Startseite CO2 gas separation using mixed matrix membranes based on polyethersulfone/MIL-100(Al)
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CO2 gas separation using mixed matrix membranes based on polyethersulfone/MIL-100(Al)

  • Witri Wahyu Lestari EMAIL logo , Robiah Al Adawiyah , Moh Ali Khafidhin , Rika Wijiyanti , Nurul Widiastuti und Desi Suci Handayani
Veröffentlicht/Copyright: 12. März 2021
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Open Chemistry
Aus der Zeitschrift Open Chemistry Band 19 Heft 1

Abstract

The excessive use of natural gas and other fossil fuels by the industrial sector leads to the production of great quantities of gas pollutants, including CO2, SO2, and NO x . Consequently, these gases increase the temperature of the earth, producing global warming. Different strategies have been developed to help overcome this problem, including the utilization of separation membrane technology. Mixed matrix membranes (MMMs) are hybrid membranes that combine an organic polymer as a matrix and an inorganic compound as a filler. In this study, MMMs were prepared based on polyethersulfone (PES) and a type of metal–organic framework (MOF), Materials of Institute Lavoisier (MIL)-100(Al) [Al3O(H2O)2(OH)(BTC)2] (BTC: benzene 1,3,5-tricarboxylate) using a phase inversion method. The influence on the properties of the produced membranes by addition of 5, 10, 20, and 30% MIL-100(Al) (w/w) to the PES was also investigated. Fourier-transform infrared spectroscopy (FTIR) analysis indicated that no chemical interactions occurred between PES and MIL-100(Al). Scanning electron microscope (SEM) images showed agglomeration at PES/MIL-100(Al) 30% (w/w) and that the thickness of the dense layer increased up to 3.70 µm. After the addition of MIL-100(Al) of 30% (w/w), the permeability of the MMMs for CO2, O2, and N2 gases was enhanced by approximately 16, 26, and 14 times, respectively, as compared with a neat PES membrane. The addition of MIL-100(Al) to PES increased the thermal stability of the membranes, reaching 40°C as indicated by thermogravimetry analysis (TGA). An addition of 20% MIL-100(Al) (w/w) increased membrane selectivity for CO2/O2 from 2.67 to 4.49 (approximately 68.5%), and the addition of 10% MIL-100(Al) increased membrane selectivity for CO2/N2 from 1.01 to 2.12 (approximately 110.1%).

Keywords: CO2 ; MMMs; MIL-100(Al); PES

1 Introduction

The consumption of energy continues to increase with population growth and further technological development. The most widely used energy sources are natural gas (53.3%) and coal (26.3%) [1]. The worldwide consumption of natural gas has reached 100 trillion ft3 in 2018 and is estimated to increase to 160 trillion ft3 in 2035. In Indonesia, natural gas is the most widely used energy source after petroleum and coal. Natural gas consists of hydrocarbon compounds and gas pollutants, such as carbon dioxide (CO2), nitrogen (N2), sulfur dioxide (SO2), and hydrogen sulfide (H2S) [2]. The emission factor of CO2 from various energy sources is very high as compared to other gases [1]. As an acid gas, CO2 is corrosive to gas pipelines and reduces heating value. Furthermore, an increase in CO2 gas in the atmosphere increases the earth’s temperature, leading to climate change and global warming [3]. CO2 pollutants also make an impact on human health and contribute to asthma and other respiratory diseases that can potentially cause cardiovascular disease and cancer [4]; therefore, a significant effort must be made to reduce CO2 emissions.

In general, CO2 gas emissions can be reduced through its absorption, adsorption, cryogenic distillation, and separation with membranes [5]. CO2 separation by the absorption method can be done using monoethanolamine [6,7]. The absorption method for CO2 gas separation has advantages because it requires less energy, has high absorption capacity, and is flexible; however, the use of this method requires high costs and an appropriate solvent [5]. Adsorption methods for CO2 gas separation can use physical or chemical adsorbents. The adsorbents that have been investigated for CO2 separation include Zeolite CaX [8] and Zeolite Ceca 13X [9]. Songolzadeh et al. stated that, while the adsorption method requires little energy, adsorption capacity is low, the process of regenerating adsorbents is difficult, and further research is required to find new adsorbents [5]. Gas separation by a cryogenic distillation method has been investigated by Li et al. and includes technology that is relatively easy to produce and can be used on an industrial scale. In addition, this method does not use solvents or produce liquid CO2. However, the amount of energy required for cooling and compacting the CO2 at low temperatures is great, which can cause other operational problems [10]. Gas separation using membrane technology depends on gas pressure. This technology has advantages over other CO2 gas separation techniques for reasons such as its use of simple tools, clear processes, high permeability and selectivity, high thermal and chemical stability, resistance to plasticization, and low production costs [5].

Membrane technology for gas separation is highly developed in the industry because it can be easily applied and is environmentally friendly; therefore, membranes have been widely commercialized [11]. Membrane applications have been found for the separation of O2/N2 CO2/N2, and vapors, air dehydration, and the removal of volatile organic compounds from waste [12]. Metal membranes made of platinum or palladium have good performance, but the high cost of these metals greatly influences their selection. Inorganic membranes can be used as alternatives because of their better chemical stability and lower fabrication costs; however, their use requires high temperatures of 200 to 900°C. Organic polymer membranes increasingly dominate the field because they are economical and their performance is quite competitive [11]. However, the selectivity and permeability properties of polymer membranes are limited [13]. These deficiencies have pushed researchers toward the development of alternative ways of making membranes that are more stable and economical and have a high separation performance, namely through combinations of membrane materials known as mixed matrix membranes (MMMs). The fabrication technology for MMMs promises to improve mechanical properties, producing better separation capabilities and stability than organic polymer membranes [14]. MMMs are composite membranes consisting of an organic polymer matrix as a continuous phase and filler particles as a dispersion phase [15]. One polymer matrix that has potential in the fabrication of MMMs is polyethersulfone (PES). This polymer is widely used in the manufacture of membranes because it has good mechanical properties, good thermal and chemical stability [16], and high glass transition temperatures (T g) of up to 225°C [17]. With addition of ethylenediamine (EDA)-TiO2 of 5%, PES-based MMMs had the highest selectivity for CO2/CH4 gas separation at 41.42 and CO2 permeability at 10.11 Barrers (4 bars) [18]. In addition, PES/Zeolitic Imidazolate Framework-8 (ZIF-8) MMMs have been investigated for H2/CO2 gas separation, demonstrating a selectivity of 9.3, and H2/N2 gas separation, demonstrating a selectivity of 11.5 [19]. CO2/CH4 gas selectivity increases from 3.57 to 11.15 with the addition of a 15% carbon molecular sieve in PES membranes [20].

Promising fillers can increase both permeability and selectivity. So far, the materials that have been most widely used as fillers are porous materials such as silica, carbon nanotubes, zeolites, and graphite, as well as used in the development of metal–organic frameworks (MOFs) [15]. MOFs have good porosity, large surface areas, and adjustable pore sizes and topology, making them ideal selections as fillers in MMMs [21]. Research on MOF-based MMMs for CO2 gas separation has been performed in the past, including on loading of 30 wt% [Ti8O8(OH)4(C6H3–C2O4–NH2)6] also known as NH2-Material of Institute Lavoisier (MIL)-125(T i) on polysulfone (PSf) have shown an increase of 320% compared with pristine PSf membrane [22], [Al(OH)(O2C–C6H4–CO2)] also known as Material of Institute Lavoisier (MIL)-68(Al) modified into PSf showed only small increases in H2 and CO2 permeabilities in the ranges of 11.1–12.4 and 4.7–5.4 Barrer, respectively [23]. MMMs containing [Zr6O4(OH)4(C8H4O4)6(NH2)6] also known as UiO-66-NH2 and Matrimid® polymer [24] exhibited not only enhanced mechanical and thermal stabilities, but also CO2 permeability was increased by 200% and CO2/N2 ideal selectivity was increased by 25%. In addition, NH2-Cu3(BTC)2 (BTC: benzene 1,3,5-tricarboxylate) deposited on Pebax (Pebax/sub-NH2-Cu-BTC) showed 303% higher CO2 permeability than neat Pebax due to the fine dispersion and the presence of groups with a superior CO2-philicity in the framework [25], and incorporation of MOF-5 (15 wt%) into polyimide (PI) increased the permeability toward CO2 gas up to 290% [26].

