Qingrui Zhang

Unique Lead Adsorption Behavior of Activated Hydroxyl Group in Two-Dimensional Titanium Carbide

The functional groups and site interactions on the surfaces of two-dimensional (2D) layered titanium carbide can be tailored to attain some extraordinary physical properties. Herein a 2D alk-MXene (Ti3C2(OH/ONa)(x)F(2-x)) material, prepared by chemical exfoliation followed by alkalization intercalation, exhibits preferential Pb(II) sorption behavior when competing cations (Ca(II)/Mg(II)) coexisted at high levels. Kinetic tests show that the sorption equilibrium is achieved in as short a time as 120 s. Attractively, the alk-MXene presents efficient Pb(II) uptake performance with the applied sorption capacities of 4500 kg water per alk-MXene, and the effluent Pb(II) contents are below the drinking water standard recommended by the World Health Organization (10 μg/L). Experimental and computational studies suggest that the sorption behavior is related to the hydroxyl groups in activated Ti sites, where Pb(II) ion exchange is facilitated by the formation of a hexagonal potential trap.

Preparation of Graphene Oxide-Based Hydrogels as Efficient Dye Adsorbents for Wastewater Treatment

Graphene oxide (GO) sheets exhibit superior adsorption capacity for removing organic dye pollutants from an aqueous environment. In this paper, the facile preparation of GO/polyethylenimine (PEI) hydrogels as efficient dye adsorbents has been reported. The GO/PEI hydrogels were achieved through both hydrogen bonding and electrostatic interactions between amine-rich PEI and GO sheets. For both methylene blue (MB) and rhodamine B (RhB), the as-prepared hydrogels exhibit removal rates within about 4 h in accordance with the pseudo-second-order model. The dye adsorption capacity of the hydrogel is mainly attributed to the GO sheets, whereas the PEI was incorporated to facilitate the gelation process of GO sheets. More importantly, the dye-adsorbed hydrogels can be conveniently separated from an aqueous environment, suggesting potential large-scale applications of the GO-based hydrogels for organic dye removal and wastewater treatment.

Sorption enhancement of lead ions from water by surface charged polystyrene-supported nano-zirconium oxide composites.

A novel hybrid nanomaterial was fabricated by encapsulating ZrO2 nanoparticles into spherical polystyrene beads (MPS) covalently bound with charged sulfonate groups (-SO3(-)). The resultant adsorbent, Zr-MPS, exhibited more preferential sorption toward Pb(II) than the simple equivalent mixture of MPS and ZrO2. Such observation might be ascribed to the presence of sulfonate groups of the polymeric host, which could enhance nano-ZrO2 dispersion and Pb(II) diffusion kinetics. To further elucidate the role of surface functional groups, we encapsulated nano-ZrO2 onto another two macroporous polystyrene with different surface groups (i.e., -N(CH3)3(+)/-CH2Cl, respectively) and a conventional activated carbon. The three obtained nanocomposites were denoted as Zr-MPN, Zr-MPC, and Zr-GAC. The presence of -SO3(-) and -N(CH3)3(+) was more favorable for nano-ZrO2 dispersion than the neutral -CH2Cl, resulting in the sequence of sorption capacities as Zr-MPS > Zr-MPN > Zr-GAC > Zr-MPC. Column Pb(II) sorption by the four nanocomposites further demonstrated the excellent Pb(II) retention by Zr-MPS. Comparatively, Zr-MPN of well-dispersed nano-ZrO2 and high sorption capacities showed much faster breakthrough for Pb(II) sequestration than Zr-MPS, because the electrostatic repulsion of surface quaternary ammonium group of MPN and Pb(II) ion would result in a poor sorption kinetics. This study suggests that charged groups in the host resins improve the dispersion of embedded nanoparticles and enhance the reactivity and capacity for sorption of metal ions. Suitably charged functional groups in the hosts are crucial in the fabrication of efficient nanocomposites for the decontamination of water from toxic metals and other charged pollutants.

Reduced Graphene Oxide-Based Silver Nanoparticle-Containing Composite Hydrogel as Highly Efficient Dye Catalysts for Wastewater Treatment

New reduced graphene oxide-based silver nanoparticle-containing composite hydrogels were successfully prepared in situ through the simultaneous reduction of GO and noble metal precursors within the GO gel matrix. The as-formed hydrogels are composed of a network structure of cross-linked nanosheets. The reported method is based on the in situ co-reduction of GO and silver acetate within the hydrogel matrix to form RGO-based composite gel. The stabilization of silver nanoparticles was also achieved simultaneously within the gel composite system. The as-formed silver nanoparticles were found to be homogeneously and uniformly dispersed on the surface of the RGO nanosheets within the composite gel. More importantly, this RGO-based silver nanoparticle-containing composite hydrogel matrix acts as a potential catalyst for removing organic dye pollutants from an aqueous environment. Interestingly, the as-prepared catalytic composite matrix structure can be conveniently separated from an aqueous environment after the reaction, suggesting the potentially large-scale applications of the reduced graphene oxide-based nanoparticle-containing composite hydrogels for organic dye removal and wastewater treatment.

Hydrothermal synthesis of hierarchical core–shell manganese oxide nanocomposites as efficient dye adsorbents for wastewater treatment

In this work, hierarchical core-shell manganese oxide nanocomposites (Fe3O4@MnO2 and Fe2O3@MnO2) were synthesized via a facile hydrothermal process without using any templates or organic surfactants. The effect of reaction time on the microstructure and morphology of composite samples was systemically investigated. The formation mechanism of the core-shell structure was carefully analyzed by using field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Brunauer-Emmett-Teller (BET) surface area measurement. Both nitrogen adsorption-desorption experiments and morphological study showed that the composite obtained through 6 hour hydrothermal reaction has fairly large specific surface area, uniform pore-size distribution, and good adsorption capability. The dye adsorption experiments further demonstrated the potential applications of the manganese oxide nanocomposites as efficient dye adsorbents for wastewater treatment.

