Heterogeneous catalyst

Aspergillus oryzae β-D-Galactosidase (β-Gal) efficiently hydrolyzes sesaminol triglucoside into sesaminol, which has higher biological activity. However, β-Gal is difficult to be separate from the reaction mixture and limited by stability. To resolve these problems, β-Gal was immobilized on amino-functionalized magnetic nanoparticles mesoporous silica pre-activated with glutaraldehyde (Fe3 O4 @mSiO2 -β-Gal), which was used for the first time to prepare sesaminol. Under the optimal conditions, the immobilization yield and recovered activity of β-Gal were 57...

Copper-catalyzed azide-alkyne cycloaddition click (CuAAC) reaction is widely used to synthesize drug candidates and other biomolecule classes. Homogeneous catalysts, which consist of copper coordinated to a ligand framework, have been optimized for high yield and specificity of the CuAAC reaction, but CuAAC reaction with these catalysts requires the addition of a reducing agent and basic conditions, which can complicate some of the desired syntheses. Additionally, removing copper from the synthesized CuAAC-containing biomolecule is necessary for biological applications but inconvenient and requires additional purification steps...

The layered double hydroxides (LDHs) of transition metals are of great interest as building blocks for the creation of composite photocatalytic materials for hydrogen production, environmental remediation and other applications. However, the synthesis of most LDHs is reported only by the conventional coprecipitation method, which makes it difficult to control the catalyst's crystallinity. In the present study, ZnCr- and NiCr-LDHs have been successfully prepared using a facile hydrothermal approach. Varying the hydrothermal synthesis conditions allowed us to obtain target products with a controllable crystallite size in the range of 2-26 nm and a specific surface area of 45-83 m2 ∙g-1 ...

The qualitative impact of pollutants on water quality is mainly related to their nature and their concentration, but in any case, they determine a strong impact on the involved ecosystems. In particular, refractory organic compounds represent a critical challenge, and several degradation processes have been studied and developed for their removal. Among them, heterogeneous Fenton treatment is a promising technology for wastewater and liquid waste remediation. Here, we have developed mono- and bimetallic formulations based on Co, Cu, Fe, and Mn, which were investigated for the degradation of three model organic dyes (methylene blue, rhodamine B, and malachite green)...

Graphitic carbon nitride ( g -C3 N4 ), recognized for its considerable potential as a heterogeneous photocatalyst in water splitting, has attracted extensive research interest. By using density functional theory (DFT) calculations, the regulatory role of p -block metal (PM) single atoms on the photocatalytic activity of g -C3 N4 in overall water splitting was systematically explored. The incorporation of PM atoms (Ge, Sn and Pb) led to a reduction in the overpotentials required for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER)...

The transformation of carbon dioxide (CO2 ) into functional materials has garnered considerable worldwide interest. Metal-organic frameworks (MOFs), as a distinctive class of materials, have made great contributions to CO2 capture and conversion. However, facile conversion of CO2 to stable porous MOFs for CO2 utilization remains unexplored. Herein, we present a facile methodology of using CO2 to synthesize stable zirconium-based MOFs. Two zirconium-based MOFs CO2 -Zr-DEP and CO2 -Zr-DEDP with face-centered cubic topology were obtained via a sequential desilylation-carboxylation-coordination reaction...

Revealing the spatiotemporal evolution characteristics and key driving processes behind the habitat quality is of great significance for the scientific management of production, living, and ecological spaces in resource-based cities, as well as for the efficient allocation of resources. Focusing on the largest coal-mining subsidence area in Jiangsu Province of China, this study examines the spatiotemporal evolution of land use intensity, morphology, and functionality across different time periods. It evaluates the habitat quality characteristics of the Pan'an Lake area by utilizing the InVEST model, spatial autocorrelation, and hotspot analysis techniques...

Multimetallic synergistic effects have the potential to improve CO2 cycloesterification and Knoevenagel reaction processes, outperforming monometallic MOFs. The results demonstrate superior performance in these processes. To investigate this, we created and characterized a selection of single-component Ln(III)-MOFs (Ln = Eu, Tb, Gd, Dy, Ho) and high-entropy lanthanide-organic framework (HE-LnMOF) using solvent-thermal conditions. The experiments revealed that HE-LnMOF exhibited heightened catalytic efficiency in CO2 cycloesterification and Knoevenagel reactions compared to single-component Ln(III) MOFs...

Here, we present the results of the synthesis, surface modification, and properties analysis of magnetite-based nanoparticles, specifically Co0.047 Fe2.953 O4 (S1) and Co0.086 Fe2.914 O4 (S2). These nanoparticles were synthesized using the co-precipitation method at 80 °C for 2 h. They exhibit a single-phase nature and crystallize in a spinel-type structure (space group Fd 3¯ m ). Transmission electron microscopy analysis reveals that the particles are quasi-spherical in shape and approximately 11 nm in size...

A mixed metal oxide W-TiO2 nanopowder photocatalyst was prepared by using the sol-gel method with a broad range of elemental compositions x = CW /(CW + CTi ), including TiO2 and WO3 . The material was structurally characterized and evaluated in adsorption and photocatalytic processes by testing its removal capacity of a representative pollutant methylene blue (MB) in aqueous solutions and under UV-A and sunlight illuminations. The nanopowders appeared to be more effective adsorbents than pure TiO2 and WO3 materials, showing a maximum at 15 mol% W, which was set as the tungsten solubility limit in anatase titania...

