One-Pot Synthesis and Surfactant Removal from MCM-41 Using Microwave Irradiation.

This research pioneers the application of microwave irradiation as an innovative strategy for one-pot synthesis and surfactant elimination (cetyltrimethylammonium bromide-CTAB) from MCM-41, introducing a rapid and efficient methodology. MCM-41 silica is widely utilized in various applications due to its unique textural and structural properties. Nonetheless, the presence of residual surfactants after synthesis poses a challenge to its effective application. MCM-41 synthesis, conducted in a microwave reactor at 60 °C, provided a result within 0.5 to 1 h. Comprehensive analyses of structural, chemical, morphological, and surface characteristics were undertaken, with a focus on the impact of synthesis time on these properties. Surfactant extraction involved the use of ethanol as a solvent at 120 °C for 6 min within the microwave reactor. The acquired particles, coupled with the properties of textural and structural features, affirmed the efficacy of the synthesis process, resulting in the synthesis of MCM-41 within 36 min. This study presents the first instance of one-pot synthesis and surfactant removal from MCM-41 using a microwave reactor. The proposed method not only addresses the surfactant removal challenge, but also substantially accelerates the synthesis process, thereby enhancing the potential for MCM-41's application in diverse fields.

Microwave-Assisted Synthesis of Zeolite A from Metakaolinite for CO2 Adsorption.

The global demand for energy and industrial growth has generated an exponential use of fossil fuels in recent years. It is well known that carbon dioxide (CO2) is mainly produced, but not only from fuels, which has a negative impact on the environment, such as the increasing emission of greenhouse gases. Thus, thinking about reducing this problem, this study analyzes microwave irradiation as an alternative to conventional heating to optimize zeolite A synthesis conditions for CO2 capture. Synthesis reaction parameters such as different temperatures (60-150 °C) and different time durations (1-6 h) were evaluated. The CO2 adsorption capacity was evaluated by CO2 adsorption-desorption isotherms at 25 °C and atmospheric pressure. The results showed that the synthesis of zeolite A by microwave irradiation was successfully obtained from natural kaolinite (via metakaolinization), reducing both temperature and time. Adsorption isotherms show that the most promising adsorbent for CO2 capture is a zeolite synthesized at 100 °C for 4 h, which reached an adsorption capacity of 2.2 mmol/g.

A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in 'Metal Efficient' Palladium/In2 O3 /Al2 O3 Catalysts for CO2 Hydrogenation.

CO2 hydrogenation to methanol has the potential to serve as a sustainable route to a wide variety of hydrocarbons, fuels and plastics in the quest for net zero. Synergistic Pd/In2 O3 (Palldium on Indium Oxide) catalysts show high CO2 conversion and methanol selectivity, enhancing methanol yield. The identity of the optimal active site for this reaction is unclear, either as a Pd-In alloy, proximate metals, or distinct sites. In this work, we demonstrate that metal-efficient Pd/In2 O3 species dispersed on Al2 O3 can match the performance of pure Pd/In2 O3 systems. Further, we follow the evolution of both Pd and In sites, and surface species, under operando reaction conditions using X-ray Absorption Spectroscpy (XAS) and infrared (IR) spectroscopy. In doing so, we can determine both the nature of the active sites and the influence on the catalytic mechanism.

Shared Hydrogen Atom Location and Chemical Composition in Picolinic Acid and Pyridoxal Hydrochloride Derivatives Determined by X-ray Crystallography.

Three new single-crystal structures were isolated for picolinic acid (2), the trifluoroacetate salt of picolinic acid (1), and pyridoxal hydrochloride (3). These compounds displayed unconventional crystallographic features that must be considered when structural refinements are carried out. Thus, the generated Fourier differences map obtained with the diffraction data collected at 100 K was crucial to visualize electron densities, which were balanced by either one hydrogen atom or a hydrogen atom with an occupancy factor of 1/2 located between either two carboxylate moieties, two phenolic oxygen atoms, or two pyridinic nitrogen atoms. Moreover, NMR studies were conducted to analyze the bulk chemical composition of single crystals of 2-pyridinecarboxylic acid obtained from the gem-diol/hemiacetal forms and the polymerization products after the treatment of 2-pyridinecarboxaldehyde with TFA:H2O (1) or a diluted Cu(NO3)2 solution (2). The quantitative yield of the pyridoxal hydrochloride crystalline material (3) obtained from a diluted CuCl2 solution was exhaustively characterized by solid-state NMR methods. These methods allowed the resolution of the signals corresponding to the protons of the hydroxyl moiety of the intramolecular hemiacetal group and the phenolic hydrogen. Theoretical calculations using DFT methods were done to complement the atomic location of the hydrogen atoms obtained from the X-ray analysis.

