Weiqing Han

Biodegradation of 2,4,6-trinitrophenol by Rhodococcus sp. isolated from a picric acid-contaminated soil.

A picric acid-degrading bacterium, strain NJUST16, was isolated from a soil contaminated by picric acid and identified as a member of Rhodococcus sp. based on 16S rRNA sequence. The degradation assays suggested that the strain NJUST16 could utilize picric acid as the sole source of carbon, nitrogen and energy. The isolate grew optimally at 30 degrees C and initial pH 7.0-7.5 in the mineral salts medium supplemented with picric acid. It was basically consistent with degradation of picric acid by the isolate. Addition of nitrogen sources such as yeast extract and peptone accelerated the degradation of picric acid. However, the stimulation was concentration dependent. The degradation was accompanied by release of stoichiometric amount of nitrite and acidification. The degradation of picric acid at relatively high concentrations (>3.93 mM) demonstrated that the degradation was both pH and nitrite dependent. Neutral and slightly basic pH was crucial to achieve high concentrations of picric acid degradation by the NJUST16 strain.

Synthesis of nanoscale zero-valent iron/ordered mesoporous carbon for adsorption and synergistic reduction of nitrobenzene.

Nanoscale zero-valent iron (NZVI) supported on ordered mesoporous carbon (OMC) was synthesized through liquid phase reduction route. The NZVI/OMC composite was characterized by X-ray diffraction, N(2) adsorption/desorption and transmission electron microscopy. Results reveal that the composite possesses ordered mesostructure with NZVI distributing homogeneously on the surface of OMC support. The removal effects of nitrobenzene (NB) in water with OMC, NZVI/OMC and non-supported NZVI were evaluated. Results indicate that NZVI/OMC shows enhanced removal efficiency, which is attributed to its adsorption and synergistic reduction for NB. The transformation process of NB was further investigated by HPLC. Nitrosobenzene and phenylhydroxylamine were detected as intermediate products and aniline was the final reductive product.

Biodegradation of 2,4,6-trinitrophenol (picric acid) in a biological aerated filter (BAF).

This study demonstrated the microbial purification of a model wastewater containing 2,4,6-trinitrophenol (TNP), which was carried out in a continuously working biological aerated filter (BAF). The main emphasis was on the operating performance of the reactor as a function of the pollution load. TNP was degraded at a maximum volumetric removal rate of 2.53gTNP/Ld, with low residual COD and TNP concentration. Overloading of TNP inhibited the nitrite-oxidizing activity, resulting in poor TNP degradation performance in the BAF system. The inhibition depended on some factors, such as influent concentrations and flow rates of the influent. It is assumed that nitrite-oxidizing occurred spontaneously during TNP degradation in the BAF system, could have significant influence on TNP wastewater treatment. One year after the reactor start-up, the dominance of Rhodococcus, which was initially inoculated in the reactor, was confirmed by analysis of 16S rDNA sequence of the PCR products separated by DGGE.

Controllable Synthesis of Functional Hollow Carbon Nanostructures with Dopamine As Precursor for Supercapacitors

N-doped hollow carbon spheres (N-HCSs) are promising candidates as electrode material for supercapacitor application. In this work, we report a facile one-step synthesis of discrete and highly dispersible N-HCSs with dopamine (DA) as a carbon precursor and TEOS as a structure-assistant agent in a mixture containing water, ethanol, and ammonia. The architectures of resultant N-HCSs, including yolk-shell hollow carbon spheres (YS-HCSs), single-shell hollow carbon spheres (SS-HCSs), and double-shells hollow carbon spheres (DS-HCSs), can be efficiently controlled through the adjustment of the amount of ammonia. To explain the relation and formation mechanism of these hollow carbon structures, the samples during the different synthetic steps, including polymer/silica spheres, carbon/silica spheres and silica spheres by combustion in air, were characterized by TEM. Electrochemical measurements performed on YS-HCSs, SS-HCSs, and DS-HCSs showed high capacitance with 215, 280, and 381 F g(-1), respectively. Moreover, all the nitrogen-doped hollow carbon nanospheres showed a good cycling stability 97.0% capacitive retention after 3000 cycles. Notably, the highest capacitance of DS-HCSs up to 381 F g(-1) is higher than the capacitance reported so far for many carbon-based materials, which may be attributed to the high surface area, hollow structure, nitrogen functionalization, and double-shell architecture. These kinds of N-doped hollow-structured carbon spheres may show promising prospects as advanced energy storage materials and catalyst supports.