Trivalent metals, for example, Al3+ ions, are promising candidates for the synthesis of MOFs because of their porosity, low density, and high thermal and physicochemical stability [27]. Al-fumarate-based MOFs have been investigated by Nuhnen et al. as a filler in Matrimid® polymers, showing increased permeability for the separation of CO2 and CH4 gases [28]. One type of MOF is the Material of Institute Lavoisier (MIL). MIL-n types based on Al3+ metal ions that have been investigated in gas separation processes include MIL-53(Al) and NH2-MIL-53(Al) in polyvinylidene fluoride [29] and MIL-68(Al) in polysulfone [23]. Another aluminum-based MIL-n is MIL-100(Al). The synthesis of an aluminum trimesate-based MIL-100 was first performed by Volkringer et al. using the hydrothermal method [30], and MIL-100(Al) has been investigated for hydrogen storage with a Pd metal carrier [31], as a catalyst in sulfoxidation reactions [32], and for the loading of doxorubicin hydrochloride on MIL-100(Al) gel as an anticancer treatment [33]. The use of MIL-100(Al) filler for separation applications has never been done; therefore, this study aimed at researching the development of MMMs using MIL-100(Al) with PES polymers, expecting that this would improve the CO2 gas separation abilities of MMMs.

2 Materials and methods

2.1 Materials

All chemicals were used in analytical grade without further purification. Aluminum nitrate nonahydrate (99%) and benzene-1,3,5 tricarboxylic acid (95%) were commercially provided by Sigma Aldrich, Germany. Ethanol (99%), N,N′-dimethylformamide (DMF, 99.8%), PES (99%), and N,N′-dimethylacetamide (99%) were supplied by Merck EMSURE, Germany. Nitrogen (UHP 99.995%), oxygen (UHP 99.9%), and carbon dioxide (UHP 99.9%) gases were purchased from Samator, Indonesia.

2.2 Methods

2.2.1 Synthesis of MIL-100(Al)

The MIL-100(Al) was synthesized under the solvothermal conditions according to a procedure modified from the literature [33]. Al(NO3)3·9H2O (2.851 g, 7.6 mmol) and trimesic acid (H3BTC: benzene 1,3,5-tricarboxylate) (1.051 g, 5 mmol) were dissolved in ethanol (36 mL) and stirred for 15 min at room temperature. The solution was then placed in a Teflon linedSS Autoclave and heated at 120°C for 1 h. The resulting white gel was dried in an oven at 80°C for 19 h until a yellow solid was obtained, which was then washed with DMF (1 × 30 mL) and ethanol (1 × 30 mL) to remove the remaining ligand. The MIL-100(Al) material was activated at 100°C for 2 h and sonicated for 5 h to reduce particle size (yield: 87.19%).

2.2.2 Preparation of MMMs based on PES/MIL-100(Al)

The preparation of MMMs was performed with a phase inversion method modified from the study by Dama et al. [34]. Filler MIL-100(Al) in different weight percentages of 5, 10, 20, and 30% (w/w) was added to dimethylacetamide. Each mixture was sonicated for 20–30 min so that the MIL-100(Al) was well dispersed in the solution and then stirred for 1 h at room temperature to homogenize it. Afterward, PES (35%) (w/w) was added to each mixture and stirred for 24 h at room temperature. Each obtained dope solution was cast on a glass plate (20 × 15 cm). Next, each membrane on a glass plate was evaporated for about 20 s and then dipped in a water-filled coagulant tub, and after the membrane was removed from the glass plate, the membrane was washed with distilled water for 24 h, followed by solvent exchange with methanol for 2 h and drying for 48 h at room temperature to evaporate the solvent.

2.2.3 Gas separation test

The resulting membranes were tested for permeability and selectivity using a single gas (N2, O2, and CO2) flat sheet membrane method as reported by Lee et al. [35]. The measurement was performed at a pressure of 1 bar and room temperature. Each membrane was fabricated by cutting it in a circle with an effective diameter of 5.7 cm, placing it on a membrane permeation cell, and then sealing it before connecting it to the gas stream. The data were collected by measuring the amount of time taken for the gas to reach a volume of 10 mL, with the volume of gas measured with a bubble flow meter and the time was measured with a stopwatch. Data retrieval was done twice. The scheme of the gas permeation test equipment is shown in Figure 1 [36]. The permeability and selectivity of each membrane were calculated based on equations (1) and (2) [37].

(1) P i l = Q ( A × Δ P ) 273 . 15 T = V t ( A × Δ P ) 273 . 15 T

where,

  • P i = gas permeability (GPU P i l [1 GPU = 1 × 10−6 cm3 (STP)/cm3 s cm Hg] or Barrer [1 Barrer = 1 × 10−10 cm3 (STP)/cm2 s cm Hg])

  • l = membrane density (cm)

  • V = measured volume (cm3, STP)

  • A = membrane area (cm2)

  • t = required time for gas to pass through the membrane (s)

  • Δ P = gas pressure (cm Hg)

  • T = temperature condition during the measurement (K)

(2) α i / j = P i P j

where,

  • α i / j = selectivity of the membrane for gas i and gas j

  • P i = permeability of gas i (Barrer)

  • P j = permeability of gas j (Barrer)

Figure 1 Single gas permeation rig (adapted from Gunawan et al. [36]).
Figure 1

Single gas permeation rig (adapted from Gunawan et al. [36]).

2.3 Characterization of the materials

X-ray diffraction (XRD) (X-Pert Pan Analytical) was used to analyze the phase purity and crystallinity of the prepared materials. The functional groups of the compounds were observed using Fourier-transform infrared spectroscopy (FTIR) (Shimadzu IR Prestige-21). The thermal stability of the materials was measured using TG analysis to a temperature of 900°C (Hitachi STA 7000) with a heating rate of 10°C/min under nitrogen flow. The morphology and elemental composition of the materials were observed by a scanning electron microscope-energy dispersion X-ray (SEM–EDX) (FEI Inspect-S50). A surface area analyzer (SAA) (Quadrasorb Evo, Quantachrome) was used to monitor the surface area and porosity of the materials.

  1. Ethical approval: The conducted research is not related to either human or animal use.

3 Results and discussion

3.1 Characterization of the materials

3.1.1 X-ray diffraction (XRD)

The characterization of the prepared materials using XRD was performed to determine the purity and suitability of the phase. The XRD analyses demonstrated that the peak of the synthesized MIL-100(Al) corresponds to the standard pattern for MIL-100(Al) (CCDC No. 789872) but has lower crystallinity as shown by the broad peak in Figure 2. This result is in accordance with the study conducted by Xia et al. [38], which stated that the powder XRD of MIL-100(Al) synthesized through gel formation shows low crystallinity.

