Promoting Plasmonic Hot Hole Extraction and Photothermal Effect for the Oxygen Evolution Reactions.

Boosting oxygen evolution reaction by local surface plasmon resonance (LSPR) provides breakthrough opportunities for the promotion of solar energy conversion; the potential of LSPR, however, has rarely been tapped and investigated. Here, we report the precise regulation of commercial Au nanoparticles plasmonic nanomaterial and OER electrocatalysts, viz., the NiCoOx electrocatalytic layer with hole transport ability and photothermal effect is prepared on the surface of Au nanoparticles by photoelectrodeposition. The NiCoOx layer not only increases the transmission distance of holes generated by plasmonic Au nanoparticles, but also reduce the agglomeration of plasmonic Au nanoparticles during long-time OER reaction, which greatly improves the OER catalytic ability. The current density of NiCoOx /Au anode achieves 16.58 mA cm-2 at 2.0 V versus RHE, which is about 6.5 times of pristine NiCoOx anode (2.56 mA cm-2 ) and 47 times of pristine Au anode (0.35 mA cm-2 ). More importantly, with the LSPR and photothermal effect of plasmonic Au nanoparticles, the NiCoOx /Au anode provides additional current density of 7.01 mA cm-2 after illumination, and maintains no attenuation for more than 2000 s. Benefiting from the solution of agglomeration problem of plasmonic Au nanoparticles in the long-time OER process and the effective utilization of generated holes of plasmonic Au nanoparticles, this design can provide guidance for the application of plasmonic materials in the field of electrocatalysis.

A modified discrete tomography for improving the reconstruction of unknown multi-gray-level material in the `missing wedge' situation.

Full angular rotational projections cannot always be acquired in tomographic reconstructions because of the limited space in the experimental setup, leading to the `missing wedge' situation. In this paper, a recovering `missing wedge' discrete algebraic reconstruction technique algorithm (rmwDART) has been proposed to solve the `missing wedge' problem and improve the quality of the three-dimensional reconstruction without prior knowledge of the material component's number or the material's values. By using oversegmentation, boundary extraction and mathematical morphological operations, `missing wedge' artifact areas can be located. Then, in the iteration process, by updating the located areas and regions, high-quality reconstructions can be obtained from the simulations, and the reconstructed images based on the rmwDART algorithm can be obtained from soft X-ray nano-computed tomography experiments. The results showed that there is the potential for discrete tomography.

A modified equally sloped algorithm based on the total variation algorithm in computed tomography for insufficient data.

Computed tomography (CT) has become an important technique for analyzing the inner structures of material, biological and energy fields. However, there are often challenges in the practical application of CT due to insufficient data. For example, the maximum rotation angle of the sample stage is limited by sample space or image reconstruction from the limited number of views required to reduce the X-ray dose delivered to the sample. Therefore, it is difficult to acquire CT images with complete data. In this work, an iterative reconstruction algorithm based on the minimization of the image total variation (TV) has been utilized to develop equally sloped tomography (EST), and the reconstruction was carried out from limited-angle, few-view and noisy data. A synchrotron CT experiment on hydroxyapatite was also carried out to demonstrate the ability of the TV-EST algorithm. The results indicated that the new TV-EST algorithm was capable of achieving high-quality reconstructions from projections with insufficient data.

A modified discrete algebraic reconstruction technique for multiple grey image reconstruction for limited angle range tomography.

The `missing wedge', which is due to a restricted rotation range, is a major challenge for quantitative analysis of an object using tomography. With prior knowledge of the grey levels, the discrete algebraic reconstruction technique (DART) is able to reconstruct objects accurately with projections in a limited angle range. However, the quality of the reconstructions declines as the number of grey levels increases. In this paper, a modified DART (MDART) was proposed, in which each independent region of homogeneous material was chosen as a research object, instead of the grey values. The grey values of each discrete region were estimated according to the solution of the linear projection equations. The iterative process of boundary pixels updating and correcting the grey values of each region was executed alternately. Simulation experiments of binary phantoms as well as multiple grey phantoms show that MDART is capable of achieving high-quality reconstructions with projections in a limited angle range. The interesting advancement of MDART is that neither prior knowledge of the grey values nor the number of grey levels is necessary.

Systematic investigation and modeling prediction of virus inactivation by ozone in wastewater: Decoupling the matrix effects.