Different behavior of two iso-structural zeolitic imidazolate frameworks in ethane-ethylene separation: Study of H2 -CO2 and CH4 -CO2 separation capacity.

The separation of ethane-ethylene mixtures was evaluated using two zeolitic imidazolate frameworks, which are only different from the assemble metal, as stationary phase from inverse gas chromatography data. The chromatographic profiles exhibited peaks adequately resolved. Separation is attributed to the pore sizes of the adsorbents that discern between ethane and ethylene molecule shapes and closed kinetic diameters. The adsorption heats were estimated for each probe molecule from the slopes of the straight lines at four temperatures. The evaluated materials are iso-structural compounds with the unique difference of assembling metal (cobalt and zinc). Cobalt material showed atypical adsorption of ethane over ethylene, which was observed taking into account the retarded elution of the paraffin. Therefore, the anomalous behavior could be ascribed to the presence of cobalt(II). Structural characterization of both materials was performed by X-ray powder diffraction, X-ray photoelectronic spectroscopy, and thermogravimetry, while morphological characterization was performed by scanning electron microscopy. H2 -CO2 and CH4 -CO2 mixtures separation were also evaluated by inverse gas chromatography. Both materials were able to separate these two mixtures. CO2 was the highest retained probe molecule due to the presence of quadrupole moment.

Protein Adsorption onto Modified Porous Silica by Single and Binary Human Serum Protein Solutions.

Typical porous silica (SBA-15) has been modified with pore expander agent (1,3,5-trimethylbenzene) and fluoride-species to diminish the length of the channels to obtain materials with different textural properties, varying the Si/Zr molar ratio between 20 and 5. These porous materials were characterized by X-ray Diffraction (XRD), N2 adsorption/desorption isotherms at -196 °C and X-ray Photoelectron Spectroscopy (XPS), obtaining adsorbent with a surface area between 420-337 m2 g-1 and an average pore diameter with a maximum between 20-25 nm. These materials were studied in the adsorption of human blood serum proteins (human serum albumin-HSA and immunoglobulin G-IgG). Generally, the incorporation of small proportions was favorable for proteins adsorption. The adsorption data revealed that the maximum adsorption capacity was reached close to the pI. The batch purification experiments in binary human serum solutions showed that Si sample has considerable adsorption for IgG while HSA adsorption is relatively low, so it is possible its separation.

Tuning of Trifunctional NiCu Bimetallic Nanoparticles Confined in a Porous Carbon Network with Surface Composition and Local Structural Distortions for the Electrocatalytic Oxygen Reduction, Oxygen and Hydrogen Evolution Reactions.

The rational design of multifunctional catalysts that use non-noble metals to facilitate the interconversion between H2, O2, and H2O is an intense area of investigation. Bimetallic nanosystems with highly tunable electronic, structural, and catalytic properties that depend on their composition, structure, and size have attracted considerable attention. Herein, we report the synthesis of bimetallic nickel-copper (NiCu) alloy nanoparticles confined in a sp2 carbon framework that exhibits trifunctional catalytic properties toward hydrogen evolution (HER), oxygen reduction (ORR), and oxygen evolution (OER) reactions. The electrocatalytic functions of the NiCu nanoalloys were experimentally and theoretically correlated with the composition-dependent local structural distortion of the bimetallic lattice at the nanoparticle surfaces. Our study demonstrated a downshift of the d-band of the catalysts that adjusts the binding energies of the intermediate catalytic species. XPS analysis revealed that the binding energy for Ni 2p3/2 band of the Ni0.25Cu0.75/C nanoparticles was shifted ∼3 times compared to other bimetallic systems, and this was correlated to the high electrocatalytic activity observed. Interestingly, the bimetallic Ni0.25Cu0.75/C catalyst surpassed the OER performance of RuO2 benchmark catalyst exhibiting a small onset potential of 1.44 V vs RHE and an overpotential of 400 mV at 10 mA·cm-2 as well as the electrochemical long-term stability of commercial RuO2 and Pt catalysts and kept at least 90% of the initial current applied after 20 000 s for the OER/ORR/HER reactions. This study reveals significant insight about the structure-function relationship for non-noble bimetallic nanostructures with multifunctional electrocatalytic properties.