Figure 2 Diffractogram of synthesized MIL-100(Al) as compared with the standard patterns of CCDC No. 789872 and the H3BTC ligand (ICSD No. 30245).
Figure 2

Diffractogram of synthesized MIL-100(Al) as compared with the standard patterns of CCDC No. 789872 and the H3BTC ligand (ICSD No. 30245).

3.1.2 Fourier transform infrared spectroscopy (FTIR)

The properties of the synthesized MIL-100(Al) can also be seen in the shift of the absorption peak shown in the FTIR analysis of this material in comparison with the H3BTC ligand (Figure 3). These results are in accordance with the research reported by Xia et al. [38].

Figure 3 FTIR spectra of the synthesized MIL-100(Al) and H3BTC ligand.
Figure 3

FTIR spectra of the synthesized MIL-100(Al) and H3BTC ligand.

The significant shift from 1,721 to 1,673 cm−1 corresponds to the stretching vibration of the carbonyl group (C═O) caused by the deprotonation of the C═O–H group by the free ligand that is coordinated with the Al3+ metal ion in MIL-100(Al). In addition, there is also a shift in the absorption peak of the OH group from 2,500–3,100 cm−1 to 2,886–3,650 cm−1, representing the formation of hydrogen bonding, whereas OH in MIL-100(Al) comes from the ligand that forms MIL-100(Al) with the formula {Al3O(OH)(H2O)2[BTC]2 · xH2O}. Al–O bonds are generally observed at wavenumbers below 700 cm−1. The absorption peak at 675 cm−1 in the synthesis results shows the Al–O bond that has been coordinated with the carboxyl group of the H3BTC ligand. The uptake of the C–O functional groups also matched the literature at wave number 1,246 cm−1 [39] (Table 1).

Table 1

Comparison of the absorption spectra of the synthesized MIL-100(Al) with the H3BTC ligand and MIL-100(Al) in the literature

Absorption Wavenumber (cm−1)
H3BTC [38] Synthesized MIL-100(Al) MIL-100(Al) literature [38]
O–H 2,500–3,100 2,886–3,650 2,500–3,500
C═O stretch 1,721 1,673 1,670–1,729
C–O 1,276 1,246 1,131–1,221
Al–O — 675 680–620

The success of the membrane preparation can be seen in a comparison of the FTIR spectra of the neat PES membrane and that of the PES/MIL-100(Al) membranes (Figure 4). The comparison of the PES FTIR spectra with those of the PES/MIL-100(Al) with different percentage additions of MIL-100(Al) shows that there were no changes to the structure of the PES, which is demonstrated by the similar FTIR spectra. The addition of MIL-100(Al) to PES causes the character of the MIL-100(Al) to be more visible. This is marked by a widening of the absorption peak of the OH functional groups at 3,447 cm−1 due to overlapping OH groups from the –OH ligand and H2O molecules in the MIL-100(Al) (formula {Al3O(OH)(H2O)2[BTC]2 · xH2O}) and overlapping OH from water during coagulation. The PES uptake band is in accordance with the study by Mushtaq et al. [40] and is listed in Table 2, showing the uptake at 1,149 and 1,241 cm−1, which corresponds to the absorption peak of the S═O group. CSO2C absorption is indicated at wavenumber 1,324 cm−1. C–O uptake at 1,237 and 1,100 cm−1 indicates the presence of ether groups. The absorption of C═C aromatic is shown in the area of 1,576–1,487 cm−1. The addition of MIL-100(Al) to PES does not produce a new absorption peak, indicating that there is no chemical bond between the PES and MIL-100(Al). However, non-covalent interactions might have occurred (but could not be observed in FTIR) such as π–π stacking between the aromatic rings, ion–dipol interaction between metal ion part of MOF and sulfon and ether group and also dipol–dipol interaction; therefore, good composite could be formed and reinforced each other. The decrements in intensity of OH band in PES/MIL-100(Al) 5% might be due to lower content of water during the coagulation process in MMM casting or during MOF activation.

Figure 4 FTIR spectra of MIL-100(Al), PES, and MIL-100(Al)/PES MMMs with several different percentage additions of MIL-100(Al) to PES.
Figure 4

FTIR spectra of MIL-100(Al), PES, and MIL-100(Al)/PES MMMs with several different percentage additions of MIL-100(Al) to PES.

Table 2

Comparison of the absorption peaks of the PES from the research results with that of the PES from the literature

Absorption Wavenumber (cm−1)
PES literature [40] MIL-100(Al) PES/MIL-100(Al)
S═O 1,150 and 1,307 — 1,149 and 1,241
CSO2C 1,322 — 1,324
C–O 1,244, 1,260–1,000 1246 1,237 and 1,100
Ar C═C 1,587–1,489 1,372–1,481 1,576–1,487
O–H — 2,886–3,650 3,447

3.1.3 Scanning electron microscopy (SEM)

SEM analysis was used in this study to determine the morphology and particle size of the MIL-100(Al) and the effect of the addition of MIL-100(Al) to PES on the density of the MMMs. The morphology of the synthesized MIL-100(Al) showed an irregular shape (Figure 5) with an average particle size of 1.69 ± 0.35 µm (see ESI Figures S1). The morphological appearance of the MIL-100(Al) is in accordance with a study conducted by Feng et al. [33]. Differences in synthesis methods can affect morphology due to different solvents that are used, for example, the MIL-100(Al) synthesized by Volkringer et al. [30] under hydrothermal conditions using H2O and HNO3 solvents had an octahedral form.

Figure 5 Depiction of the synthesized MIL-100(Al).
Figure 5

Depiction of the synthesized MIL-100(Al).

The surface morphologies of the resulting MMMs are shown in Figure 6. The neat PES membrane is almost defect-free, representing the dense layer, and the surface images of MMM up to 20 wt% MIL-100(Al) loading also look like a dense membrane. However, the MIL-100(Al) does not appear to be homogenously distributed in the MMMs with 5 and 10% additions of MIL-100(Al). This may be occurred since the amount of MIL-100(Al) incorporated is very small. In contrast, the MIL-100(Al) is well distributed at a 20% addition, but at a 30% addition, the agglomeration has occurred that might be due to too large loading of MOFs, affecting membrane performance [13], and this is shown in Figure 6e. The effect of the addition of MIL-100(Al) can also be seen from the morphologies of the cross-sections (Figure 7). Each cross-section morphology appears as an asymmetrical structure with a dense top layer where the filler is located and a lower layer with a cavity formed like fingers, which accords with a previous study conducted by Qadir et al. [41]. The distribution of the aluminum from MIL-100(Al) in the membrane is demonstrated through EDX analysis as shown in Table 3 and Appendix 2.

Figure 6 Surface morphology of (a) PES, (b) PES/MIL-100(Al) 5%, (c) PES/MIL-100(Al) 10%, (d) PES/MIL-100(Al) 20%, and (e) PES/MIL-100(Al) 30%.
Figure 6

Surface morphology of (a) PES, (b) PES/MIL-100(Al) 5%, (c) PES/MIL-100(Al) 10%, (d) PES/MIL-100(Al) 20%, and (e) PES/MIL-100(Al) 30%.

Figure 7 Cross-section of morphological appearance of (a) PES, (b) PES/MIL-100(Al) 5%, (c) PES/MIL-100(Al) 10%, (d) PES/MIL-100(Al) 20%, and (e) PES/MIL-100(Al) 30%.
Figure 7

Cross-section of morphological appearance of (a) PES, (b) PES/MIL-100(Al) 5%, (c) PES/MIL-100(Al) 10%, (d) PES/MIL-100(Al) 20%, and (e) PES/MIL-100(Al) 30%.

