Facilitating nitrification and biofilm formation of Vibrio sp. by N-acyl-homoserine lactones in high salinity environment.

The N-acyl-homoserine lactones (AHLs)-mediated quorum-sensing (QS) system played a crucial role in regulating biological nitrogen removal and biofilm formation. However, the regulatory role of AHLs on nitrogen removal bacteria in high salinity environment has remained unclear. This study evaluated the roles and release patterns of AHLs in Vibrio sp. LV-Q1 under high salinity condition. Results showed that Vibrio sp. primarily secretes five AHLs, and the AHLs activity is strongly correlated with the bacterial density. Exogenous C10-HSL and 3OC10-HSL were found to significantly enhance ammonium removal, while making a minor contribution to the growth rate. Both the C10-HSL and 3OC10-HSL promoted the biofilm formation of Vibrio sp. with an enhancement of 1.64 and 1.78 times, respectively. The scanning electron microscope (SEM) and confocal laser scanning microscope (CLSM) observations confirmed the biofilm-enhancing effect of AHLs. Further analysis revealed that AHLs significantly improved bacterial self-aggregation and motility, as well as the level of extracellular polymeric substances (EPS). These findings provide significant guidance on construction of nitrification system at high salinity.

Theoretical insight into the promotion effect of potassium additive on the water-gas shift reaction over low-coordinated Au catalysts.

CONTEXT: How to elucidate the effect of alkali metal promoters on gold-catalyzed water-gas shift reaction intrinsically remains a challenging, because that the complex synergy effects such as strong metal-support interactions, interfacial effects, and charge transfer of supported metal catalysts makes people difficulty in the understanding the alkali promotion phenomenon in nature. Herein, we report a systematically study of whole water-gas shift reaction mechanism on pure and the K-modified defected-Au(211) (i.e., by removing one surface Au atom from perfect Au(211) and make one model with the Au-Au coordination number is six) by using the microkinetic modeling based on first principles. Our results indicate that the presence of K can increase the adsorption ability of oxygen-containing species via the attractive coulomb interaction, has no significant effect on the adsorption of H species, but inhibits the adsorption of CO due to the steric effect. K promoter stabilizes the water adsorption by ~0.3 eV, which results in one order increasing of whole reaction rate. Interestingly, the strong promotion effect of the K can be assigned to the significant direct space interaction between K and the adsorbate H2O* through the inducted electric field, which can be further confirmed by the posed negative electric field on the unpromoted D-Au(211). Microkinetic modeling results revealed that the carboxyl mechanism is the most likely to occur, redox mechanism is the next one, and the formate mechanism is the least likely to occur. For different kinds of alkali metal additives, the adsorption strength of water molecules gradually weakens from Li to Cs, but Na shows the best promoter behavior at the low temperature. By considering the effect of K contents on the reactivity of water-gas shift reaction, we found that the K with the medium coverage (~0.2~0.3 ML) has the strongest promoting effect. It is expected that the conclusion of this work can be extended to other WGSR catalytic systems like Cu(or Pt). METHODS: All calculations were performed by using the plane-wave based periodic method implemented in Vienna ab initio simulation package (VASP, version 5.4.4), where the ionic cores are described by the projector augmented wave (PAW) method. The exchange and correlation energies were computed using the Perdew, Burke and Ernzerhof functional with the vdw correction (PBE-D3). The transition states (TSs) were searched using the climbing image nudged elastic band (CI-NEB) method. Some electronic structure properties like work function was predicated by the DS-PAW software. Microkinetic simulation was carried out using MKMCXX software.

Effects of Promoter and Calcination Temperatures on the Catalytic Performance of Y Promoted Co/WC-AC for Dry Reforming of Methane.