Enhanced NiO Dispersion on a High Surface Area Pillared Heterostructure Covered by Niobium Leads to Optimal Behaviour in the Oxidative Dehydrogenation of Ethane.

A Nb-containing siliceous porous clay heterostructure (PCH) with Nb contents from 0 to 30 wt %) was prepared from a bentonite and used as support in the preparation of supported NiO catalysts with NiO loading from 15 to 80 wt %. Supports and NiO-containing catalysts were characterised by several physicochemical techniques and tested in the oxidative dehydrogenation (ODH) of ethane. The characterisation studies on Nb-containing supports showed the presence of well-anchored Nb5+ species without the formation of Nb2 O5 crystals. High dispersion of nickel oxide with low crystallinity was observed for the Nb-containing PCH supports. In addition, when NiO is supported on these Nb-containing porous clays, it is more effective in the ODH of ethane (ethylene selectivity of ca. 90 %) than NiO supported on the corresponding Nb-free siliceous PCH or on Nb2 O5 (ethylene selectivities of ca. 30 and 60 %, respectively). Factors such as the NiO-Nb5+ interaction, the NiO particle size and the properties of surface Nin+ species were shown to determine the catalytic performance.

Structural Analysis and Conduction Mechanisms in Polycrystalline Zinc Hydroxide Nitrate.

The conduction and dielectric properties in zinc hydroxide nitrate (Z5HN) were studied in detail as a function of the temperature and relative humidity by impedance spectroscopy, and the structure was investigated by X-ray diffraction (XRD). Elemental analysis indicated a layered material containing carbonate anions [Zn5(OH)8(NO3)1.6(CO3)0.2·1.7H2O] due to the high capability of adsorption of Z5HN, which makes this material appropriate for applications in real conditions. The water content affected the interlayer distance, conductivity, and dielectric response of the layered material. An electrostatic repulsive interaction after reduction of the water content as a function of the temperature causes an increase of the interlayer distance and a decrease in the conductivity response and dielectric behavior. The highest conductivity, 10-7 Ω-1 cm-1, was obtained at a shorter interlayer distance for the sample heat-treated at 25 °C. The Z5HN synthesized was also characterized at different temperatures using thermogravimetric analysis and Fourier transform infrared and Raman spectroscopy. Multipeak analysis of the XRD patterns at various relative humidity levels showed the formation of a most hydrated phase and an increase of the interlayer distance related with the adsorption of water molecules. This layered material presented a conductivity of 10-5 Ω-1 cm-1 at high relative humidity (92%). The dipole-dipole interaction appeared to be the dominant mechanism for the dielectric behavior at the lowest temperatures and highest humidity due to the high water content in the Z5HN structure. Taking into account its crystallization water and high adsorption of water molecules in the interlayer region, a conduction pathway in the Z5HN structure was proposed, which provides the route for proton transport by hydrogen-bonding networks on the basis of a Grotthuss-type mechanism in facilitating the long-range proton hopping at 25 °C. The results for high relative humidity imply that a vehicular conduction mechanism also may contribute to the electrical response.

Surface Modification of a Nanoporous Carbon Photoanode upon Irradiation.

The photocorrosion of a nanoporous carbon photoanode, with low surface functionalization and high performance towards the photoelectrochemical oxidation of water using simulated solar light, was investigated. Two different light configurations were used to isolate the effect of the irradiation wavelength (UV and visible light) on the textural and chemical features of the carbon photoanode, and its long-term photocatalytic performance for the oxygen evolution reaction. A complete characterization of the carbon showed that the photocorrosion of carbon anodes of low functionalization follows a different pathway than highly functionalized carbons. The carbon matrix gets slightly oxidized, with the formation of carboxylic and carbonyl-like moieties in the surface of the carbon anode after light exposure. The oxidation of the carbon occurred due to the photogeneration of oxygen reactive species upon the decomposition of water during the irradiation of the photoanodes. Furthermore, the photoinduced surface reactions depend on the nature of the carbon anode and its ability to photogenerate reactive species in solution, rather than on the wavelength of the irradiation source. This surface modification is responsible for the decreased efficiency of the carbon photoanode throughout long illumination periods, due to the effect of the oxidation of the carbon matrix on the charge transfer. In this work, we have corroborated that, in the case of a low functionalization carbon material, the photocorrosion also occurs although it proceeds through a different pathway. The carbon anode gets gradually slightly oxidized due to the photogeneration of O-reactive species, being the incorporation of the O-groups responsible for the decreased performance of the anode upon long-term irradiation due to the effect of the oxidation of the carbon matrix on the electron transfer.

