Repurposing of steel rolling sludge: Solvent-free preparation of α-Fe2O3 nanoparticles and its application for As(III/V)-containing wastewater treatment.

Steel rolling sludge (SRS) is the by-product of metallurgical industry with abundant iron content, which needs to be utilized for producing high value-added products. Herein, cost-effective and highly adsorbent α-Fe2O3 nanoparticles were prepared from SRS via a novel solvent-free method and applied to treat As(III/V)-containing wastewater. The structure of the prepared nanoparticles was observed to be spherical with a small crystal size (12.58 nm) and high specific surface area (145.03 m2/g). The nucleation mechanism of α-Fe2O3 nanoparticles and the effect of crystal water were investigated. More importantly, compared with the traditional methods of preparation cost and yield, this study was found to have excellent economic benefits. The adsorption results indicated that the adsorbent could effectively remove arsenic over a wide pH range, and the optimal performance of nano adsorbent for As(III) and As(V) removal was observed at pH 4.0-9.0 and 2.0-4.0, respectively. The adsorption process was consistent with pseudo-second-order kinetic and Langmuir isothermal model. The maximum adsorption capacity (qm) of adsorbent for As(III) and As(V) was 75.67 mg/g and 56.07 mg/g, respectively. Furthermore, α-Fe2O3 nanoparticles exhibited great stability, and qm remained at 64.43 mg/g and 42.39 mg/g after five cycles. Particularly, the As(III) was removed by forming inner-sphere complexes with the adsorbent, and it partially oxidized to As(V) during this process. In contrast, the As(V) was removed by electrostatic adsorption and reaction with -OH on the adsorbent surface. Overall, resource utilization of SRS and the treatment of As(III)/(V)-containing wastewater in this study are in line with the current developments in the environmental and waste-to-value research.

From solvent-free microspheres to bioactive gradient scaffolds.

A solvent-free microsphere sintering technique was developed to fabricate scaffolds with pore size gradient for tissue engineering applications. Poly(D,L-Lactide) microspheres were fabricated through an emulsification method where TiO2 nanoparticles were employed both as particulate emulsifier in the preparation procedure and as surface modification agent to improve bioactivity of the scaffolds. A fine-tunable pore size gradient was achieved with a pore volume of 30±2.6%. SEM, EDX, XRD and FTIR analyses all confirmed the formation of bone-like apatite at the 14th day of immersion in Simulated Body Fluid (SBF) implying the ability of our scaffolds to bond to living bone tissue. In vitro examination of the scaffolds showed progressive activity of the osteoblasts on the scaffold with evidence of increase in its mineral content. The bioactive scaffold developed in this study has the potential to be used as a suitable biomaterial for bone tissue engineering and hard tissue regeneration.

An Efficient Green Approach to Constructing Adenine Sulfate-Derived Multicolor Sulfur- and Nitrogen-Codoped Carbon Dots and Their Bioimaging Applications.

A cost-effective and environmentally friendly approach is proposed for producing N- and S-codoped multicolor-emission carbon dots (N- and S-codoped MCDs) at a mild reaction temperature (150 °C) and relatively short time (3 h). In this process, adenine sulfate acts as a novel precursor and doping agent, effectively reacting with other reagents such as citric acid, para-aminosalicylic acid, and ortho-phenylenediamine, even during solvent-free pyrolysis. The distinctive structures of reagents lead to the increased amount of graphitic nitrogen and sulfur doping in the N- and S-codoped MCDs. Notably, the obtained N- and S-codoped MCDs exhibit considerable fluorescence intensities, and their emission color can be adjusted from blue to yellow. The observed tunable photoluminescence can be attributed to variations in the surface state and the amount of N and S contents. Furthermore, due to the favorable optical properties, good water solubility and biocompatibility, and low cytotoxicity, these N- and S-codoped MCDs, especially green carbon dots, are successfully applied as fluorescent probes for bioimaging. The affordable and environmentally friendly synthesis method employed to create N- and S-codoped MCDs, combined with their remarkable optical properties, offers a promising avenue for their use in various fields, particularly in biomedical applications.

Solvent-Free Synthesis of Hollow Carbon Nanostructures for Efficient Sodium Storage.

The structural characteristics of hollow carbon nanostructures (HCNs) result in intriguing physicochemical properties and various applications, especially for electrochemical energy storage applications. However, the currently solvent-based template methods to prepare HCNs are still far from meeting the facile, environment-friendly, and scalable demand. Herein, we explored a general and facile solvent-free block copolymer self-assembly approach to prepare various hollow hard carbon nanostructures, including hollow carbon nanofibers, hollow carbon Janus nanotadpoles, hollow carbon spheres, etc. It was found that the obtained HCNs possess abundant active sites, fast pathways for electrons/ions transport, and superior electronic conducting connectivity, which are promising for efficient electrochemical energy storage. Typically, the resultant hollow carbon nanofibers with a thick-walled tube deliver a high reversible capacity (431 mAh g-1) and excellent rate performance (259 mAh g-1 at 800 mA g-1) for sodium ion storage. This intelligent solvent-free block copolymer self-assembly method would inspire the design of hollow hard carbon-based nanostructures for advanced applications in various energy conversion and storage.