CH4 -CO2 reforming is a good way to convert two environmentally harmful greenhouse gases into a high value syngas. However, the catalytic activity and stability of the catalysts need to be further improved. In this paper, the effects of promoter Y and calcination temperature on the catalytic activity and stability of Co/WC-AC catalysts were investigated. The catalysts were characterized by BET, XRD, CO2 -TPD, H2 -TPR, XPS, and TG-DSC. XPS and H2 -TPR. The results indicated that the introduction of Y decreased the reduction temperature of Co2 O3 species and facilitated the formation of Co2+ species. Meanwhile, the addition of Y increased the content of lattice oxygen on the catalyst surface, which enhanced the carbon elimination capacity of the catalyst. The TG-DSC results showed that the activity and stability of the catalysts calcined at 550 °C were poor due to the presence of carbon materials with weak carbon interactions on the catalyst support surface. Meanwhile, the catalyst calcined at 700 °C lead to the collapse of the pores due to the high calcination temperature, which eventually led to the decrease of the catalyst stability. It was found that the Co-Y/WC-AC catalysts prepared at the calcination temperature of 600 °C had the best catalytic activity and stability.

Direct Construction of 2D Conductive Metal-Organic Frameworks from a Nonplanar Ligand: In Situ Scholl Reaction and Topological Modulation.

Two-dimensional conductive metal-organic frameworks (2D c-MOFs) are an emerging class of promising porous materials with high crystallinity, tunable structures, and diverse functions. However, the limited topologies and difficulties in synthesizing suitable organic linkers remain a great challenge for 2D c-MOFs synthesis and applications. Herein, two layered 2D c-MOF polymorphs with either a rhombus structure (sql-TBA-MOF) or kagome structure (kgm-TBA-MOF) were directly constructed via in situ Scholl reaction and coordination chemistry from a flexible and nonplanar tetraphenylbenzene-based ligand (8OH-TPB) in a one-pot manner. Interestingly, the kgm-TBA-MOF comprising hexagonal and triangular dual pores exhibit higher conductivities of 1.65 × 10-3 S/cm at 298 K and 3.33 × 10-2 S/cm at 353 K than that of sql-TBA-MOF (4.48 × 10-4 and 2.90 × 10-3 S/cm, respectively). Moreover, the morphology and topology can be modulated via the addition of ammonium hydroxide as modulator. The present work provides a new pathway for design, synthesis, and topological regulation of 2D c-MOFs.

Advances in AHLs-mediated quorum sensing system in wastewater biological nitrogen removal: mechanism, function, and application.

Biological nitrogen removal process is to convert organic nitrogen and ammonia nitrogen into nitrogen via a series of reactions by microorganisms, and is widely used in wastewater treatment for its costless, high-effective, secondary pollution-free characteristics. Quorum sensing (QS) is a communication mode for microorganisms to regulate bacteria's physiological behaviors in response to environmental changes. N-acyl-homoserine lactones (AHLs)-mediated QS system is widespread in nitrogen removal-related functional bacteria and promotes biological nitrogen removal performance by regulating bacteria behavior. Recently, there has been an increasingly investigated AHLs-mediated QS system in wastewater biological nitrogen removal process. Consequently, the AHLs-mediated QS system is considered a promising regulatory strategy in the biological nitrogen removal process. This article reviewed the QS mechanism in various nitrogen removal-related functional bacteria and analyzed its effect on biological nitrogen removal performance. Combined with the application research of the QS system for enhanced biological nitrogen removal, it further put forward some prospects and suggestions which are of practical significance in practical application.

Degradation of high concentration starch and biocathode autotrophic denitrification using photo microbial fuel cell.

In the study, a dual-chamber photo MFC was constructed with a photosynthetic bacteria consortium PB-Z and a heterotrophic nitrifier C16 as anode and cathode inoculant, respectively. The electron released from starch degradation in the anode by photosynthetic bacteria was transferred to the cathode, which was utilized by the nitrifying bacteria C16 to realize autotrophic denitrification. Lower resistance was more conducive to the electron transfer and pollutants removal. Comparing with natural light, continuous light greatly promoted starch degradation by the photosynthetic bacteria in the anode and the denitrification by the nitrifying bacteria in the cathode. Under continuous light and external resistance of 500 Ω, high concentration starch was degraded by photosynthetic bacteria PB-Z and the COD removal efficiency reached up to 88.45% within 12 d, and nitrate of 95.8% was removed within 4 d by autotrophic denitrification by heterotrophic nitrifier C16. The study provides some enlightenment and reference for the application of MFC in the field of wastewater treatment.

