[Selective Adsorption of Au(â ¢) by Activated Carbon Supported Polythioamides and Adsorption Mechanism].

By using in-situ synthesis of polythioamide (PTA) on activated carbon (AC), a polythioamide-modified activated carbon-based adsorbent (AC-PTA) was successfully prepared and used to study the selective adsorption effect and mechanism of Au(Ⅲ) in wastewater. The results showed that AC-PTA exhibited excellent selective adsorption to Au(Ⅲ) in the coexisting solution of multiple metal ions in a wide pH range (<5.0). The adsorption effect for Au(Ⅲ) was the best at a pH of 2 and 3; the concentration of residue Au(Ⅲ) was less than 0.1 mg·L-1, whereas other metals were barely adsorbed. The selective adsorption process for Au(Ⅲ) conformed to the pseudo-second kinetic model (R2=0.9853), the thermodynamic process conformed to the Langmuir isotherm process (R2=0.9936), and adsorption capacity was up to 2018 mg·g-1. Such advantages were mainly attributed to the coordination interaction between the -C([FY=,1]S)NH- functional groups on the AC-PTA surface and Au(Ⅲ), the electrostatic adsorption between the positive AC-PTA and negative Au(Ⅲ) complex anions, and the direct reduction of Au(Ⅲ) by AC. The successful recovery of gold was finally realized by burning the adsorbed AC-PTA at 1000℃ for 4 hours under air conditions, and solid gold with a mass fraction higher than 90.0% was obtained. This study provided the possibility for selective adsorption and recovery of low concentration Au(Ⅲ) from actual wastewater.

[Activating Efficiency of Iron-copper Bimetallic Organic Framework MIL-101(Fe,Cu) Toward H2 O2 for Degradation of Dyes].

Practical use of heterogeneous Fenton-like catalysis is inhibited by poor mass transfer and slow conversion of Fe(Ⅲ) to Fe(Ⅱ). In this study, we prepared a novel iron-copper bimetallic organic framework (MIL-101 (Fe,Cu)) using the solvothermal method, and carefully investigated its interfacial characters, catalytic efficacy toward dyes with methylene blue as a model pollutant, and the catalytic activating mechanisms involved in it. The MIL-101(Fe,Cu) exhibited a three-dimensional octahedral shape with a complete crystal structure. The specific BET surface area and average pore size were determined to be as high as 667.2 m2 ·g-1 and 1.9 nm, respectively. These characteristics benefits the exposure of the reactive sites and accelerates mass transfer accordingly. The MIL-101(Fe,Cu)/H2 O2 exhibited promising efficiency toward the degradation of methylene blue in a wide pH range; moreover, at a pH value of 5, the removal efficiency observed was as high as 100% after 20 min of reaction, which was 43.1% and 88.9% higher than that of MIL-101(Fe)/H2 O2 and H2 O2, respectively. Hydroxyl radical ( ·OH) is a dominant active species involved in the degradation of methylene blue using MIL-101(Fe,Cu)/H2 O2 as indicated in radicals quenching experiments. The results of species transformation in Fe and Cu indicated that Cu(Ⅱ) doping provided more active sites, and the Cu(Ⅱ)/Cu(Ⅰ) and Fe(Ⅲ)/Fe(Ⅱ) cycles synergistically facilitated ·OH generation to improve the Fenton-like catalytic efficiency accordingly. The MIL-101(Fe,Cu) as a novel heterogeneous Fenton-like catalyst achieved good performance without any significant pH adjustment and is practically viable for industrial wastewater treatment.

[Application of Fenton-like Photocatalysts Based on Defect Reconstruction in Degradation of Dye Wastewater].

In recent years, improving the performance of catalysts through defect modulation has attracted extensive attention. However, the impact of defect rearrangement on Fenton-like photocatalytic reactions has not been studied. In this study, Fe-containing polyoxometalate molecules were grafted onto the surface of defective TiO2.The influence of oxygen vacancy formation and the defect arrangement process on the catalytic activity was investigated. The results indicated that the calcination of cyanamide modified defective TiO2 is beneficial for the spatial reconstruction of oxygen vacancies generated by H2 atmosphere treatment. With rearranged structural defects, photo-generated electrons were prone to transfer from the surface of P25 to Fe-POM nanoparticles. Due to the enhanced charge separation in TiO2 and the increased reactive sites on the Fenton-like reagent, Fenton-like photocatalysts with rearranged defects showed a 13-fold increase in catalytic activity during the degradation of dye molecules.

[Simultaneous Photocatalytic Reduction of Cr(â ¥) and Oxidation of SSA by Carbon Nitride].

Carbon nitride is a novel nonmetal semiconductor photocatalyst, which has developed into an ideal environmental treatment material in recent years. Graphite carbon nitride(g-C3N4) was prepared through pyrolysis melamine, and the structure, morphology and optical properties of samples were characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM) and UV-Vis diffuse reflectance spectra(UV-Vis DRS). The potential application of g-C3N4 in the simultaneous photocatalysis reduction of Cr(Ⅵ) and oxidation of sulfosalicylic acid(SSA) was further explored. And the effects of different conditions such as catalyst dosage, pH and initial concentration ratio of Cr(Ⅵ) with SSA on the simultaneous photocatalysis were also investigated. The results showed that when the catalyst dosage was 0.5 g·L-1, pH=2, the initial concentration ratio of Cr (VI) and SSA was 1:4(10 mg·L-1:40 mg·L-1), optimal simultaneous photocatalysis efficiency was achieved, which was more than 3 times higher than that of the separated photoreduction or photooxidation reactions. Within 3 hours, the reduction ratio of Cr(Ⅵ) and oxidation ratio of SSA could reach 98.9% and 93.4%, respectively. The mechanism of simultaneous photocatalysis was discussed. Cr(Ⅵ) was reduced by electrons and SSA was oxidized by the combined function of hole, O2·- and·OH under visible light.

Direct observation of carbon nanostructure growth at liquid-solid interfaces.

Our TEM observation revealed that in a carbon-Pt3Co system, amorphous carbon first crystallized into nanoclusters at step-edges on melting Pt3Co surfaces before merging into graphene layers through a kinetic restructuring via oriented-attachment, leading to the final formation of few-layered graphene nanostructures. The result obtained from density-functional theory calculations further suggested that Co atoms rather than Pt atoms acted as initial nucleation centers.