Table 3

Results of the EDX analyses of the PES/MIL-100(Al) MMMs

Membrane %w/w C %w/w O %w/w Al
PES/MIL-100(Al) 5% 50.62 49.24 0.13
PES/MIL-100(Al) 10% 50.55 49.03 0.42
PES/MIL-100(Al) 20% 50.39 48.10 1.51
PES/MIL-100(Al) 30% 49.56 49.25 1.19

The addition of MIL-100(Al) to PES can increase the thickness of the dense layer as shown in Figure 8 and determine the nature of gas permeation. As shown in Figure 8, the dense layer thickness increases at higher MIL-100(Al) loading. It can be attributed since the exchange rate between the coagulant at the outer layer and the solvent is slower due to the high concentrated area of the polymer. It results in the delayed demixing, affecting the formation of the thicker dense layer.

Figure 8 The thickness of PES/MIL-100(Al) MMMs dense layer with different percentage additions of MIL-100(Al).
Figure 8

The thickness of PES/MIL-100(Al) MMMs dense layer with different percentage additions of MIL-100(Al).

3.1.4 Thermogravimetric analysis (TGA)

The thermal stability of the synthesized MIL-100(Al) was determined from TGA analysis. Figure 9 shows that there are two instances of mass reduction, occurring at temperatures below 200°C and at 500–550°C, which is in agreement with a previous study by Xia et al. [38]. The first mass reduction indicates loss of water molecules of approximately 11.09% at temperatures from 26 to 157°C, which is possible due to the loss of 6 water molecules. Two DMF molecules (ca. 21.12%) that were used during the purification were probably released at temperature range 162 to 277°C [30,38]. The third mass reduction was 49.99% at temperatures from 276 to 616°C due to the loss of two BTC ligand molecules. The total final product residue of 17.80% Al2O3 was obtained at 520°C [30]. The calculation of the mass reduction is given in ESI Appendix 3.

Figure 9 Thermogram of the synthesized MIL-100(Al).
Figure 9

Thermogram of the synthesized MIL-100(Al).

Figure 10 Thermogram of different percentage additions of MIL-100(Al) to PES.
Figure 10

Thermogram of different percentage additions of MIL-100(Al) to PES.

The addition of MIL-100(Al) to the MMMs to form PES/MIL-100(Al) increases the thermal stability of the MMMs by 40°C as compared with neat PES membrane (Figure 10), which had thermal stability of up to 500°C. This is because the thermal stability of MIL-100(Al) (600°C) is higher than that of PES [32]. The presence of filler inside the PES membrane can act as a barrier, obstructing the transport of degradation product.

3.1.5 Surface area analyzer (SAA)

SAA analysis was used to determine the surface area and pore chrematistics of the MIL-100(Al) material, including pore volume, pore radius, and pore size distribution. The results of the SAA analysis are shown through the adsorption–desorption isotherm graph in Figure 11.

Figure 11 Nitrogen sorption isotherm analysis of MIL-100(Al).
Figure 11

Nitrogen sorption isotherm analysis of MIL-100(Al).

The adsorption–desorption isotherm graph for MIL-100(Al), based on the International Union of Pure and Applied Chemistry classifications, shows type II, which indicates a nonporous or macropore material character [42]. Based on an analysis using the Brunauer–Emmett–Teller (BET) method, a surface area of 1.844 m2/g was obtained. The synthesized MIL-100(Al) does not have the same character as that shown in the study by Feng et al., where the MIL-100(Al) from a gel formation included microporous material (type I) with a BET surface area of 920 m2/g and a pore volume of 0.535 cm3/g [33]. Figure 12 shows the results for the MIL-100(Al) pore size distribution using the Barrett, Joyner, and Halenda (BJH) method with a pore volume and radius of 0.026 cc/g and 18.437 Å, respectively.

Figure 12 Graph of MIL-100(Al) pore distribution.
Figure 12

Graph of MIL-100(Al) pore distribution.

3.2 Gas separation performance of the PES/MIL-100(Al) MMMs

The gas separation performance by the MMMs can be known from a gas permeability test using a single gas (CO2, O2, and N2). A gas permeability test was used to determine the nature of the gas transport and the effect of different additions of MIL-100(Al) on the permeability and selectivity of the membranes. The results for the gas permeability tests for different additions of MIL-100(Al) to PES are shown in Figure 13, Table 4, and Appendix 4.

Figure 13 Gas permeability graph of CO2, O2, and N2 for different percentage additions of MIL-100 (Al) to PES.
Figure 13

Gas permeability graph of CO2, O2, and N2 for different percentage additions of MIL-100 (Al) to PES.

Table 4

Gas Permeability of the PES/MIL-100(Al) MMMs

Membrane Permeability (Barrer)
N2 O2 CO2
PES neat 564.52 ± 5.54 213.89 ± 6.81 570.03 ± 6.37
PES/MIL-100(Al) 5% 1149.91 ± 63.09 862.13 ± 157.42 1799.51 ± 23.09
PES/MIL-100(Al) 10% 824.62 ± 128.68 448.06 ± 26.78 1749.68 ± 99.05
PES/MIL-100(Al) 20% 1194.20 ± 139.31 492.21 ± 4.99 2210.77 ± 308.46
PES/MIL-100(Al) 30% 8536.14 ± 744.06 5743.87 ± 27.61 9741.99 ± 1519.91

Figure 13 shows that CO2 gas permeation was higher than that of N2 or O2. This is because the kinetic diameter of CO2 (3.20 Å) is smaller than that of O2 (3.46 Å) and N2 (3.64 Å) [42], which can affect gas flow. O2 gas has a smaller kinetic diameter than N2, but O2 (32) has a greater molecular weight than N2 (28), and thus molecular weight can also affect gas flow [44]. The addition of MIL-100(Al) to PES can increase permeability with a similar pattern of increase for each gas. Increasing the maximum permeability of the CO2, O2, and N2 gases with the addition of 30% MIL-100(Al) causes the permeability of the CO2 gas to increase 16 times (1,609%) from 570.03 ± 6.37 Barrer to 9741.99 ± 1519.91 Barrer, O2 gas to increase 26 times from 213.89 ± 6.81 Barrer to 5743.87 ± 27.61 Barrer, and N2 gas to increase 14 times from 564.52 ± 5.54 Barrers to 8536.14 ± 744.06 Barrers. The increase in CO2 gas permeability in these PES/MIL-100(Al) MMMs is greater than that of Matrimid®-based MMMs and UiO-66-NH2 type MOFs (∼200%) [24].

The addition of MIL-100(Al) fillers to PES/MIL-100(Al) MMMs can increase CO2/O2 gas selectivity as shown in Figure 14, Table 5, and Appendix 6. An addition of MIL-100(Al) of 20% can increase the selectivity for CO2/O2 gas separation from 2.67 ± 0.04 to 4.49 ± 0.67 (68.5%), which then decreases with an addition of MIL-100(Al) of 30%. This phenomenon is due to the presence of the filler agglomeration as shown in Figure 6e and permeability that is too high. The existence of agglomeration that is too large will reduce the performance of membrane separation [13]. CO2/N2 gas selectivity was increased by 110.1% to 2.16 ± 0.46 as compared to a neat PES membrane (1.01 ± 0.00) with an addition of MIL-100(Al) of 10%. The increase in the CO2 gas separation performance is influenced by polarity and high CO2 quadrupole moments as compared with N2 [45], causing the CO2 to be more easily adsorbed, and so the selectivity for CO2 increases. The increased selectivity for CO2/N2 from the obtained MMMs is higher than that of Matrimid®/UiO-66-NH2 MMMs (∼25%) [24].

