Xiang-Ning Song

Novel Bi12O15Cl6 Photocatalyst for the Degradation of Bisphenol A under Visible-Light Irradiation

Bisphenol A (BPA), a typical endocrine-disrupting chemical, is widely present in water environments, and its efficient and cost-effective removal is greatly needed. Among various physicochemical methods for BPA degradation, visible-light-driven catalytic degradation of BPA is a promising approach because of its utilization of solar energy. Bismuth oxychloride (BiOCl) is recognized as an efficient photocatalyst, but its band gap, >3.0 eV, makes it inefficient for solar energy utilization, especially for degrading nondye pollutants like BPA. Thus, preparation and application of bismuth oxychloride photocatalysts with an increased visible-light activity are essential. In this work, inspired by density functional theory calculations, a novel bismuth oxychloride photocatalyst, Bi12O15Cl6, was designed. The nanosheets were successfully synthesized using a facile solvothermal method followed by a thermal treatment route. The prepared Bi12O15Cl6 nanosheets had a favorable energy band structure and thus exhibited a superior visible-light photocatalytic activity for degrading BPA. The BPA degradation rate by the Bi12O15Cl6 was determined to be 13.6 and 8.7 times faster than those for BiOCl and TiO2 (P25), respectively. The photogenerated reactive species and degradation intermediates were identified, and the photocatalytic mechanism was elucidated. Furthermore, the as-synthesized Bi12O15Cl6 nanosheets remained stable in the photocatalytic process and could be used repeatedly, demonstrating their promising application in the degradation of diverse pollutants in water and wastewater.

Oxygen promotes biofilm formation of Shewanella putrefaciens CN32 through a diguanylate cyclase and an adhesin

Although oxygen has been reported to regulate biofilm formation by several Shewanella species, the exact regulatory mechanism mostly remains unclear. Here, we identify a direct oxygen-sensing diguanylate cyclase (DosD) and reveal its regulatory role in biofilm formation by Shewanella putrefaciens CN32 under aerobic conditions. In vitro and in vivo analyses revealed that the activity of DosD culminates to synthesis of cyclic diguanylate (c-di-GMP) in the presence of oxygen. DosD regulates the transcription of bpfA operon which encodes seven proteins including a large repetitive adhesin BpfA and its cognate type I secretion system (TISS). Regulation of DosD in aerobic biofilms is heavily dependent on an adhesin BpfA and the TISS. This study offers an insight into the molecular mechanism of oxygen-stimulated biofilm formation by S. putrefaciens CN32.

Quorum quenching is responsible for the underestimated quorum sensing effects in biological wastewater treatment reactors.

Quorum sensing (QS) and quorum quenching (QQ) are two antagonistic processes coexisting in various bacterial communities in bioreactors, e.g., activated sludge for biological wastewater treatment. Although QS signal molecules are detected in activated sludge reactors and known to affect sludge properties and reactor performance, there has been no direct evidence to prove the endogenous existence of QQ effects in activated sludge. In this study, for the first time, acyl homoserine lactones-degrading enzymatic activity, a typical QQ effect, was discovered in activated sludge and found to considerably affect the QS detection results. The coexistence of QS and QQ bacteria in activated sludge was further confirmed by bacterial screening and denaturing gradient gel electrophoresis analysis. The method developed in this study could also be used to evaluate QQ activities in bioreactors, and a possible way is provided to tune bioreactor performance through balancing the QS and QQ processes.

An UV-vis spectroelectrochemical approach for rapid detection of phenazines and exploration of their redox characteristics

Phenazines are widely distributed in the environment and play an important role in various biological processes to facilitate microbial metabolism and electron transfer. In this work, an efficient and reliable spectroelectrochemical method is developed to quantitatively detect 1-hydroxyphenazine (1-OHPZ), a representative phenazine, and explore its redox characteristics. This approach is based on the sensitive absorption change of 1-OHPZ in response to its changes under redox state in rapid electrochemical reduction. The redox reaction of 1-OHPZ in aqueous solution is a proton-coupled electron transfer process, with a reversible one-step 2e(-)/2H(+) transfer reaction. This spectroelectrochemical approach exhibits good linear response covering two magnitudes to 1-OHPZ with a detection limit of 0.48µM, and is successfully applied to detect 1-OHPZ from a mixture of phenazines produced by Pseudomonas aeruginosa cultures. This method might also be applicable in exploring the abundance and redox processes of a wide range of other redox-active molecules in natural and engineered environments.

Electrocatalytic hydrodehalogenation of atrazine in aqueous solution by Cu@Pd/Ti catalyst.

