; Reddad et al. 2002; Coleman et al. 2006):

$${\text{log}}\left( {q_{{\text{e}}} {-} \, q_{{\text{t}}} } \right) = {\text{log}}q_{{\text{e}}} {-}\left( {k_{{1}} /{2}.{3}0{3}} \right)t,$$
(3)
$$t/q_{{\text{t}}} = {1}/\left( {k_{{2}} q_{{\text{e}}}^{{2}} } \right) + \left( {{1}/q_{{\text{e}}} } \right)t,$$
(4)

where qt and qe are, respectively, the concentrations of fixed cation on phillipsite [meq/g], at time t and at equilibrium. The k1 [min–1] and k2 [g/(meq min)] are the apparent pseudo-first- and pseudo-second-order rate constants.

The experimental data are better fitted applying the pseudo-second-order kinetic model (Eq. 4). The correlation coefficient, R2, indicating the conformity of the pseudo-second-order kinetic model, attains value of 0.99. Additionally, applying Eq. 4, good agreement between experimentally measured, qe,exp and calculated equilibrium capacities values, qe,calc is observed. The calculated parameters are presented in Table 1. The pseudo-first-order kinetic model shows that it is less appropriate (0.85 < R2 < 0.93). Experimentally measured data points and the theoretically fitted curves, obtained by the pseudo-second-order kinetic model are shown on Fig. 6b.

Table 1 Calculated parameters for the pseudo-second-order kinetic model for Cs+, Sr2+ and K+ ions fixation by phillipsite

Additionally, in Table 1 is presented the parameter, h, [meq/(g min)], characterizing the initial cation uptake, calculated according to Eq. (5).

$$h = k_{{2}} q_{{\text{e}}}^{{2}} .$$
(5)

Comparing the h parameter values for the studied cations (Table 1), it could be concluded that at the chosen experimental conditions, the Cs+ ions are about two times more rapidly exchanged than Sr2+ and the latter about the same time more rapidly fixated on phillipsite, than K+ ions.

The kinetics of immobilization of the three cations was studied by comparing the effectiveness of their uptake from mixed solution, where they are presented in equivalent concentration of 2.10–3 N (Fig. 7).

Fig. 7
figure7

Effectiveness (E, %) of Cs+, Sr2+ and K+ removal from a mixed solution with concentration 2 × 10–3 N of each ion

The run of the effectiveness with time indicates that at low initial concentrations, equilibrium of Cs+ and K+ uptake is achieved within the first 2 h of interaction and removal efficiency is ~ 93% for Cs+ and 69% for K+. The Sr2+ uptake is slower, but for 48 h it achieves the values of Cs+ − 93%.

The distribution coefficient expresses the chemical binding affinity of ion in solution to a solid material and is commonly used for characterization of ions uptake. The distribution coefficients (Kd) for K+, Cs+ and Sr2+ in the present work were determined in comparable conditions with Behrens and Clearfield (1997). Other literature data (Munthali et al. 2015) is also presented in Table 2. It is seen that phillipsite, prepared in the present work from perlite shows high values of Kd for both Cs+ and Sr2+.

Table 2 Distribution coefficients, Kd, for K+, Cs+ and Sr2+ ions for phillipsite, prepared from Blue Pacific perlite in comparison with other sorbents

In the paper of Adabbo et al. (1999), it is just reported that “the sedimentary and synthetic phillipsites display a good selectivity for Cs+ and a modest selectivity for Sr2+” without giving quantitative results for distribution coefficient Kd or maximum exchanges capacities. As it concerns the synthetic phillipsite, the authors found that “it still exhibits a satisfactory selectivity for Cs+ and a markedly increased selectivity for Sr2+” but for both ions the selectivity is lower compared to sedimentary phillipite.

Ion exchange experiments in the presence of nonionic surfactant were additionally conducted. The effect of Pluronic 123 with concentration 0.02 × 10–4 mol/L in solutions of Cs+ and Sr2+ on cation-exchange effectiveness of phillipsite is presented on Fig. 8a, b. As seen from Fig. 8a, the effectiveness of Cs+ ions fixation is not affected by the presence of nonionic surfactant. For Sr2+, after about 10 h of exchange, decrease of the immobilization effectiveness is observed. After about 40 h of ion exchange, the values of Sr2+ effectiveness for immobilization are about 10–12% less in comparison to the values, obtained in the experiment with pure Sr2+ solution (Fig. 8b).