Figure 14 Gas selectivity graph of CO2/O2, CO2/N2, and O2/N2 for different percentage additions of MIL-100(Al) to PES.
Figure 14

Gas selectivity graph of CO2/O2, CO2/N2, and O2/N2 for different percentage additions of MIL-100(Al) to PES.

Table 5

The selectivity of the PES/MIL-100(Al) MMMs

Membrane Selectivity
O2/N2 CO2/N2 CO2/O2
PES neat 0.38 ± 0.01 1.01 ± 0.00 2.67 ± 0.04
PES/MIL-100(Al) 5% 0.75 ± 0.18 1.57 ± 0.11 2.12 ± 0.36
PES/MIL-100(Al) 10% 0.55 ± 0.12 2.16 ± 0.46 3.91 ± 0.01
PES/MIL-100(Al) 20% 0.42 ± 0.05 1.85 ± 0.04 4.49 ± 0.67
PES/MIL-100(Al) 30% 0.68 ± 0.06 1.15 ± 0.28 1.70 ± 0.26
Knudsen selectivity [47] 0.94 0.80 0.85

The gas transport in the membrane is controlled by the solution–diffusion mechanism of PES matrix with a portion of the filler particles. The MIL-100(Al) particles have pores of about 1.8 nm, which is microporous and below the region of Knudsen diffusion. Also, the Knudsen selectivity values are not in agreement with calculated selectivity values (Table 5), indicating that the gas transport is not controlled by the Knudsen mechanism. The pore of MIL-100(Al) is bigger than the gas molecular diameter, leading to the conclusion that the transport mechanism is not controlled by molecular sieving. The transport mechanism can be explained by surface diffusion, with a mechanism of more favorable surface diffusion of fast, lower kinetic diameter gas (CO2), relative to slow, larger kinetic diameter gas (O2 and N2), followed by gas diffusion in the MIL pores. CO2 gas has higher polarizability and quadrupole moments (29.11 × 1025/cm3 and 4.30 × 1026/esu cm2, respectively) as compared with N2 (17.403 × 1025/cm3; 1.52 × 1026/esu cm2) or O2 gas (15.812 × 1025/cm3; 0.39 × 1026/esu cm2) [45]. This shows that CO2 gas can be adsorbed more selectively than N2 or O2 gas due to the greater presence of CO2 quadrupole moments that can affect the gas separation selectivity [45]. In addition, after the activation process, the metal ions in MIL-100(Al) do not have coordinatively saturated bonds, allowing the CO2 gas to be easily adsorbed. The interaction with the absorbed gas shows a strong activity to adsorb in the pore walls, thus gas separation occurs based on surface diffusion [46].

The separation of O2/N2 gas with an addition of 30% MIL-100(Al) increased selectivity by 97.9% to 0.75 ± 0.18 as compared with neat PES (0.38 ± 0.01). However, the O2/N2 performance has lower selectivity than CO2/O2 or CO2/N2. This is because gas permeation is influenced by the molecular weight of O2 (32), which is greater than that of N2 (28) [44]. As a result, gas permeation based on Knudsen diffusion, as shown by produced O2/N2 selectivity, is close to Knudsen selectivity (0.94). Knudsen selectivity is calculated based on equation (3) [47].

(3) α i , j = M j M i

where, α i , j is the selectivity of the membrane in gases i and j, M i is the molecular weight of gas i, and M j is the molecular weight of gas j.

The successful preparation of the MMMs can be evaluated by comparing them with the Robeson upper bound as a dividing boundary between organic and inorganic polymer membranes. The for O2/N2 (Figure 15) and CO2/N2 gas separation performance (Figure 16) of the produced MMMs has not been able to reach the upper bound due to low selectivity, but different additions of MIL-100(Al) can push gas permeation performance toward the upper bound as compared with neat PES membranes, so the preparation of the PES/MIL-100(Al) MMMs can be categorized as successful.

Figure 15 Comparison of the O2/N2 gas separation performance as compared with the literature [48,49].
Figure 15

Comparison of the O2/N2 gas separation performance as compared with the literature [48,49].

Figure 16 Comparison of CO2/N2 gas separation performance as compared with the literature [49].
Figure 16

Comparison of CO2/N2 gas separation performance as compared with the literature [49].

4 Conclusion

The addition of MIL-100(Al) to PES can affect the characteristics of the produced MMMs, including an increase in thermal stability of 40°C and in the thickness of the dense membrane layer of up to 3.70 μm. Moreover, the addition of MIL-100(Al) to PES can improve membrane performance for the permeability of CO2, O2, and N2 gases by 16, 26, and 14 times, respectively, as compared with neat PES membranes. Furthermore, an addition of 20% MIL-100(Al) can increase the selectivity for CO2/O2 gas separation from 2.67 to 4.49. CO2/N2 gas selectivity can be increased from 1.01 to 2.12 with an addition of 10% MIL-100(Al) as filler. Another strategy for increasing membrane performance is to modify the membrane surface with the use of a coating material such as polydimethylsiloxane.

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Acknowledgments

The authors acknowledge Dr. rer. nat. Ubed Sonai Fahruddin Arrozzi from the State University of Malang for the nitrogen sorption isotherm measurement and Dr. Grandprix T. M. Kadja from Bandung Institute of Technology for the thermogravimetry measurement. Moreover, we thank the Ministry of Research, Technology and Higher Education of the Republic of Indonesia through the University Leading Fundamental Research Grant (PDUPT) 2021 for funding.

  1. Funding information: The funding of this research was supported by the Ministry of Research, Technology and Higher Education of the Republic of Indonesia through the University Leading Fundamental Research Grant (PDUPT) 2021.

  2. Authors’ contributions: W. W. L. – conceptualization; W. W. L., N. W., D. S. H. – data curation; R. A. A., R. W. – formal analysis: W. W. L. – funding acquisition; R. A. A., M. A. K. – investigation; R. A. A., M. A. K., R. W. – methodology; W. W. L. – project administration; W. W. L., N. W. – resources; R. A. A., M. A. K. – software; W. W. L, N. W. – supervision; W. W. L, N. W. – validation; R. A. A., M. A. K., R. W. – visualization; R. A. A., W. W. L. – writing – original draft; W. W. L., D. S. H., N. W., R. W. – writing – review & editing.

  3. Conflict of interest: Authors state no conflict of interest.

  4. Data availability statement: All data generated or analyzed during this study are included in this published article [and its supplementary information files].