Facile and Scalable Preparation of Graphene Oxide-Based Magnetic Hybrids for Fast and Highly Efficient Removal of Organic Dyes

This study reports the facile preparation and the dye removal efficiency of nanohybrids composed of graphene oxide (GO) and Fe3O4 nanoparticles with various geometrical structures. In comparison to previously reported GO/Fe3O4 composites prepared through the one-pot, in situ deposition of Fe3O4 nanoparticles, the GO/Fe3O4 nanohybrids reported here were obtained by taking advantage of the physical affinities between sulfonated GO and Fe3O4 nanoparticles, which allows tuning the dimensions and geometries of Fe3O4 nanoparticles in order to decrease their contact area with GO, while still maintaining the magnetic properties of the nanohybrids for easy separation and adsorbent recycling. Both the as-prepared and regenerated nanohybrids demonstrate a nearly 100% removal rate for methylene blue and an impressively high removal rate for Rhodamine B. This study provides new insights into the facile and controllable industrial scale fabrication of safe and highly efficient GO-based adsorbents for dye or other organic pollutants in a wide range of environmental-related applications.

Synthesis of MXene/Ag Composites for Extraordinary Long Cycle Lifetime Lithium Storage at High Rates

A new MXene/Ag composite was synthesized by direct reduction of a AgNO3 aqueous solution in the presence of MXene (Ti3C2(OH)0.8F1.2). The as-received MXene/Ag composite can be deemed as an excellent anode material for lithium-ion batteries, exhibiting an extraordinary long cycle lifetime with a large capacity at high charge-discharge rates. The results show that Ag self-reduction in MXene solution is related to the existence of low-valence Ti. Reversible capacities of 310 mAh·g(-1) at 1 C (theoretical value being ∼320 mAh·g(-1)), 260 mAh·g(-1) at 10 C, and 150 mAh·g(-1) at 50 C were achieved. Remarkably, the composite withstands more than 5000 cycles without capacity decay at 1-50 C. The main reasons for the long cycle life with high capacity are relevant to the reduced interface resistance and the occurrence of Ti(II) to Ti(III) during the cycle process.

Self-assembly, interfacial nanostructure, and supramolecular chirality of the Langmuir-Blodgett films of some schiff base derivatives without alkyl chain

A special naphthyl-containing Schiff base derivative, N, N′-bis(2-hydroxy-1-naphthylidene)-1,2-phenylenediamine, was synthesized, and its coordination with various metal ions in situ at the air/water interface has been investigated. Although the ligand contains no alkyl chain, it can be spread on water surface. When metal ions existed in the subphase, an interfacial coordination between the ligand and different metal ions occurred in the spreading film, while different Nanostructures were fabricated in the monolayers. Interestingly to note that among various metal ions, only the in situ coordination-induced Cu(II)-complex film showed supramolecular chirality, although the multilayer films from the ligand or preformed complex are achiral. The chirality of the in situ Cu(II)-coordinated Langmuir film was developed due to the special distorted coordination reaction and the spatial limitation at the air/water interface. A possible organization mechanism at the air/water interface was suggested.

Self-assembly of organogels via new luminol imide derivatives: diverse nanostructures and substituent chain effect

Luminol is considered as an efficient sycpstem in electrochemiluminescence (ECL) measurements for the detection of hydrogen peroxide. In this paper, new luminol imide derivatives with different alkyl substituent chains were designed and synthesized. Their gelation behaviors in 26 solvents were tested as novel low molecular mass organic gelators. It was shown that the length and number of alkyl substituent chains linked to a benzene ring in gelators played a crucial role in the gelation behavior of all compounds in various organic solvents. Longer alkyl chains in molecular skeletons in present gelators are favorable for the gelation of organic solvents. Scanning electron microscope and atomic force microscope observations revealed that the gelator molecules self-assemble into different micro/nanoscale aggregates from a dot, flower, belt, rod, and lamella to wrinkle with change of solvents. Spectral studies indicated that there existed different H-bond formations and hydrophobic forces, depending on the alkyl substituent chains in molecular skeletons. The present work may give some insight to the design and characteristic of new versatile soft materials and potential ECL biosensors with special molecular structures.

Distinguished Cr(VI) capture with rapid and superior capability using polydopamine microsphere: Behavior and mechanism

Toxic heavy metal containing Cr(VI) species is a serious threat for ecological environment and human beings. In this work, a new mussel-inspired polydopamine microsphere (PDA-sphere) is prepared through in situ oxidative polymerization at air condition with controllable sizes. The adsorption of Cr(VI) ions onto PDA-sphere is highly pH dependent with the optimal pH ranging from 2.5 to 3.8. A rapid Cr(VI) removal can approach in 8min for equilibrium. More importantly, the prepared materials exhibit a remarkable sorption selectivity, coexisting SO42-, NO3- and Cl- ions at high levels; The applicability model further proves its effective performances with treated capacity of 42,000kg/kg sorbent, and the effluent can be reduced from 2000ppb to below 50ppb, which meets the drinking water criterions recommended by WHO. 1kg sorbent can also purify approximately 100t Cr(VI) contaminated wastewaters basing on the wastewater discharges of China. Such capacity for application ranks the top level for Cr(VI) removal. Additionally, the exhausted materials can be well regenerated by binary alkaline and salts mixtures. Such efficient adsorption can be ascribed to the well-dispersed morphology as well as the strong affinity between Cr(VI) and catechol or amine groups by XPS investigation. All the results suggest that polydopamine microspheres may be ideal materials for Cr(VI) treatment in waters.