The composites of heteropolyacids (H3 PW12 , H3 PMo12 ) incorporated into amine-functionalized silica materials were used for the first time as heterogeneous catalysts in the valorization of glycerol (a major waste from the biodiesel industry) through acetalization reaction with acetone. The polyoxotungstate catalyst H3 PW12 @ Aptes SBA-15 exhibited higher catalytic efficiency than the phosphomolybdate, achieving 97% conversion and 97% of solketal selectivity, after 60 min at 25 °C, or 91% glycerol conversion and the same selectivity, after 5 min, performing the reaction at 60 °C...

Benzene, a high-volume chemical, is produced from larger molecules by inefficient and environmentally harmful processes. Recent changes in hydrocarbon feedstocks from oil to gas motivate research into small molecule upgrading. For example, the cyclotrimerization of acetylene reaction has been demonstrated on Pd, Pd alloy, and Cu surfaces and catalysts, but they are not 100% selective to benzene. We discovered that acetylene can be converted to benzene with 100% selectivity on the Ag(111) surface. Our temperature programmed desorption experiments reveal a threshold acetylene surface coverage of ∼one monolayer, above which benzene is formed...

An industrially viable catalyst for heterogeneous catalytic ozonation (HCO) in water purification requires the characteristics of good dispersion of active species on its surface, efficient electron transfer for ozone decay, and maximum active species utilization. While metal-organic frameworks (MOFs) represent an attractive platform for HCO, the metal nodes in the unmodified MOFs exhibit low catalytic activity. Herein, we present a perfluorinated Fe-MOF catalyst by substituting H atoms on the metalated ligands with F atoms (termed 4F-MIL-88B) to induce structure evolution...

A two-step treatment  of mahua oil was conducted to synthesize mahua biodiesel using heterogeneous biomass-based catalyst derived from mahua shell. Mahua oil having higher free fatty acid (FFA) content (about 19%) was esterified to reduce the FFA content up to 1%. The esterification process was carried out using 200 mL mahua oil, 5:1 molar ratio (methanol:oil), and 2.25 weight% of H2 SO4 at a temperature of 60 °C for 3 h. Post esterification, a set of 16 experiments were created using a Box-Behnken design (BBD)-based response surface methodology (RSM) approach to conduct the transesterification of the esterified oil...

Photo(electro)catalysts use sunlight to drive chemical reactions such as water splitting. A major factor limiting photocatalyst development is physicochemical heterogeneity which leads to spatially dependent reactivity. To link structure and function in such systems, simultaneous probing of the electrochemical environment at microscopic length scales and a broad range of timescales (ns to s) is required. Here, we address this challenge by developing and applying in-situ (optical) microscopies to map and correlate local electrochemical activity, with hole lifetimes, oxygen vacancy concentrations and photoelectrode crystal structure...

Creating affordable electrocatalysts and understanding the real-time catalytic process of the urea oxidation reaction (UOR) are crucial for advancing urea-based technologies. Herein, a Cu-Ni based selenide electrocatalyst (CuSe y /NiSe x /NF) was created using a hydrothermal technique and selenization treatment, featuring a heterogeneous interface rich in Cu2- x Se, Cu3 Se2 , Ni3 Se4 , and NiSe2 . This catalyst demonstrated outstanding urea electrooxidation performance, achieving 10 mA cm-2 with just 1.31 V and sustaining stability for 96 h...

The electro-Fenton with in situ generated 1 O2 and • OH is a promising method for the degradation of micropollutants. However, its application is hindered by the lack of catalysts that can efficiently generate 1 O2 and • OH from electrochemical oxygen reduction. Herein, N-doped stacked carbon nanosheets supported Fe single atoms (Fe-NSC) with FeN4 sites were designed for simultaneous generation of 1 O2 and • OH to enhance electro-Fenton degradation. Due to the synergistic effect of 1 O2 and • OH, a variety of contaminants (phenol, 2,4-dichlorophenol, sulfamethoxazole, atrazine and bisphenol A) were efficiently degraded with high kinetic constants of 0...

Wolframite (FeWO4 ), a typical polyoxometalate, serves as an auspicious candidate for heterogeneous catalysts, courtesy of its high chemical stability and electronic properties. However, the electron-deficient surface-active Fe species in FeWO4 are insufficient to cleave H2 O2 via Fe redox-mediated Fenton-like catalytic reaction. Herein, we doped Sulfur (S) atom into FeWO4 catalysts to refine the electronic structure of FeWO4 for H2 O2 activation and sulfamethoxazole (SMX) degradation. Furthermore, spin-state reconstruction on S-doped FeWO4 was found to effectively refine the electronic structure of Fe in the d orbital, thereby enhancing H2 O2 activation...

Natural manganese oxides could induce the intermolecular coupling reactions among small-molecule organics in aqueous environments, which is one of the fundamental processes contributing to natural humification. These processes could be simulated to design novel advanced oxidation technology for water purification. In this study, periodate (PI) was selected as the supplementary electron-acceptor for colloidal manganese oxides (Mn(IV)aq ) to remove phenolic contaminants from water. By introducing polyferric sulfate (PFS) into the Mn(IV)aq /PI system and exploiting the flocculation potential of Mn(IV)aq , a post-coagulation process was triggered to eliminate soluble manganese after oxidation...

Construction of robust heterogeneous catalysts with atomic precision is a long-sought pursuit in the catalysis field due to its fundamental significance in taming chemical transformations. Herein, we present the synthesis of a single-crystalline pyrazolate metal-organic framework (MOF) named PCN-300, bearing a lamellar structure with two distinct Cu centers and one-dimensional (1D) open channels when stacked. PCN-300 exhibits exceptional stability in aqueous solutions across a broad pH range from 1 to 14. In contrast, its monomeric counterpart assembled through hydrogen bonding displays limited stability, emphasizing the role of Cu-pyrazolate coordination bonds in framework robustness...