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Received: 2019-11-21
Revised: 2021-02-01
Accepted: 2021-02-09
Published Online: 2021-03-12

© 2021 Witri Wahyu Lestari et al., published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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  59. Presence of short and cyclic peptides in Acacia and Ziziphus honeys may potentiate their medicinal values
  60. The role of vitamin D deficiency and elevated inflammatory biomarkers as risk factors for the progression of diabetic nephropathy in patients with type 2 diabetes mellitus
  61. Quantitative structure–activity relationship study on prolonged anticonvulsant activity of terpene derivatives in pentylenetetrazole test
  62. GADD45B induced the enhancing of cell viability and proliferation in radiotherapy and increased the radioresistance of HONE1 cells
  63. Cannabis sativa L. chemical compositions as potential plasmodium falciparum dihydrofolate reductase-thymidinesynthase enzyme inhibitors: An in silico study for drug development
  64. Dynamics of λ-cyhalothrin disappearance and expression of selected P450 genes in bees depending on the ambient temperature
  65. Identification of synthetic cannabinoid methyl 2-{[1-(cyclohexylmethyl)-1H-indol-3-yl] formamido}-3-methylbutanoate using modern mass spectrometry and nuclear magnetic resonance techniques
  66. Study on the speciation of arsenic in the genuine medicinal material honeysuckle
  67. Two Cu(ii)-based coordination polymers: Crystal structures and treatment activity on periodontitis
  68. Conversion of furfuryl alcohol to ethyl levulinate in the presence of mesoporous aluminosilicate catalyst
  69. Review Articles
  70. Hsien Wu and his major contributions to the chemical era of immunology
  71. Overview of the major classes of new psychoactive substances, psychoactive effects, analytical determination and conformational analysis of selected illegal drugs
  72. An overview of persistent organic pollutants along the coastal environment of Kuwait
  73. Mechanism underlying sevoflurane-induced protection in cerebral ischemia–reperfusion injury
  74. COVID-19 and SARS-CoV-2: Everything we know so far – A comprehensive review
  75. Challenge of diabetes mellitus and researchers’ contributions to its control
  76. Advances in the design and application of transition metal oxide-based supercapacitors
  77. Color and composition of beauty products formulated with lemongrass essential oil: Cosmetics formulation with lemongrass essential oil
  78. The structural chemistry of zinc(ii) and nickel(ii) dithiocarbamate complexes
  79. Bioprospecting for antituberculosis natural products – A review
  80. Recent progress in direct urea fuel cell
  81. Rapid Communications
  82. A comparative morphological study of titanium dioxide surface layer dental implants
  83. Changes in the antioxidative properties of honeys during their fermentation
  84. Erratum
  85. Erratum to “Corrosion study of copper in aqueous sulfuric acid solution in the presence of (2E,5E)-2,5-dibenzylidenecyclopentanone and (2E,5E)-bis[(4-dimethylamino)benzylidene]cyclopentanone: Experimental and theoretical study”
  86. Erratum to “Modified TDAE petroleum plasticiser”
  87. Corrigendum
  88. Corrigendum to “A nitric oxide-releasing prodrug promotes apoptosis in human renal carcinoma cells: Involvement of reactive oxygen species”
  89. Special Issue on 3rd IC3PE 2020
  90. Visible light-responsive photocatalyst of SnO2/rGO prepared using Pometia pinnata leaf extract
  91. Antihyperglycemic activity of Centella asiatica (L.) Urb. leaf ethanol extract SNEDDS in zebrafish (Danio rerio)
  92. Selection of oil extraction process from Chlorella species of microalgae by using multi-criteria decision analysis technique for biodiesel production
  93. Special Issue on the 14th Joint Conference of Chemistry (14JCC)
  94. Synthesis and in vitro cytotoxicity evaluation of isatin-pyrrole derivatives against HepG2 cell line
  95. CO2 gas separation using mixed matrix membranes based on polyethersulfone/MIL-100(Al)
  96. Effect of synthesis and activation methods on the character of CoMo/ultrastable Y-zeolite catalysts
  97. Special Issue on Electrochemical Amplified Sensors
  98. Enhancement of graphene oxide through β-cyclodextrin composite to sensitive analysis of an antidepressant: Sulpiride
  99. Investigation of the spectroelectrochemical behavior of quercetin isolated from Zanthoxylum bungeanum
  100. An electrochemical sensor for high sensitive determination of lysozyme based on the aptamer competition approach
  101. An improved non-enzymatic electrochemical sensor amplified with CuO nanostructures for sensitive determination of uric acid
  102. Special Issue on Applied Biochemistry and Biotechnology 2020
  103. Fast discrimination of avocado oil for different extracted methods using headspace-gas chromatography-ion mobility spectroscopy with PCA based on volatile organic compounds
  104. Effect of alkali bases on the synthesis of ZnO quantum dots
  105. Quality evaluation of Cabernet Sauvignon wines in different vintages by 1H nuclear magnetic resonance-based metabolomics
  106. Special Issue on the Joint Science Congress of Materials and Polymers (ISCMP 2019)
  107. Diatomaceous Earth: Characterization, thermal modification, and application
  108. Electrochemical determination of atenolol and propranolol using a carbon paste sensor modified with natural ilmenite
  109. Special Issue on the Conference of Energy, Fuels, Environment 2020
  110. Assessment of the mercury contamination of landfilled and recovered foundry waste – a case study
  111. Primary energy consumption in selected EU Countries compared to global trends
  112. Modified TDAE petroleum plasticiser
  113. Use of glycerol waste in lactic acid bacteria metabolism for the production of lactic acid: State of the art in Poland
  114. Topical Issue on Applications of Mathematics in Chemistry
  115. Theoretical study of energy, inertia and nullity of phenylene and anthracene
  116. Banhatti, revan and hyper-indices of silicon carbide Si2C3-III[n,m]
  117. Topical Issue on Agriculture
  118. Occurrence of mycotoxins in selected agricultural and commercial products available in eastern Poland
  119. Special Issue on Ethnobotanical, Phytochemical and Biological Investigation of Medicinal Plants
  120. Acute and repeated dose 60-day oral toxicity assessment of chemically characterized Berberis hispanica Boiss. and Reut in Wistar rats
  121. Phytochemical profile, in vitro antioxidant, and anti-protein denaturation activities of Curcuma longa L. rhizome and leaves
  122. Antiplasmodial potential of Eucalyptus obliqua leaf methanolic extract against Plasmodium vivax: An in vitro study
  123. Prunus padus L. bark as a functional promoting component in functional herbal infusions – cyclooxygenase-2 inhibitory, antioxidant, and antimicrobial effects
  124. Molecular and docking studies of tetramethoxy hydroxyflavone compound from Artemisia absinthium against carcinogens found in cigarette smoke
  125. Special Issue on the Joint Science Congress of Materials and Polymers (ISCMP 2020)
  126. Preparation of cypress (Cupressus sempervirens L.) essential oil loaded poly(lactic acid) nanofibers
  127. Influence of mica mineral on flame retardancy and mechanical properties of intumescent flame retardant polypropylene composites
  128. Production and characterization of thermoplastic elastomer foams based on the styrene–ethylene–butylene–styrene (SEBS) rubber and thermoplastic material
  129. Special Issue on Applied Chemistry in Agriculture and Food Science
  130. Impact of essential oils on the development of pathogens of the Fusarium genus and germination parameters of selected crops
  131. Yield, volume, quality, and reduction of biotic stress influenced by titanium application in oilseed rape, winter wheat, and maize cultivations
  132. Influence of potato variety on polyphenol profile composition and glycoalcaloid contents of potato juice
  133. Carryover effect of direct-fed microbial supplementation and early weaning on the growth performance and carcass characteristics of growing Najdi lambs
  134. Special Issue on Applied Biochemistry and Biotechnology (ABB 2021)
  135. The electrochemical redox mechanism and antioxidant activity of polyphenolic compounds based on inlaid multi-walled carbon nanotubes-modified graphite electrode
  136. Study of an adsorption method for trace mercury based on Bacillus subtilis
  137. Special Issue on The 1st Malaysia International Conference on Nanotechnology & Catalysis (MICNC2021)
  138. Mitigating membrane biofouling in biofuel cell system – A review
  139. Mechanical properties of polymeric biomaterials: Modified ePTFE using gamma irradiation
https://doi.org/10.1515/chem-2021-0033
Schlagwörter für diesen Artikel
CO2; MMMs; MIL-100(Al); PES
Creative Commons
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Artikel in diesem Heft