Water disinfection is undoubtedly regarded as a critical step in ensuring the water safety for human consumption, and ozone is widely used as a highly effective disinfectant for the control of pathogenic microorganisms in water. Although the diminished ozone efficiencies in complex water matrices have been widely reported, the specific extent to which individual components of matrix act on the virus inactivation by ozone remains unclear, and effective methodologies to predict the comprehensive effects of various factors are needed. In this study, the decoupled impact of the intricate water matrix on the ozone inactivation of viruses was systematically investigated and assessed from a simulative perspective. The concept of "equivalent ozone depletion rate constant" (k') was introduced to quantify the influence of different species, and a kinetic model was developed based on the k' values for simulating the ozone inactivation processes in complex matrix. The mechanisms through which diverse species influenced the ozone inactivation effectiveness were identified: 1) competition effects (k' = 105∼107 M-1s-1), including organic matters and reductive ions (SO32-, NO2-, and I-), which were the most influential species inhibiting the virus inactivation; 2) shielding effects (k' = 103∼104 M-1s-1), including Ca2+, Mg2+, and kaolin; 3) insignificant effects (k' = 0∼1 M-1s-1), including Cl-, SO42-, NO3-, NH4+, and Br-; 4) promotion effects (k' = ∼-103 M-1s-1), including CO32- and HCO3-. Prediction of ozone disinfection efficiency and evaluation of species contribution under complex aquatic matrices were successfully realized utilizing the model. The systematic understanding and methodologies developed in this research provide a reliable framework for predicting ozone inactivation efficiency under complex matrix, and a potential tool for accurate disinfectant dosage determination and interfering factors control in actual wastewater treatment processes.

Low cost and highly dispersed Ce/Na-ZSM-5 catalysts close to atomic dispersion for enhancing formaldehyde oxidation.

Formaldehyde oxidation at room temperature with low-cost catalysts is one of the main development directions of environmental governance. Herein, we developed a low-cost and superior performance highly dispersed Ce on Na-ZSM-5 (Ce/Na-ZSM-5) catalyst, which is close to atomic dispersion for indoor formaldehyde (HCHO) oxidation at low temperature. The highly dispersed catalyst that was similar to atomic dispersion was characterized by EXAFS and AC HAADF-STEM. The optimal Ce/Na-ZSM-5 displays high HCHO removal performance (95%, at room temperature), as well as 100 h stable testing (∼90% HCHO removal). In addition, a reasonable reaction mechanism of the HCHO catalytic oxidation is proposed based on the in situ DRIFT spectra and DFT calculation. This work provides a new way to design an efficient catalyst for the complete oxidation of formaldehyde.

Synergistic effect of ozone and chlorine on inactivating fungal spores: Influencing factors and mechanisms.

Effective control of fungal contamination in water is vital to provide healthy and safe drinking water for human beings. Although ozone was highly effective in inactivating fungi in water, it was limited by a lack of continuous disinfection ability in water supply system. In present study, the inactivation of fungal spores by combining ozone and chlorine was investigated. The synergistic effects of Aspergillus niger and Trichoderma harzianum spores reached 0.47- and 0.55-log within 10 min, respectively. The inactivation efficiency and the synergistic effect would be affected by disinfectant concentration, pH, and temperature. The combined inactivation caused more violent oxidative stimulation and more severe damage to the fungal spores than the individual inactivation based on the flow cytometry analysis and the scanning electron microscopy observation. The synergistic effect during the combined inactivation process was attributed to the generation of hydroxyl radicals by the reaction between ozone and chlorine and the promotion of chlorine penetration by the destruction of cell wall by ozone. The combined inactivation efficiency in natural water samples was reduced by 26.4-43.8% compared with that in PBS. The results of this study provided an efficient and feasible disinfection method for the control of fungi in drinking water.

The aggregation of Aspergillus spores and the impact on their inactivation by chlorine-based disinfectants.

The formation of fungal biofilm goes through some different states, including monodisperse state, aggregated state, germinated state, hyphal and biofilm. The aggregation of spores is a primary step of fungal biofilm development in aquatic systems. Previous studies on the inactivation of fungi were mostly performed in the monodisperse state of fungal spores and biofilm state, however, the inactivation of aggregated fungal spores is still unclear. In this study, the aggregated characteristics of fungal spores (Aspergillus fumigatus and Aspergillus flavus) at different pH values were firstly studied, and the inactivation efficiency of fungal spores at different aggregation degree by chlorine-based disinfectants was also clarified. The results showed that the aggregation degree of Aspergillus fumigatus was the highest at pH 9.0 while it was the lowest at pH 5.0. Aggregation between fungal spores was mainly mediated by occasional adhesin-adhesin interactions and electrostatic interactions. Compared with monodisperse spores, fungal spores were more resistant to chlorine-based disinfectants with the increase of spore aggregation degree. The inactivation rate constants of Aspergillus fumigatus at 30% and 63% aggregation degree were 1.5- and 4-folds lower than that of monodisperse spores, respectively. The lower proportion of membrane damage and higher intracellular reactive oxygen species level for aggregated spores than monodisperse spores was observed according to the flow cytometric results after chlorine-based disinfectants treatment. The reasons for the lower inactivation efficiency of aggregated spores are as following: the protection of outer layer spores and signals between aggregates lead to the increase of resistance for aggregated spores. This study is meaningful for the control of the fungal spores at different states in water.