Fig. 8
figure8

Effect of Pluronic 123 on cation-exchange (immobilization) effectiveness on phillipsite in solutions of: a Cs+ and b Sr2+

At the studied experimental conditions, the effectiveness of Cs+ ions fixation is about 90–94%, while the value for Sr2+ ions is about 56–58%. These features could be explained with stronger shielding by complexation of the Sr2+ ion (possessing smaller ionic radius than Cs+ ion) with relatively bulk molecules of the surfactant. The effectiveness could be affected by the type of ion, its concentration, and the surfactant concentration. Further ion-exchange experiments to investigate the effects in this respect are planned.

Conclusions

A supplementary method was elaborated for synthesis of phillipsite from perlite utilizing mother waters from wet gel EMT preparation. The method is reproducible and cheap and was applied to three samples of perlite from Australian and New Zeeland field deposits, differing in color, chemical, and phase composition. One of the obtained phillipsite samples was tested as ion exchanger for K+, Cs+ and Sr2+, which are the basic contaminants in radioactive wastes. The kinetics of the uptake of the above cations is fast. The experimental data is adequately described by pseudo-second-order kinetic model equations. The estimated rate constants k2 [g/(meq min)] for the studied experimental conditions are 0.0316 for Cs+, 0.0037 for Sr2+, and 0.0063 for K+. The distribution coefficient Kd for both Cs+ and Sr2+ is with high value (> 59,000 mL/g) and that for K+ is 5500 mL/g, which values are comparable with other zeolites. The obtained parameters for the ion exchange properties of the synthesized phillipsite show that this material could be used in the Cs+ and Sr2+ removal in decontamination processes. Cation-exchange effectiveness was also tested for Cs+ and Sr2+ solutions, contaminated with model nonionic surfactant Pluronic 123, which may appear as a municiple pollutant.

References

  1. Adabbo M, Caputo D, de Gennaro B, Pansini M, Colella C (1999) Ion exchange selectivity of phillipsite for Cs and Sr as a function of framework composition. Microporous Mesoporous Mater 28:315–324. https://doi.org/10.1016/S1387-1811(98)00246-7

    Article  Google Scholar 

  2. Barrer RM, Klinowski J (1972) Influence of framework charge density on ion-exchange properties of zeolites. J Chem Soc Faraday Trans 1(68):1956–1963. https://doi.org/10.1039/F19726801956

    Article  Google Scholar 

  3. Behrens E, Clearfield A (1997) Titanium silicates, M3HTi4O4(SiO4)3.4H2O (M=Na+, K+), with three dimensional tunnel structures for the selective removal of strontium and cesium from wastewater solutions. Microporous Mater 11:65–75. https://doi.org/10.1016/S0927-6513(97)00022-9

    Article  Google Scholar 

  4. Brundu A, Cerri G (2015) Thermal transformation of Cs-clinoptilolite to CsAlSi5O12. Microporous Mesoporous Mater 208:44–49. https://doi.org/10.1016/j.micromeso.2015.01.029

    Article  Google Scholar 

  5. Caputo D, Pepe F (2007) Experiments and data processing of ion exchange equilibria involving Italian natural zeolites: a review. Microporous Mesoporous Mater 105:222–231. https://doi.org/10.1016/j.micromeso.2007.04.024

    Article  Google Scholar 

  6. Chakarova K, Andonova S, Dimitrov L, Hadjiivanov K (2016) FTIR study of CO and N2 adsorption on [Ge]FAU zeolites in their Na- and H-forms. Microporous Mesoporous Mater 220:188–197. https://doi.org/10.1016/j.micromeso.2015.09.002

    Article  Google Scholar 

  7. Colella C, Torracca E, Colella A, de Gennaro B, Caputo D, de Gennaro M (2001) Ion-exchange features of intermediate-silica sedimentary phillipsite. In: Galarneau A, De Renzo F, Fajula F, Vedrine J (eds) Zeolites and mesoporous materials at the Dawn of the 21st Century, studies in surface science and catalysis. Elsevier, Amsterdam

    Google Scholar 

  8. Coleman NJ, Brassington DS, Raza A, Mendham AP (2006) Sorption of Co2+ and Sr2+ by waste-derived 11 A tobermorite. Waste Manag 26:260–267. https://doi.org/10.1016/j.wasman.2005.01.019

    Article  Google Scholar 

  9. Flanigen EM (1976) Structural Analysis by Infrared Spectroscopy. In: Rabo JA (ed) Zeolite Chemistry and Catalysis, ACS Monograph 171. Washington D.C, American Chemical Soc., pp 80–117

    Google Scholar 

  10. Hou J, Yuan J, Xu J, Sun L (2013) Synthesis and characterization of K-phillipsite (K-PHI) membrane for potassium extraction from seawater. Microporous Mesoporous Mater 172:217–221. https://doi.org/10.1016/j.micromeso.2013.01.034