  1. Regular Articles
  2. Qualitative and semi-quantitative assessment of anthocyanins in Tibetan hulless barley from different geographical locations by UPLC-QTOF-MS and their antioxidant capacities
  3. Effect of sodium chloride on the expression of genes involved in the salt tolerance of Bacillus sp. strain “SX4” isolated from salinized greenhouse soil
  4. GC-MS analysis of mango stem bark extracts (Mangifera indica L.), Haden variety. Possible contribution of volatile compounds to its health effects
  5. Influence of nanoscale-modified apatite-type calcium phosphates on the biofilm formation by pathogenic microorganisms
  6. Removal of paracetamol from aqueous solution by containment composites
  7. Investigating a human pesticide intoxication incident: The importance of robust analytical approaches
  8. Induction of apoptosis and cell cycle arrest by chloroform fraction of Juniperus phoenicea and chemical constituents analysis
  9. Recovery of γ-Fe2O3 from copper ore tailings by magnetization roasting and magnetic separation
  10. Effects of different extraction methods on antioxidant properties of blueberry anthocyanins
  11. Modeling the removal of methylene blue dye using a graphene oxide/TiO2/SiO2 nanocomposite under sunlight irradiation by intelligent system
  12. Antimicrobial and antioxidant activities of Cinnamomum cassia essential oil and its application in food preservation
  13. Full spectrum and genetic algorithm-selected spectrum-based chemometric methods for simultaneous determination of azilsartan medoxomil, chlorthalidone, and azilsartan: Development, validation, and application on commercial dosage form
  14. Evaluation of the performance of immunoblot and immunodot techniques used to identify autoantibodies in patients with autoimmune diseases
  15. Computational studies by molecular docking of some antiviral drugs with COVID-19 receptors are an approach to medication for COVID-19
  16. Synthesis of amides and esters containing furan rings under microwave-assisted conditions
  17. Simultaneous removal efficiency of H2S and CO2 by high-gravity rotating packed bed: Experiments and simulation
  18. Design, synthesis, and biological activities of novel thiophene, pyrimidine, pyrazole, pyridine, coumarin and isoxazole: Dydrogesterone derivatives as antitumor agents
  19. Content and composition analysis of polysaccharides from Blaps rynchopetera and its macrophage phagocytic activity
  20. A new series of 2,4-thiazolidinediones endowed with potent aldose reductase inhibitory activity
  21. Assessing encapsulation of curcumin in cocoliposome: In vitro study
  22. Rare norisodinosterol derivatives from Xenia umbellata: Isolation and anti-proliferative activity
  23. Comparative study of antioxidant and anticancer activities and HPTLC quantification of rutin in white radish (Raphanus sativus L.) leaves and root extracts grown in Saudi Arabia
  24. Comparison of adsorption properties of commercial silica and rice husk ash (RHA) silica: A study by NIR spectroscopy
  25. Sodium borohydride (NaBH4) as a high-capacity material for next-generation sodium-ion capacitors
  26. Aroma components of tobacco powder from different producing areas based on gas chromatography ion mobility spectrometry
  27. The effects of salinity on changes in characteristics of soils collected in a saline region of the Mekong Delta, Vietnam
  28. Synthesis, properties, and activity of MoVTeNbO catalysts modified by zirconia-pillared clays in oxidative dehydrogenation of ethane
  29. Synthesis and crystal structure of N,N′-bis(4-chlorophenyl)thiourea N,N-dimethylformamide
  30. Quantitative analysis of volatile compounds of four Chinese traditional liquors by SPME-GC-MS and determination of total phenolic contents and antioxidant activities
  31. A novel separation method of the valuable components for activated clay production wastewater
  32. On ve-degree- and ev-degree-based topological properties of crystallographic structure of cuprite Cu2O
  33. Antihyperglycemic effect and phytochemical investigation of Rubia cordifolia (Indian Madder) leaves extract
  34. Microsphere molecularly imprinted solid-phase extraction for diazepam analysis using itaconic acid as a monomer in propanol
  35. A nitric oxide-releasing prodrug promotes apoptosis in human renal carcinoma cells: Involvement of reactive oxygen species
  36. Machine vision-based driving and feedback scheme for digital microfluidics system
  37. Study on the application of a steam-foam drive profile modification technology for heavy oil reservoir development
  38. Ni–Ru-containing mixed oxide-based composites as precursors for ethanol steam reforming catalysts: Effect of the synthesis methods on the structural and catalytic properties
  39. Preparation of composite soybean straw-based materials by LDHs modifying as a solid sorbent for removal of Pb(ii) from water samples
  40. Synthesis and spectral characterizations of vanadyl(ii) and chromium(iii) mixed ligand complexes containing metformin drug and glycine amino acid
  41. In vitro evaluation of lactic acid bacteria with probiotic activity isolated from local pickled leaf mustard from Wuwei in Anhui as substitutes for chemical synthetic additives
  42. Utilization and simulation of innovative new binuclear Co(ii), Ni(ii), Cu(ii), and Zn(ii) diimine Schiff base complexes in sterilization and coronavirus resistance (Covid-19)
  43. Phosphorylation of Pit-1 by cyclin-dependent kinase 5 at serine 126 is associated with cell proliferation and poor prognosis in prolactinomas
  44. Molecularly imprinted membrane for transport of urea, creatinine, and vitamin B12 as a hemodialysis candidate membrane
  45. Optimization of Murrayafoline A ethanol extraction process from the roots of Glycosmis stenocarpa, and evaluation of its Tumorigenesis inhibition activity on Hep-G2 cells
  46. Highly sensitive determination of α-lipoic acid in pharmaceuticals on a boron-doped diamond electrode
  47. Synthesis, chemo-informatics, and anticancer evaluation of fluorophenyl-isoxazole derivatives
  48. In vitro and in vivo investigation of polypharmacology of propolis extract as anticancer, antibacterial, anti-inflammatory, and chemical properties
  49. Topological indices of bipolar fuzzy incidence graph
  50. Preparation of Fe3O4@SiO2–ZnO catalyst and its catalytic synthesis of rosin glycol ester
  51. Construction of a new luminescent Cd(ii) compound for the detection of Fe3+ and treatment of Hepatitis B
  52. Investigation of bovine serum albumin aggregation upon exposure to silver(i) and copper(ii) metal ions using Zetasizer
  53. Discoloration of methylene blue at neutral pH by heterogeneous photo-Fenton-like reactions using crystalline and amorphous iron oxides
  54. Optimized extraction of polyphenols from leaves of Rosemary (Rosmarinus officinalis L.) grown in Lam Dong province, Vietnam, and evaluation of their antioxidant capacity
  55. Synthesis of novel thiourea-/urea-benzimidazole derivatives as anticancer agents
  56. Potency and selectivity indices of Myristica fragrans Houtt. mace chloroform extract against non-clinical and clinical human pathogens
  57. Simple modifications of nicotinic, isonicotinic, and 2,6-dichloroisonicotinic acids toward new weapons against plant diseases
  58. Synthesis, optical and structural characterisation of ZnS nanoparticles derived from Zn(ii) dithiocarbamate complexes
  59. Presence of short and cyclic peptides in Acacia and Ziziphus honeys may potentiate their medicinal values
  60. The role of vitamin D deficiency and elevated inflammatory biomarkers as risk factors for the progression of diabetic nephropathy in patients with type 2 diabetes mellitus
  61. Quantitative structure–activity relationship study on prolonged anticonvulsant activity of terpene derivatives in pentylenetetrazole test
  62. GADD45B induced the enhancing of cell viability and proliferation in radiotherapy and increased the radioresistance of HONE1 cells