Cyclodextrin Complexation of Fenofibrate by Co-Grinding Method and Monitoring the Process Using Complementary Analytical Tools.

Solvent-free preparation types for cyclodextrin complexation, such as co-grinding, are technologies desired by the industry. However, in-depth analytical evaluation of the process and detailed characterization of intermediate states of the complexes are still lacking in areas. In our work, we aimed to apply the co-grinding technology and characterize the process. Fenofibrate was used as a model drug and dimethyl-ß-cyclodextrin as a complexation excipient. The physical mixture of the two substances was ground for 60 min; meanwhile, samples were taken. A solvent product of the same composition was also prepared. The intermediate samples and the final products were characterized with instrumental analytical tools. The XRPD measurements showed a decrease in the crystallinity of the drug and the DSC results showed the appearance of a new crystal form. Correlation analysis of FTIR spectra suggests a three-step complexation process. In vitro dissolution studies were performed to compare the dissolution properties of the pure drug to the products. Using a solvent-free production method, we succeeded in producing a two-component system with superior solubility properties compared to both the active ingredient and the product prepared by the solvent method. The intermolecular description of complexation was achieved with a detailed analysis of FTIR spectra.

A Brief Review on Solvent-Free Synthesis of Zeolites.

The traditional hydrothermal method to prepare zeolite will inevitably use a large amount of water as a solvent, which will lead to higher autogenous pressure, low efficiency, and wastewater pollution. The solvent-free method can be used to synthesize various types of zeolites by mechanical mixing, grinding, and heating of solid raw materials, which exhibits the apparent advantages of high yield, low pollution, and high efficiency. This review mainly introduces the development process of solvent-free synthesis, preparation of hierarchical zeolite, morphology control, synthesis mechanism and applications of solvent-free methods. It can be believed that solvent-free methods will become a research focus and have enormous industrial application potential.

Highly efficient WO3-FeOx catalysts synthesized using a novel solvent-free method for NH3-SCR.

WO3-FeOx catalysts with various WO3 contents were synthesized through a facile solvent-free method, satisfying the selective catalytic reduction of NO (NH3-SCR). Strikingly, the optimum 30 %WO3-FeOx catalyst with the largest surface area exhibited the most outstanding catalytic activity, achieving the nearly 100 % NOx removal efficiency in a wide temperature window between 225-500 °C, which was better than that of Fe-W series catalysts reported in other studies. In addition, Raman and XPS results proved that the introduction of WO3 altered the electronic environment of Fe2O3, inducing the formation of Fe3O4 (Fe2+) and surface adsorbed oxygen. In situ DRIFTS demonstrated that the interaction between WO3 and Fe2O3 not only promoted the adsorption capacity of NH3 on the catalyst, but also contributed to the formation of adsorbed NOx species. NOx reduction reaction on WO3-FeOx catalyst proceeded via the Eley-Rideal and Langmuir-Hinshelwood mechanism synchronously. All of these factors, jointly, accounted for the superior catalytic activity and N2 selectivity of WO3-FeOx catalysts.

Hydrophobic ion pairing (HIP) of (poly)peptide drugs: Benefits and drawbacks of different preparation methods.

In order to incorporate hydrophilic macromolecular drugs into lipid-based formulations (LBF), HIP has shown great potential. In this study, different HIP methods were compared with each other. Hydrophobic complexes were formed between bovine serum albumin (BSA) and either dodecyl sulfate, cetyl trimethylammonium or 1,2-dipalmitoyl-sn-glycero-3-phosphate applying the organic solvent-free method, Bligh-Dyer method and biphasic metathesis reaction either with ethyl acetate or chloroform as organic phase. Complex formation efficiency was determined. Hydrophobicity of the obtained complexes was characterized by their apparent partition coefficient between 1-butanol and water. The highest complex formation efficiency was achieved with the Bligh-Dyer method, followed by the organic solvent-free method and the biphasic metathesis reaction. When applying the organic solvent-free method, complex formation efficiency was hampered at higher surfactant concentrations due to the formation of micelles. Furthermore, this method could only be applied for water-soluble compounds. On the contrary, the Bligh-Dyer method was robust towards high surfactant concentrations. Moreover, it enables the use of water-insoluble compounds. The rank order Bligh-Dyer method > organic solvent-free method > biphasic metathesis reaction was confirmed by the log D. According to these results, the Bligh-Dyer method appears advantageous for HIP. However, the organic-solvent free method is an adequate alternative for water-soluble compounds.