Electrocatalytic hydrodehalogenation is a cost-effective approach to degrade halogenated organic pollutants in groundwater, and Pd-based catalysts have been found to be an efficient cathode material for this purpose. In this work, a novel Cu@Pd bimetallic catalyst loaded on Ti plate was prepared via combined electrodeposition and galvanic replacement for electrocatalytic hydrodehalogenation of atrazine, a typical halogenated pollutant. The obtained bimetallic catalyst with uniformly dispersed Pd nanoparticles possessed a large electrochemically active surface area of 572 cm2. The Cu@Pd/Ti cathode exhibited a higher electrocatalytic efficiency towards atrazine reduction than the individual Pd/Ti or Cu/Ti cathodes, and achieved up to 91.5% within 120 min under a current density of 1 mA cm(-2). Such an electrocatalytic reduction followed pseudo-first-order kinetics with a rate constant of 0.0214 min(-1). Atrazine was selectively transformed to dechlorinated atrazine, and its degradation pathway was identified. Current density was found to have a critical influence on the atrazine reduction due to the competitive hydrogen evolution reaction at a higher current density. The fabricated bimetallic catalyst also exhibited a good stability. This work provides an efficient and stable electrocatalyst for chlorinated contaminate removal and groundwater remediation.

Determination of autoinducer-2 in biological samples by high-performance liquid chromatography with fluorescence detection using pre-column derivatization

Autoinducer-2 (AI-2), as a small-molecular-weight organic molecule secreted and perceived by various bacteria, enables intra- and inter-species communications. Quantitative determination of AI-2 is essential for exploring the bacterial AI-2-related physiological and biochemical processes. However, current strategies for sensitive detection of AI-2 require sophisticated instruments and complicated procedures. In this work, on the basis of the derivatization of AI-2 with 2,3-diaminonaphthalene, a simple, sensitive and cost-effective high-performance liquid chromatography with fluorescence detector (HPLC-FLD) method is developed for the quantitative detection of AI-2. Under the optimized conditions, this method had a broad linear range of 10-14,000 ng/ml (R(2)=0.9999), and a low detection limit of 1.0 ng/ml. Furthermore, the effectiveness of this approach was further validated through measuring the AI-2 concentrations in the cell-free culture supernatants of both Escherichia coli and Vibrio harveyi.

Augmentation of acyl homoserine lactones-producing and -quenching bacterium into activated sludge for its granulation

Quorum sensing (QS), especially acyl homoserine lactone (AHL)-mediated QS, in activated sludge arouses great interests because of its vital role in the formation of biofilm and aerobic granules (AG). Although QS is reported to be largely related to the properties of activated sludge, it is not economically feasible to tune QS in an activated sludge reactor through dosing pure AHL or AHL hydrolase. A more reasonable way to tune QS is to augment reactors with AHL-producing or -quenching bacteria. In this work, the impacts of continuous dose of AHL-producing or -quenching strains on the activated sludge during its granulation process were explored. Augmentation of AHL-producing or -quenching strains resulted in up- or down-regulation of the AHL concentration in the reactors. Granulation of activated sludge was also accomplished in all reactors, but the granules showed negligible or slight differences in the physicochemical properties of sludge, such as nutrients removal, biomass concentration, extracellular polymeric substances, and zeta potential. Interestingly, a smaller granule size was observed for both the reactor augmented with either an AHL-quenching strain or an AHL-producing strain, suggesting that the AHL augmentation suppressed the biofilm development. Pyrosequencing analysis reveals that the granules cultured in the reactors varied widely in bacterial community structure, indicating that the AHL augmentation had a greater impact on the bacterial community structure, rather than on the physicochemical properties of activated sludge. These results demonstrate that the role of QS in the biofilm formation in complex wastewater treatment bioreactors should be re-evaluated.

Quantitative determination of AI-2 quorum-sensing signal of bacteria using high performance liquid chromatography–tandem mass spectrometry

Autoinducer 2 (AI-2), an important bioactive by-product of the LuxS-catalyzed S-ribosylhomocysteine cleavage reaction in the activated-methyl-cycle, has been suggested to serve as a universal intra- and inter-species signaling molecule. The development of reliable and sensitive methods for quantitative determination of AI-2 is highly desired. However, the chemical properties of AI-2 cause difficulty in its quantitative analysis. Herein, we report a high performance liquid chromatography-tandem mass spectrometric method that enables reproducible and sensitive measurement of AI-2 concentrations in complex matrixes. 4,5-Dimethylbenzene-1,2-diamine (DMBDM), an easy-to-obtain commercial reagent, was used for the derivatization treatment. The assay was linear in the concentration range of 1.0-1000ng/mL (R2=0.999) and had a lower limit of quantification of 0.58ng/mL. The method exhibited several advantages, e.g., high selectivity, wide linear response range, and good sensitivity. Furthermore, the effectiveness of the method was further validated through measuring AI-2 concentrations in the cell-free culture supernatant from Escherichia coli wild type.