Preparation of a heterogeneous biocatalyst through Thermomyces lanuginosus lipase immobilization on pore-expanded SBA-15.

Heterogeneous biocatalysts were prepared by adsorbing T. lanuginosus lipase (TLL) onto uncalcined (SBAUC-TLL) and calcined (SBAC-TLL) SBA-15, using ammonium fluoride as a pore expander to facilitate TLL immobilization. At an enzyme load of 1 mg/g, high immobilization yields (>90 %) and recovered activities (>80 % for SBAUC-TLL and 70 % for SBAC-TLL) were achieved. When increasing the enzyme load to 5 mg/g, the immobilization yield of SBAUC-TLL was 80 %, and the recovered activity was 50 %, while SBAC-TLL had a yield of 100 % and a recovered activity of 36 %. Crosslinking with glutaraldehyde (GA) was conducted to improve stability (SBAUC-TLL-GA and SBAC-TLL-GA). Although SBAC-TLL-GA lost 25 % of initial activity after GA modifications, it exhibited the highest thermal (t1/2 = 5.7 h at 65 °C), when compared to SBAC-TLL (t1/2 = 12 min) and the soluble enzyme (t1/2 = 36 min), and operational stability (retained 100 % activity after 5 cycles). Both biocatalysts presented high storage stability since they retained 100 % of initial activity for 30 days. These results highlight SBA-15's potential as an enzyme support and the protocol's efficacy in enhancing stability, with implications for industrial applications in the food, chemical, and pharmaceutical sectors.

Highly Efficient Solar-Light-Driven Photodegradation of Metronidazole by Nickel Hexacyanoferrate Nanocubes Showing Enhanced Catalytic Performances.

Environmental pollution is a complex problem that threatens the health and life of animal and plant ecosystems on the planet. In this respect, the scientific community faces increasingly challenging tasks in designing novel materials with beneficial properties to address this issue. This study describes a simple yet effective synthetic protocol to obtain nickel hexacyanoferrate (Ni-HCF) nanocubes as a suitable photocatalyst, which can enable an efficient photodegradation of hazardous anthropogenic organic contaminants in water, such as antibiotics. Ni-HCF nanocubes are fully characterized and their optical and electrochemical properties are investigated. Preliminary tests are also carried out to photocatalytically remove metronidazole (MDZ), an antibiotic that is difficult to degrade and has become a common contaminant as it is widely used to treat infections caused by anaerobic microorganisms. Under simulated solar light, Ni-HCF displays substantial photocatalytic activity, degrading 94.3% of MDZ in 6 h. The remarkable performance of Ni-HCF nanocubes is attributeto a higher ability to separate charge carriers and to a lower resistance toward charge transfer, as confirmed by the electrochemical characterization. These achievements highlight the possibility of combining the performance of earth-abundant catalysts with a renewable energy source for environmental remediation, thus meeting the requirements for sustainable development.

Metal-doped niobate pyrochlores and double-perovskites for glycerol valorization: structural and electronic properties and DFT calculations.

In this study, metal-doped niobates and perovskites were obtained by a solid-state reaction. The solids were evaluated in the esterification of glycerol in the presence of acetic acid to produce valuable esters of glycerol. The structural features of the solids indicated the ZnNb2O6, Pb2.8Nb2O7.8 and CuNb2O6 columbite main phases and La2MnFeO6 double-perovskite. Density functional theory (DFT) studies of Pb2.8Nb2O7.8 clearly confirmed the existence of a robust orthorhombic structure and its electronic properties were correlated with the Nb and Pb interactions. The morphological and elemental analyses also indicated that not all surface elements, as well as morphology, were crucial for catalytic properties. All solids were active and selective toward triacetin formation upon glycerol esterification with acetic acid. The catalytic performance depends mainly on the availability of the surface and its structural stability, as well as defects formation. Recyclability studies indicated that the La2MnFeO6 double-perovskite was an efficient catalyst, achieving glycerol conversion of 68% and triacetin selectivity of 25% up to 4 cycles of use in the reaction. The structural defects near the Mn4+/Mn3+ surface sites resulted in the diffusion of anions and an increased concentration of oxygen vacancies contributed to the stable performance of the solid in glycerol ester production.