Biological denitrification of high-nitrate wastewater in a modified anoxic/oxic-membrane bioreactor (A/O-MBR)

A modified anoxic/oxic-membrane bioreactor has been applied to the denitrification of a high strength nitrate waste (about 3600 mg/L nitrate-N) generated from an initiating explosive factory. Nitrate removal efficiency and nitrite accumulation in the treated water were investigated under various conditions set by several factors including the type of carbon source used, ratios of carbon to nitrogen, pH and hydraulic retention times (HRTs). The results of the preliminary experiments, which were carried out in parallel CSTR systems, demonstrated that sodium acetate had shown the best performance as the external carbon source. The optimal reaction parameters in the anoxic/oxic-membrane bioreactor were pH 7.5-8.5, C/N 1.56 and HRT 30 h, with over 99.9% of nitrate removed and without accumulation of nitrite. Explicitly high average-specific denitrification rate of 324 mg NO(3)(-)-N/g VSS/h could be attained under these conditions. The aerobic process and membrane module used subsequently could remove the residual COD, excessive biomass and soluble microbial products generated during the denitrification process.

Electrochemical degradation of nitrobenzene by anodic oxidation on the constructed TiO2-NTs/SnO2-Sb/PbO2 electrode

The interlayer of Sb-doped SnO2 (SnO2-Sb) and TiO2 nanotubes (TiO2-NTs) on Ti has been introduced into the PbO2 electrode system with the aim to reveal the mechanism of enhanced electrochemical performance of TiO2-NTs/SnO2-Sb/PbO2 electrode. In contrast with the traditional Ti/SnO2-Sb/PbO2 electrode, the constructed PbO2 electrode has a more regular and compact morphology with better oriented crystals of lower size. The TiO2-NTs/SnO2-Sb interlayer prepared by electrodeposition process improves PbO2 coating structure effectively, and enhances the electrochemical performance of PbO2 electrode. Kinetic analyses indicated that the electrochemical oxidation of nitrobenzene on the PbO2 electrodes followed pseudo-first-order reaction, and mass transport was enhanced at the constructed electrode. The accumulation of nitrocompounds of degradation intermediates on constructed electrode was lower, and almost all of the nitro groups were eliminated from aromatic rings after 6h of electrolysis. Higher combustion efficiency was obtained on the constructed TiO2-NTs/SnO2-Sb/PbO2 electrode. The intermediates of nitrobenzene oxidation were confirmed by IC and GC/MS.

Electrochemical degradation of pyridine by Ti/SnO2-Sb tubular porous electrode.

Diffusion in electrochemistry is a critical issue for water purification. Electrocatalytic reactor system in improving water quality is a useful way to induce convection to enhance diffusion. This study focuses on the preparation and the characterization of Ti/SnO2-Sb tubular porous electrode for degrading pyridine wastewater. The electrode as an anode in reactor system is prepared by coating SnO2-Sb as an electro-catalyst via Pechini method on the tubular porous Ti. Scanning Electron Microscopy, Energy Dispersive Spectrum, X-ray Diffraction and Pore Distribution are employed to evaluate the structure and morphology of the electrodes coatings, and Linear Sweep Voltammetry and Cyclic Voltammetry are used to illustrate the electrochemical properties of the electrodes coatings. Furthermore, the electrochemical oxidation performance of Ti/SnO2-Sb tubular porous electrode is characterized by degrading pyridine wastewater. The effects of flow and static pattern, initial pyridine concentration, supporting electrolyte concentration, current density and pH on the performance of the reactor were investigated in the electrocatalytic reactor system. The results indicated that the removal ratio of pyridine reaches maximum which is 98% under the optimal operation conditions, that are 100 mg L(-1) initial pyridine concentration, 10 g L(-1) supporting electrolyte concentration, 30 mA cm(-2) current density and pH 3. Transition state calculation based on the density function theory was combined with High Performance Liquid Chromatography, Gas Chromatography and Ionic Chromatography results to describe the pathway of pyridine degradation.