Nitrate removal performances of a new aerobic denitrifier, Acinetobacter haemolyticus ZYL, isolated from domestic wastewater.

A new aerobic denitrifying bacterium ZYL was isolated from domestic wastewater sludge and identified as Acinetobacter haemolyticus (similarity 99%) by the 16S rDNA sequencing analysis. The strain could use nitrate, nitrite and ammonium as the sole N-source for growth with a final product of N2, demonstrating its good abilities for aerobic denitrification and heterotrophic nitrification. Single-factor experiment results showed that the effective removal of nitrate by strain ZYL occurred with carbon source sodium succinate, C/N 16-24, pH 5-9, temperature 20-40 °C, DO ≥ 4.84 mg/L. Ammonium was preferentially used by strain ZYL with nitrate and ammonium as the mixed nitrogen sources. According to nitrogen utilization, nitrogen balance analysis, enzyme assay and denitrifying gene amplification, nitrate was assimilated directly by the isolate for cell synthesis and also converted into N2 through aerobic denitrification. All these make strain ZYL an ideal choice for treating nitrogen-containing wastewater.

Simultaneous removal characteristics of ammonium and phenol by Alcaligenes faecalis strain WY-01 with the addition of acetate.

In this study, simultaneous removal of ammonium plus phenol could be achieved by Alcaligenes faecalis strain WY-01 with the addition of acetate, although acetate delayed the phenol degradation, probably due to the delayed expression of phenol hydroxylase gene under the presence of acetate. Moreover, the successful expression of key enzyme genes in strain WY-01 provided some evidence to illustrate its metabolic pathways of ammonium and phenol under aerobic conditions. Furthermore, SEM was used to clarify the role of acetate in resisting phenol toxicity, and these results demonstrated that strain WY-01 has the ability to form cell flocs when sodium acetate is used as co-substrate for a high concentration of phenol, and these flocs could protect cells against the toxicity of phenol, further enhancing phenol degradation in a high concentration of phenol. All these will provide further insights into the efficacy of strain WY-01 for treating wastewater cocontaminated by ammonium and phenol.

Polymorphism of 2D Imine Covalent Organic Frameworks.

We designed and synthesized A2 B2 type tetraphenyl benzene monomers (p-, m-, and o-TetPB) which have the para-, meta, and ortho-substituted isomeric structures, for the direct construction of isomeric frameworks. Interestingly, both kagome (kgm) and monoclinic square (sql) framework isomers are produced from either p-TetPB (C2h symmetry) or m-TetPB (C2v symmetry) by changing reaction solvents, while their isomeric structures are characterized by X-ray diffraction, computational simulation, microscopy, and sorption isotherm measurements. Only sql frameworks was formed for o-TetPB (C2v symmetry), irrespective of reaction solvents. These results disclose a unique feature in the framework structural formation, that is, the geometry of monomers directs and dominates the lattice growth process while the solvent plays a role in the perturbation of chain growth pattern. The isomeric frameworks exhibit highly selective adsorption of vitamin B12 owing to pore shape and size differences.

A new approach for the effective removal of NOx from flue gas by using an integrated system of oxidation-absorption-biological reduction.

A new process of NOx removal from flue gas, using an integrated system of oxidation-absorption-biological reduction (OABR), is introduced. The experimental results show that increasing the NOx oxidation ratio in flue gas can effectively improve the NOx removal efficiency of the OABR system. The NOx removal efficiency could reach 98.8% with 0.02 M NaHCO3 as the chemical absorbent and under the condition of the optimal NOx oxidation ratio of 50%. During stable operation, the OABR system could maintain a high NOx removal efficiency (above 94%) under the following conditions: 1-8 vol% (104-8 × 104 ppmv) O2, 200-800 ppmv NOx, 0.5-1.5 L/min gas flow rate and 100-800 ppmv SO2. The nitrogen equilibrium results showed that about 59% of the nitrogen in the inlet NOx were transformed to N2 through microbial denitrification, 37% of the nitrogen were converted to biological nitrogen for microbial growth, and only 1.1% of the nitrogen remained in the liquid phase. This new approach has an excellent NOx removal performance and great potential for industrial application.