Composite MAX phase/MXene/Ni electrodes with a porous 3D structure for hydrogen evolution and energy storage application.

MXenes, a family of two-dimensional (2D) transition metal carbides, have been discovered as exciting candidates for various energy storage and conversion applications, including green hydrogen production by water splitting. Today, these materials mostly remain interesting objects for in-depth fundamental studies and scientific curiosity due to issues related to their preparation and environmental stability, limiting potential industrial applications. This work proposes a simple and inexpensive concept of composite electrodes composed of molybdenum- and titanium-containing MAX phases and MXene as functional materials. The concept is based on the modification of the initial MAX phase by the addition of metallic Ni, tuning Al- and carbon content and synthesis conditions, followed by fluoride-free etching under alkaline conditions. The proposed methodology allows producing a composite electrode with a well-developed 3D porous MAX phase-based structure acting as a support for electrocatalytic species, including MXene, and possessing good mechanical integrity. Electrochemical tests have shown a high electrochemical activity of such electrodes towards the hydrogen evolution reaction (HER), combined with a relatively high areal capacitance (up to 10 F cm-2).

Zeolites synthesis from phyllosilicates and their performance for CO2 adsorption.

Five phyllosilicates (kaolinite, montmorillonite, saponite, sepiolite and palygorskite) have been selected as starting materials for the synthesis of zeolites. Among them, kaolinite and montmorillonite display the lowest Si/Al molar ratio leading to aluminosilicates with high crystallinity. Thus, the hydrothermal treatment under basic conditions forms 4A zeolite when kaolinite is used as starting material while 13X zeolite is obtained when montmorillonite is used as starting material. The microporosity and CO2-adsorption capacity of the prepared zeolites are directly related to its crystallinity. Thus, in order to improve it, raw phyllosilicates were subjected to a microwave-assisted treatment to remove undesired Mg or Fe-species, which have a negative effect in the assembling of the zeolites by hydrothermal basic conditions in a second step. The highest adsorption value was 3.85 mmol/g at 25 °C and 760 mm of Hg for Mont-A-B sample after the consecutive treatments.

Effects on structure by spectroscopic investigations, valence state and morphology properties of FeCo-containing SnO2 catalysts for glycerol valorization to cyclic acetals.

The effects on the structure, valence state and morphological properties of FeCo-containing SnO2 nanostructured solids were investigated. The physicochemical features were tuned by distinct synthesis routes e.g., sol-gel, coprecipitation and nanocasting, to apply them as catalysts in the glycerol valorization to cyclic acetals. Based on Mössbauer and XPS spectroscopy results, all nanosized FeCoSn solids have Fe-based phases, which contain Co and Sn included in the structure, and well-dispersed Fe3+ and Fe2+ surface active sites. Raman, FTIR and EPR spectroscopies measurements of the spent solids demonstrated structural stability for the sol-gel based solid, which is indeed responsible for the highest catalytic performance, among the nanocasted and coprecipitated counterparts. Morphological and elemental analyses illustrated distinct morphologies and composition on solid surface, depending on the synthesis route. The Fe/Co and Fe/Sn surface ratios are closely related to the catalytic performance. The improved glycerol conversion and selectivities of the solid obtained by sol-gel method was ascribed to the leaching resistance and the Sn action as a structural promoter.

Fe3O4@UiO-66-NH2 based on magnetic solid phase extraction for determination of organic UV filters in environmental water samples.

In this work, a nanocomposite structured magnetic metal-organic framework named as Fe3O4@UiO-66-NH2 was prepared via a simple hydrothermal approach. The as-mentioned nanocomposite was characterized by Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction analysis (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and the Brunauer-Emmett-Teller (BET) techniques. Using the Fe3O4@UiO-66-NH2 as a nanosorbent, an easy and highly effective approach was developed to preconcentrate nine organic UV filters before gas chromatography-mass spectrometry (GC-MS) analysis. Different conditions influencing the extraction efficiency encompassing the sorbent amount, nature and volume of desorption solvent, desorption time, pH of the sample, and extraction time, were examined. Under the optimal experimental parameters, the Fe3O4@UiO-66-NH2-based magnetic solid phase extraction and GC-MS (MSPE-GC-MS) demonstrated linearity in the range of 0.03-1500 ng/L (R2 ≥ 0.9974) and the reproducibility, expressed as RSD, was ≤7.5%. The limits of detection ranged between 0.01 and 0.07 ng/L and limits of quantification were in the range of 0.03-0.4 ng/L. Finally, the suggested approach was satisfactorily utilized to determine nine organic UV filters in different water samples (analytical recoveries between 86.5% and 104.2%).