  63. Cannabis sativa L. chemical compositions as potential plasmodium falciparum dihydrofolate reductase-thymidinesynthase enzyme inhibitors: An in silico study for drug development
  64. Dynamics of λ-cyhalothrin disappearance and expression of selected P450 genes in bees depending on the ambient temperature
  65. Identification of synthetic cannabinoid methyl 2-{[1-(cyclohexylmethyl)-1H-indol-3-yl] formamido}-3-methylbutanoate using modern mass spectrometry and nuclear magnetic resonance techniques
  66. Study on the speciation of arsenic in the genuine medicinal material honeysuckle
  67. Two Cu(ii)-based coordination polymers: Crystal structures and treatment activity on periodontitis
  68. Conversion of furfuryl alcohol to ethyl levulinate in the presence of mesoporous aluminosilicate catalyst
  69. Review Articles
  70. Hsien Wu and his major contributions to the chemical era of immunology
  71. Overview of the major classes of new psychoactive substances, psychoactive effects, analytical determination and conformational analysis of selected illegal drugs
  72. An overview of persistent organic pollutants along the coastal environment of Kuwait
  73. Mechanism underlying sevoflurane-induced protection in cerebral ischemia–reperfusion injury
  74. COVID-19 and SARS-CoV-2: Everything we know so far – A comprehensive review
  75. Challenge of diabetes mellitus and researchers’ contributions to its control
  76. Advances in the design and application of transition metal oxide-based supercapacitors
  77. Color and composition of beauty products formulated with lemongrass essential oil: Cosmetics formulation with lemongrass essential oil
  78. The structural chemistry of zinc(ii) and nickel(ii) dithiocarbamate complexes
  79. Bioprospecting for antituberculosis natural products – A review
  80. Recent progress in direct urea fuel cell
  81. Rapid Communications
  82. A comparative morphological study of titanium dioxide surface layer dental implants
  83. Changes in the antioxidative properties of honeys during their fermentation
  84. Erratum
  85. Erratum to “Corrosion study of copper in aqueous sulfuric acid solution in the presence of (2E,5E)-2,5-dibenzylidenecyclopentanone and (2E,5E)-bis[(4-dimethylamino)benzylidene]cyclopentanone: Experimental and theoretical study”
  86. Erratum to “Modified TDAE petroleum plasticiser”
  87. Corrigendum
  88. Corrigendum to “A nitric oxide-releasing prodrug promotes apoptosis in human renal carcinoma cells: Involvement of reactive oxygen species”
  89. Special Issue on 3rd IC3PE 2020
  90. Visible light-responsive photocatalyst of SnO2/rGO prepared using Pometia pinnata leaf extract
  91. Antihyperglycemic activity of Centella asiatica (L.) Urb. leaf ethanol extract SNEDDS in zebrafish (Danio rerio)
  92. Selection of oil extraction process from Chlorella species of microalgae by using multi-criteria decision analysis technique for biodiesel production
  93. Special Issue on the 14th Joint Conference of Chemistry (14JCC)
  94. Synthesis and in vitro cytotoxicity evaluation of isatin-pyrrole derivatives against HepG2 cell line
  95. CO2 gas separation using mixed matrix membranes based on polyethersulfone/MIL-100(Al)
  96. Effect of synthesis and activation methods on the character of CoMo/ultrastable Y-zeolite catalysts
  97. Special Issue on Electrochemical Amplified Sensors
  98. Enhancement of graphene oxide through β-cyclodextrin composite to sensitive analysis of an antidepressant: Sulpiride
  99. Investigation of the spectroelectrochemical behavior of quercetin isolated from Zanthoxylum bungeanum
  100. An electrochemical sensor for high sensitive determination of lysozyme based on the aptamer competition approach
  101. An improved non-enzymatic electrochemical sensor amplified with CuO nanostructures for sensitive determination of uric acid
  102. Special Issue on Applied Biochemistry and Biotechnology 2020
  103. Fast discrimination of avocado oil for different extracted methods using headspace-gas chromatography-ion mobility spectroscopy with PCA based on volatile organic compounds
  104. Effect of alkali bases on the synthesis of ZnO quantum dots
  105. Quality evaluation of Cabernet Sauvignon wines in different vintages by 1H nuclear magnetic resonance-based metabolomics
  106. Special Issue on the Joint Science Congress of Materials and Polymers (ISCMP 2019)
  107. Diatomaceous Earth: Characterization, thermal modification, and application
  108. Electrochemical determination of atenolol and propranolol using a carbon paste sensor modified with natural ilmenite
  109. Special Issue on the Conference of Energy, Fuels, Environment 2020
  110. Assessment of the mercury contamination of landfilled and recovered foundry waste – a case study
  111. Primary energy consumption in selected EU Countries compared to global trends
  112. Modified TDAE petroleum plasticiser
  113. Use of glycerol waste in lactic acid bacteria metabolism for the production of lactic acid: State of the art in Poland
  114. Topical Issue on Applications of Mathematics in Chemistry
  115. Theoretical study of energy, inertia and nullity of phenylene and anthracene
  116. Banhatti, revan and hyper-indices of silicon carbide Si2C3-III[n,m]
  117. Topical Issue on Agriculture
  118. Occurrence of mycotoxins in selected agricultural and commercial products available in eastern Poland
  119. Special Issue on Ethnobotanical, Phytochemical and Biological Investigation of Medicinal Plants
  120. Acute and repeated dose 60-day oral toxicity assessment of chemically characterized Berberis hispanica Boiss. and Reut in Wistar rats
  121. Phytochemical profile, in vitro antioxidant, and anti-protein denaturation activities of Curcuma longa L. rhizome and leaves
  122. Antiplasmodial potential of Eucalyptus obliqua leaf methanolic extract against Plasmodium vivax: An in vitro study
  123. Prunus padus L. bark as a functional promoting component in functional herbal infusions – cyclooxygenase-2 inhibitory, antioxidant, and antimicrobial effects
  124. Molecular and docking studies of tetramethoxy hydroxyflavone compound from Artemisia absinthium against carcinogens found in cigarette smoke
  125. Special Issue on the Joint Science Congress of Materials and Polymers (ISCMP 2020)
  126. Preparation of cypress (Cupressus sempervirens L.) essential oil loaded poly(lactic acid) nanofibers
  127. Influence of mica mineral on flame retardancy and mechanical properties of intumescent flame retardant polypropylene composites
  128. Production and characterization of thermoplastic elastomer foams based on the styrene–ethylene–butylene–styrene (SEBS) rubber and thermoplastic material
  129. Special Issue on Applied Chemistry in Agriculture and Food Science
  130. Impact of essential oils on the development of pathogens of the Fusarium genus and germination parameters of selected crops
  131. Yield, volume, quality, and reduction of biotic stress influenced by titanium application in oilseed rape, winter wheat, and maize cultivations
  132. Influence of potato variety on polyphenol profile composition and glycoalcaloid contents of potato juice
  133. Carryover effect of direct-fed microbial supplementation and early weaning on the growth performance and carcass characteristics of growing Najdi lambs
  134. Special Issue on Applied Biochemistry and Biotechnology (ABB 2021)
  135. The electrochemical redox mechanism and antioxidant activity of polyphenolic compounds based on inlaid multi-walled carbon nanotubes-modified graphite electrode
  136. Study of an adsorption method for trace mercury based on Bacillus subtilis
  137. Special Issue on The 1st Malaysia International Conference on Nanotechnology & Catalysis (MICNC2021)
  138. Mitigating membrane biofouling in biofuel cell system – A review
  139. Mechanical properties of polymeric biomaterials: Modified ePTFE using gamma irradiation
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