Hollow I-Cu2MoS4 nanocubes coupled with an ether-based electrolyte for highly reversible lithium storage.

Anode materials based on transition metal sulfides suffer from poor electrochemical reversibility, which limits their cycling stability. Herein, we synthesize hollow I-Cu2MoS4 nanocubes composed of ultrathin nanosheets using a solvothermal method with Cu2O nanocubes as sacrificial templates. The presence of a surfactant is a key factor that prevents the structural collapse of the hollow cubic structure of Cu2MoS4 and the formation of nanoplates. An ether-based electrolyte shows better compatibility with the Cu2MoS4 electrode than a carbonate-based electrolyte, which is reflected in high reversible capacity, superior rate performance, and remarkably improved cycling performance. Ex-situ XRD analysis demonstrates a highly reversible electrochemical reaction in the ether-based electrolyte, which enhances the cycling stability.

Correction: Visible-light photocatalytic performance, recovery and degradation mechanism of ternary magnetic Fe3O4/BiOBr/BiOI composite.

[This corrects the article DOI: 10.1039/C9RA04412D.].

Draft Genome Sequence of Thermophilic Bacillus sp. TYF-LIM-B05 Directly Producing Ethanol from Various Carbon Sources Including Lignocellulose.

Bacillus sp. TYF-LIM-B05, which is isolated from spoilage vinegar, is resistant to high temperature, high concentrated alcohol, acid, and salt, and can produce ethanol from mono-, di-, polysaccharide, and complex biomass as the sole carbon source. Thus, this strain is a potential candidate for consolidated bioprocessing (CBP) of fermenting lignocellulose to ethanol in a single step. To provide insight into the key enzymes involved in lignocellulose degradation and ethanol production, a draft genome of TYF-LIM-B05 was developed in this study. The results indicated that 348 genes are related to carbohydrate transport and metabolism according to the clusters of orthologous groups of proteins and annotated 187 CAZy domains from a total of 61 different families. The presence of genes encoding laccases, quinone oxidoreductases/reductases, and aryl-alcohol dehydrogenases further implies that TYF-LIM-B05 has the potential to degrade lignin. Remarkably, this strain has the ability to catalyze the oxidative decarboxylation of pyruvate to acetyl-CoA by pyruvate dehydrogenase complexes. The genomic information provided in this study will help researchers to better understand the mechanisms of the lignocellulose degradation and ethanol production pathway in thermophiles.

Draft Genome Sequence of Rummeliibacillus sp. Strain TYF005, a Physiologically Recalcitrant Bacterium with High Ethanol and Salt Tolerance Isolated from Spoilage Vinegar.

Rummeliibacillus sp. strain TYF005 is a thermophilic bacterium with high ethanol (8% vol/vol) and salt (13% wt/vol) tolerance that was isolated from spoilage vinegar. Here, we report the draft genome sequence of this strain, which has 117 scaffolds with a total genome size of 3.7 Mb and a 34.4% GC content.

Improved bioelectricity production using potassium monopersulfate as cathode electron acceptor by novel bio-electrochemical activation in microbial fuel cell.