Magnetic mining waste based-geopolymers applied to catalytic reactions with ozone.

The demand for sustainable and low-cost materials for wastewater treatment is increasing considerably. In this scenario, geopolymers have gained great interest, due to their good mechanical properties, their ability to be produced from industrial waste and their adsorbent or catalytic properties. In this study, novel magnetic mining waste based-geopolymers were produced by incorporating a residue from phosphate waste rocks, which were extensively characterized (XRD, TGA/DTA, SEM, BET, XRF, FTIR, Mössbauer, ss-NMR and XPS). The materials produced showed formation of a dense framework, even with 75% incorporation of the residue. The iron oxides and their magnetic properties remained unchanged, and their application in advanced oxidation reactions were evaluated, in particular, as catalysts in ozonation reactions. All of the geopolymers presented catalytic activity in the ozonation reaction, with catalytic ozone decomposition values of up to 2.98 min-1, which is 99 times greater than non-catalyzed reactions. Moreover, the reuse (performed in three cycles) and hot filtration-like experiments demonstrated, respectively, the regenerability and heterogeneous catalytic properties of the produced materials, showcasing the potential of these waste materials for catalytic geopolymer production. demonstrating the potential of this waste to produce catalytic geopolymers.

Catalytic dehydration of glycerol over Cu-Fe-Al-based oxides: understanding changes in active sites throughout the reaction.

The glycerol conversion into acetol using Fe, Al and Cu-based oxides was investigated. XRD results indicate the formation of nanosized particles with high phase dispersion, however, Raman, Mössbauer, 27Al NMR and XPS spectroscopies suggest the presence of iron(iii) oxide, Al2O3 and CuO phases. The FTIR with pyridine adsorption revealed high Lewis acidity. The TPR profile showed the reduction temperature range for the Fe3+ and Cu2+ sites, indicating the suitable condition for pretreatment. The N2 adsorption-desorption isotherms indicated the presence of micro-mesopores with interesting textural properties and specific area varying between 71 and 220 m2 g-1, while the porous morphology was observed by SEM and TEM images. The optimized catalytic tests showed glycerol conversion of 60% and acetol selectivity of 92% with 17% of coke according to TG profile. The recycling tests confirmed the efficiency of the solid, reaching 28% conversion and 91% acetol selectivity after four reuses and, after reactivation in an oxidizing atmosphere, the catalytic performance obtained results close to the second reuse. The interaction between the different Lewis acid sites involved in the mechanisms for the acetol and coke formation on the catalyst surface is discussed. The charge distribution represented by colors which indicates the acid-base surface was evaluated by a simple theoretical-computational study based on the DFT approach. The synergy between the active sites indicates that the presence of Cu0/Cu+ drastically increases the acetol selectivity which is a more important characteristic than the high Lewis acidity of Fen+ and Al3+.

Linear Polyethyleneimine-Based and Metal Organic Frameworks (DUT-67) Composite Hydrogels as Efficient Sorbents for the Removal of Methyl Orange, Copper Ions, and Penicillin V.

This research explores the integration of DUT-67 metal organic frameworks into polyethyleneimine-based hydrogels to assemble a composite system with enough mechanical strength, pore structure and chemical affinity to work as a sorbent for water remediation. By varying the solvent-to-modulator ratio in a water-based synthesis path, the particle size of DUT-67 was successfully modulated from 1 µm to 200 nm. Once DUT-67 particles were integrated into the polymeric hydrogel, the composite hydrogel exhibited enhanced mechanical properties after the incorporation of the MOF filler. XPS, NMR, TGA, FTIR, and FT Raman studies confirmed the presence and interaction of the DUT-67 particles with the polymeric chains within the hydrogel network. Adsorption studies of methyl orange, copper(II) ions, and penicillin V on the composite hydrogel revealed a rapid adsorption kinetics and monolayer adsorption according to the Langmuir's model. The composite hydrogel demonstrated higher adsorption capacities, as compared to the pristine hydrogel, showcasing a synergistic effect, with maximum adsorption capacities of 473 ± 21 mg L-1, 86 ± 6 mg L-1, and 127 ± 4 mg L-1, for methyl orange, copper(II) ions, and penicillin V, respectively. This study highlights the potential of MOF-based composite hydrogels as efficient adsorbents for environmental pollutants and pharmaceuticals.