    Article  Google Scholar 

  11. Itabashi K, Kamimura Y, Iyoki K, Shimojima A, Okubo T (2012) A working hypothesis for broadening framework types of zeolites in seed-assisted synthesis without organic structure-directing agent. J Am Chem Soc 134:11542–11549. https://doi.org/10.1021/ja3022335

    Article  Google Scholar 

  12. Kamimura Y, Itabashi K, Okubo T (2012) Seed-assisted, OSDA-free synthesis of MTW-type zeolite and “Green MTW” from sodium aluminosilicate gel systems. Microporous Mesoporous Mater 147:149–156. https://doi.org/10.1016/j.micromeso.2011.05.038

    Article  Google Scholar 

  13. Komarneni S (1985) Phillipsite in Cs decontamination and immobilization. Clays Clay Miner 33:145–151. https://doi.org/10.1346/CCMN.1985.0330209

    Article  Google Scholar 

  14. Lucovsky G, Wong CK, Pollard WB (1983) Vibrational properties of glasses: Intermediate range order. J Non-Cryst Solids 59–60:839–846. https://doi.org/10.1016/0022-3093(83)90301-0

    Article  Google Scholar 

  15. Munthali MW, Johan E, Aono H, Matsue N (2015) Cs+and Sr2+ adsorption selectivity of zeolites in relation to radioactive decontamination. J Asian Ceram Soc 3:245–250. https://doi.org/10.1016/j.jascer.2015.04.002

    Article  Google Scholar 

  16. Ng E-P, Chateigner D, Bein T, Valtchev V, Mintova S (2012) Capturing ultrasmall EMT zeolite from template-free systems. Science 335:70–73. https://doi.org/10.1126/science.1214798

    Article  Google Scholar 

  17. Notario JS, Garcia JE, Caceres JM, Arteaga IJ, Gonzalez MM (1995) Characterization of natural phillipsite modified with orthophosphoric acid. Appl Clay Sci 10:209–217. https://doi.org/10.1016/0169-1317(95)00025-Y

    Article  Google Scholar 

  18. Osacký M, Pálková H, Hudec P, Czímerová A, Galusková D, Vítková M (2020) Effect of alkaline synthesis conditions on mineralogy, chemistry and surface properties of phillipsite, P and X zeolitic materials prepared from fine powdered perlite by-product. Microporous Mesoporous Mater 294:109852. https://doi.org/10.1016/j.micromeso.2019.109852

    Article  Google Scholar 

  19. Powder Diffraction File (PDF-4 Data Base 2016), International Centre for Diffraction Data (ICDD), Newtown Square, PA, USA, 2016

  20. Reddad Z, Gerente C, Andres Y, Le Cloirec P (2002) Adsorption of several metal ions onto a low-cost biosorbent: kinetic and equilibrium studies. Environ Sci Technol 36:2067–2073. https://doi.org/10.1021/es0102989

    Article  Google Scholar 

  21. Robson H (ed) (2001) Verified syntheses of zeolitic materials. Elsevier, Amsterdam

    Google Scholar 

  22. Singh V, Khullar P, Dave PN, Kaur N (2013) Micelles, mixed micelles, and applicatiuons of polyoxypropylene (PPO)-polyoxyethylene (PEO)-polyoxypropylene (PPO) triblock polymers. Int J Ind Chem 4(12):1–18. https://doi.org/10.1186/2228-5547-4-12

    Article  Google Scholar 

  23. Wu FC, Tseng RL, Juang RS (2001) Kinetic modeling of liquid-phase adsorption of reactive dyes and metal ions on chitosan. Water Res 35:613–618. https://doi.org/10.1016/S0043-1354(00)00307-9

    Article  Google Scholar 

  24. Yoldi M, Fuentes-Ordoñez EG, Korili SA, Gil A (2019) Zeolite synthesis from industrial wastes. Microporous Mesoporous Mater 287:183–191. https://doi.org/10.1016/j.micromeso.2019.06.009

    Article  Google Scholar 

Download references

Author information

Affiliations

Authors

Corresponding author

Correspondence to O. Petrov.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Dimitrov, L., Lihareva, N., Tzvetanova, Y. et al. Synthesis of phillipsite from perlite utilizing mother waters from wet gel EMT preparation and study of the obtained zeolitic material as ion exchanger. Environ Earth Sci 80, 86 (2021). https://doi.org/10.1007/s12665-021-09378-z

Download citation

Keywords

  • Perlite
  • Synthesis
  • Phillipsite
  • Ion exchange
  • Kinetics