Bioelectrochemical system for recalcitrant p-nitrophenol removal

Bioelectrochemical system (BES) for recalcitrant p-nitrophenol (PNP) removal was investigated in this study. Effective removal of PNP at rates up to 9.14 ± 0.48 mol m(-3)d(-1) was achieved at an energy consumption as low as 0.010 ± 0.002 kWh mol(-1) PNP. PNP removal rate was enhanced with negative cathode potential, increased influent PNP concentration and shortened hydraulic retention time (HRT). Although the coulombic efficiencies at the anode did not exceed 40%, coulombic efficiencies for PNP removal at the cathode were above 70% at various cathode potentials. Compared with conventional anaerobic process, the cosubstrate dosage in BES was significantly reduced due to the high coulombic efficiencies at the cathode. p-Aminophenol (PAP) was identified as the dominant product of PNP reduction at the abiotic graphite cathode of BESs. This study demonstrated that the BES had a potential for efficient removal of nitrophenol pollutants from wastewater.

Comprehensive comparison of bacterial communities in a membrane-free bioelectrochemical system for removing different mononitrophenols from wastewater.

Membrane-free bioelectrochemical systems (MFBESs) have been developed for the degradation of nitro-aromatic contaminants, but the microbial communities that are involved have not been comprehensively investigated. In this study, the microbial communities were evaluated and compared for treating different structures of nitrophenols (NPs), i.e., o-nitrophenol (ONP), m-nitrophenol (MNP) and p-nitrophenol (PNP), in the MFBES. The results demonstrated that NPs reduction in the MFBES decreased in efficiency in the following order: ONP>MNP>PNP. Illumina MiSeq sequencing results showed that richness and diversity of bacterial species in the anodic and cathodic communities decreased when fed different NPs. Though remarkable differences in community composition were found between anodic and cathodic biofilms in the MFBES, three core genera-Treponema, Desulfovibrio and Geobacter-were dominant in the anodic or cathodic biofilm, regardless of various NPs. Other functional genera in the anodic or cathodic biofilm were selectively enriched in the MFBES treating the three NPs with different structures.

Electrospun ZIF-based hierarchical carbon fiber as an efficient electrocatalyst for the oxygen reduction reaction

The inherently granular nature of nitrogen and metal co-doped carbons derived from metal–organic frameworks (MOFs) hinders their practical application in the oxygen reduction reaction (ORR). In this work, we have developed a novel N, Co-containing MOF-based hierarchical carbon fiber as an ORR catalyst. The products (ZCP-CFs) are synthesized by the incorporation of a Zn, Co-zeolitic imidazolate framework (Zn, Co-ZIF) with electrospun Co2+/poly(acrylonitrile) fiber, followed by carbonization and acid leaching treatment. The effects of the pyrolysis temperature and precursor on the ORR performance of the final samples were systematically studied. The results indicated that the material prepared at 900 °C (ZCP-CFs-9) was identified as the best ORR catalyst in the series of samples. Further comparison among samples obtained from different catalyst precursors also demonstrated the superior performance of ZCP-CFs-9, with its more positive half-wave potential (−0.135 V vs. Ag/AgCl), higher diffusion-limited and kinetic-limiting currents and higher selectivity (number of electrons transferred n = ∼3.97) than Zn, Co-ZIF derived carbon and Zn, Co-ZIF free carbon fiber. Notably, the ZCP-CFs-9 catalyst exhibited very close activity to a commercial Pt/C catalyst with better durability and stronger tolerance to methanol crossover. The remarkable ORR performance may be ascribed to its unique structure, such as its large surface area and hierarchical porosity, the dispersed and protected Co nanoparticles and N functionalized carbon framework, as well as the abundant graphitic carbon and its 1D fibrous structure. Considering the diversity of MOFs and electrospinnable polymer precursors, this strategy may be further extended to other MOF-based carbon fibers for energy storage and conversion.