Potassium monopersulfate (PMS) without a catalyst as cathode electron acceptor was first established to improve the electricity generation performance of a microbial fuel cell (MFC) in this study. The work investigated the performance with pure PMS (PPMS) and compound PMS (CPMS). The concentration and initial pH of PMS had an effect on the electricity generation, which increased with higher PMS concentration and lower catholyte pH. In the PPMS-MFC system, the maximum voltage (0.972 V), power density (16.37 W/m3), optimal exchange current density (2.000 A/m3) and minimum polarization impedance (Rp: 97.33 Ω) were reached at 10 mM PMS and pH 3.0. However, the maximum power density (8.60 W/m3) was exhibited at 70 mM PMS and pH 3.0 in the CPMS system. Additionally, high COD removals of 99.41% and 98.71% in anode chambers were obtained in the two systems, respectively. Sulfate radicals (SO4-) and hydroxyl radicals (OH) played significant roles in the PPMS-MFC, while HClO was also a contributor in addition to SO4- and OH in the CPMS-MFC. Furthermore, SO4- and OH was generated in situ in the cathode to promote the reduction reaction. The inorganic anion had different effects on electricity generation. Finally, while energy was recovered, rhodamine B (RhB) was added to the cathode chamber and then removed successfully in PPMS-MFC system. This work confirmed that only PMS could be activated by bio-electrochemical method, which is an energy-saving, environmentally friendly and effective activation approach, and thus, it could be used as an efficient acceptor in a MFC.

A regularly combined magnetic 3D hierarchical Fe3O4/BiOBr heterostructure: Fabrication, visible-light photocatalytic activity and degradation mechanism.

The magnetic Fe3O4/BiOBr composites with different molar ratios were prepared by a new two-step method. The effect of different Fe3O4 contents on composites' properties was detected through XRD, SEM, TEM, HR-TEM, XPS, Uv-vis DRS, PL and BET. When the molar ratio of Fe3O4 nanospheres and BiOBr nanosheets is 0.5:1, the two are combined regularly to form 3D flower-like hierarchical heterostructure. This phenomenon is firstly found and can provide a reference for synthesizing other regularly combined magnetic heterostructure catalysts. The degradation activity for Rhodamine B (RhB) is much stronger than that of the previous studies under visible-light irradiation. 3D flower-like Fe3O4/BiOBr (0.5:1) heterostructure possesses great advantages including excellent magnetic separation, remarkable reutilization and stability. Through active species detection and liquid chromatography mass spectrometry (LC-MS) analysis, the degradation mechanisms of RhB are summarized (a) RhB photosensitization and (b) RhB moleculs attacked by radicals and a new possible degradation path was to be presented. This study offers a new method to prepare a regularly combined magnetic Fe3O4/BiOBr photocatalytic material and demonstrates its wonderful application for degradation of organic contaminants in aquatic environment.

Low temperature hydrodeoxygenation of guaiacol into cyclohexane over Ni/SiO2 catalyst combined with Hß zeolite.

Hydrodeoxygenation (HDO) of guaiacol to cyclohexane, important for bio-oil upgrading, is usually performed at high reaction temperature (≥200 °C). In this work, low temperature transformation of guaiacol to cyclohexane was achieved at 140 °C over non-noble metal Ni/SiO2 and various zeolites. Among zeolites tested (HUSY, HMOR, Hß, HZSM-5, SAPO-34), Hß zeolite exhibited superior catalytic activity due to its appropriate pore structure and acid strength. The open pore with three-dimensional structure of Hß facilitates the diffusion of guaiacol and intermediates. Meanwhile, weak acid strength of Hß efficiently reduces the competitive adsorption of guaiacol, and then promotes the dehydration of intermediate 2-methoxycyclohexanol. Moreover, the catalytic performance in guaiacol HDO to cyclohexane is also closely related to Si/Al ratio of Hß. Owing to its moderate acid density, the maximum yield of cyclohexane reaches 91.7% on Hß(Si/Al = 50) combined with Ni/SiO2 at 140 °C, which is the lowest temperature ever reported over non-noble metal catalysts.

Visible-light photocatalytic performance, recovery and degradation mechanism of ternary magnetic Fe3O4/BiOBr/BiOI composite.