Inactivation of fungal spores in water using ozone: Kinetics, influencing factors and mechanisms.

Fungal contamination of drinking water sources is increasingly threatening the environment and human health. In this study, the inactivation of three genera of dominant fungi in drinking water sources using ozone was first reported. The inactivation of the fungal spores by ozone could be divided into two distinct stages: first a rapid reduction in survival, and then the inactivation at a slower rate. The secondary stage inactivation fitted the Chick-Watson model well, and there was no significant difference in the second-order inactivation rate constants of the three fungal spores (0.199-0.209 L mg-1 min-1). The inactivation rate constants of fungal spores by molecular ozone were much lower than those of viruses, which were equivalent to that of Cryptosporidium. The increase in pH and temperature showed a positive effect on the inactivation rate. Damage to cell membranes, leakage of intracellular compounds, and changes of reactive oxygen species and esterase activity in the spores were detected after inactivation. The results indicated that ozone inactivated fungal spores by firstly destroying cell walls and membranes and then causing the release of intracellular compounds. The fungicidal efficiency of ozone was superior to those of chlorine and chlorine dioxide. In addition, the inactivation efficiency of ozone on fungal spores in real water matrices was reduced to 50.7-91.2% of the efficiency in phosphate buffer. In conclusion, ozone showed high efficiency in the inactivation of fungal spores and could be used as an alternative disinfectant for fungal contamination in drinking water sources.

Efficient inactivation of bacteria in ballast water by adding potassium peroxymonosulfate alone: Role of halide ions.

In recent years, ballast water disinfection has been paid much more attention due to the untreated discharged ballast water posing threaten of biological invasion and health related consequences. In this study, an effective and simple approach for ballast water disinfection by just adding potassium peroxymonosulfate (PMS) was assessed, and the role of halide ions in seawater on the enhancement of inactivation was revealed. The reactive species responsible for inactivation, the leakage of intracellular materials, and changes of cellular morphology after inactivation were evaluated to explore the inactivation mechanism. The results showed that Escherichia coli and Bacillus subtilis in ballast water could be totally inactivated within 10 min by adding 0.2 mM PMS alone. The inactivation of bacteria in ballast water fitted to the delayed Chick-Watson model. Chloride and bromide ion in seawater were found to play a crucial role in inactivating bacteria, while the effect of iodide ion could be negligible due to its relative lower concentration in seawater. Chlorine and bromine, produced by the reaction of PMS with chloride and bromide ion, were proved to be the main reactive components that were responsible for the inactivation of bacteria. The extracellular ATP and total nitrogen concentration increased after inactivation which indicated that cell membrane was destroyed by reactive oxidants produced by the reaction between PMS and halide ions. The change of cell morphology confirmed that bacteria were seriously damaged after inactivation. The results suggest that PMS is an attractive alternative disinfectant for ballast water disinfection and this application deserved further research.

Microfluidic dielectrophoresis device for trapping, counting and detecting Shewanella oneidensis at the cell level.

Shewanella oneidensis, a model organism for electrochemical activity bacteria, has been widely studied at the biofilm level. However, to obtain more information regarding this species, it is essential to develop an approach to trap and detect S. oneidensis at the cell level. In this study, we report a rapid and label-free microfluidic platform for trapping, counting and detecting S. oneidensis cells. A microfluidic chip was integrated with a modified dielectrophoresis (DEP) trapping technique and hole arrays of different hole sizes. By numerical simulation and an elaborate electric field distribution design, S. oneidensis cells were successfully trapped and positioned in the hole arrays. Real time fluorescence imaging was also used to observe the trapping process. With the aid of a homemade image program, the trapped bacteria were accurately counted, and the results demonstrated that the amount of bacteria correlated with the hole sizes. As one of the significant applications of the device, Raman identification and detection of countable S. oneidensis cells was accomplished in two kinds of holes. The microfluidic platform provides a quantitative sample preparation and analysis method at the cell level that could be widely applied in the environmental and energy fields.