The ternary magnetic Fe3O4/BiOBr/BiOI (x : 3 : 1) photocatalysts were successfully synthesized by a facile solvothermal method. The samples were characterized by XRD, SEM, EDS, ICP-AES, XPS, UV-vis DRS, PL and VSM. Nitrogen-containing dye RhB was used as a degradation substrate to evaluate the photocatalytic degradation activities of the samples. The photocatalytic performance of Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) is superior to other Fe3O4/BiOBr/BiOI (x : 3 : 1). Compared with binary magnetic Fe3O4/BiOBr (0.5 : 1) prepared in our previous work, the Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) has obvious advantages in photocatalytic activity and adsorption capacity. And the specific surface area (48.30 m2 g-1) is much larger than that of the previous report (Fe3O4/BiOBr/BiOI (0.5 : 2 : 2)) synthesized by a co-precipitation method. Besides, after 25 s of magnetic field, Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) can be rapidly separated from water. After eight recycling cycles, the magnetic properties, photocatalytic activity, crystallization and morphology of the Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) catalyst remain good. The possible photocatalytic degradation mechanism of RhB under Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) photocatalyst was also proposed. The results indicate that the ternary magnetic Fe3O4/BiOBr/BiOI (0.4 : 3 : 1) composite with high photocatalytic degradation efficiency, good magnetic separation performance and excellent recyclability and stability has potential application prospect in wastewater.

A New Anode for Lithium-Ion Batteries Based on Single-Walled Carbon Nanotubes and Graphene: Improved Performance through a Binary Network Design.

Carbon nanomaterials, especially graphene and carbon nanotubes, are considered to be favorable alternatives to graphite-based anodes in lithium-ion batteries, owing to their high specific surface area, electrical conductivity, and excellent mechanical flexibility. However, the limited number of storage sites for lithium ions within the sp2 -carbon hexahedrons leads to the low storage capacity. Thus, rational structure design is essential for the preparation of high-performance carbon-based anode materials. Herein, we employed flexible single-walled carbon nanotubes (SWCNTs) with ultrahigh electrical conductivity as a wrapper for 3D graphene foam (GF) by using a facile dip-coating process to form a binary network structure. This structure, which offered high electrical conductivity, enlarged the electrode/electrolyte contact area, shortened the electron-/ion-transport pathways, and allowed for efficient utilization of the active material, which led to improved electrochemical performance. When used as an anode in lithium-ion batteries, the SWCNT-GF electrode delivered a specific capacity of 953 mA h g-1 at a current density of 0.1 A g-1 and a high reversible capacity of 606 mA h g-1 after 1000 cycles, with a capacity retention of 90 % over 1000 cycles at 1 A g-1 and 189 mA h g-1 after 2200 cycles at 5 A g-1 .

The formation mechanism of the initial C-C chain in ethanol synthesis on γ-AlOOH(100).

An in-depth understanding of the reaction mechanism at the molecular level is the key to guide the synthesis of ethanol over the CuZnAl catalyst, which is one of the major challenges for ethanol application in energy. Reported herein is a density functional theory study of ethanol synthesis from mixed methanol and syngas on the γ-AlOOH(100) surface. The possible elementary reactions are unambiguously identified and for the first time we confirm the high reactivity of the γ-AlOOH(100) surface for the initial C-C chain formation via CO insertion into CH3, which has a 62.8 kJ mol-1 (0.65 eV) activation barrier that is significantly lower than the barriers previously reported. And its corresponding reaction energy is -288.2 kJ mol-1 (-2.99 eV). Bader charge analyses indicate that it is advantageous for the nucleophilic attack of CO to the neighboring CH3 on the γ-AlOOH(100) surface. Our calculations show that ethanol synthesis starts with CH3OH dissociation, goes through CH3O dissociation to yield CH3, subsequently, CO inserts into CH3 to form CH3CO, which is further hydrogenated to yield CH3CHO and eventually obtain C2H5OH. And the formation of intermediate CH3 is the rate-determining step of the overall reaction. The results not only provide new mechanistic insights into the role of γ-AlOOH but also may be useful for the rational designing and optimizing of the CuZnAl catalyst for ethanol synthesis.