Multifunctionality promotes the prosperity of riverine planktonic diatoms in plateau.

Interpreting the biogeographic distribution and underlying mechanisms of functional traits not only contributes to revealing the spatiotemporal dynamics of species biodiversity but also helps to maintain ecological stability during environmental variations. However, little is known about the functional profiles of diatom communities over large river systems. Herein, we provided the first blueprints about the spatiotemporal distributions and driving forces of functional traits for both planktonic and sedimentary diatoms over the 6030 km continuum of the Yangtze River, with the help of the high-throughput sequencing and functional identification. By investigating the 28 functional traits affiliated into five categories, we found that planktonic diatom functions showed clearer landform-heterogeneity patterns (ANOSIM R = 0.336) than sedimentary functions (ANOSIM R = 0.172) along the river, represented by life-forms and ecological-guilds prominent in water-plateau as well as cell-sizes and life-forms particularly in sediment-plateau. Planktonic diatom functions also displayed higher richness and network complexity in plateau (richness: 58.70 ± 9.30, network edges: 65) than in non-plateau regions (23.82 ± 13.16, 16), promoting the stability and robustness of diatom functions against the high-radiation and low-temperature plateau environment. Environmental selection (mainly exerted by PAR, UV, and Tw) played crucial roles in determining the functional variations of planktonic diatoms (explaining 80.5%) rather than sedimentary diatoms (14.5%) between plateau and non-plateau regions. Meanwhile, planktonic diatom traits within life-forms were identified to be well responsive to the ecological environment quality (r = 0.56-0.60, P < 0.001) in the Yangtze. This study provided comprehensive insights into the multifunctionality of diatoms and their responses to environmental disturbance and environment quality, which helps to develop effective strategies for maintaining ecological stability in changing river environments.

Efficient Photosynthesis of Hydrogen Peroxide by Cyano-Containing Covalent Organic Frameworks from Water, Air and Sunlight.

The insufficient exciton (e- -h+ pair) separation/transfer and sluggish two-electron water oxidation are two main factors limiting the H2 O2 photosynthetic efficiency of covalent organic frameworks (COFs) photocatalysts. Herein, we present an alternative strategy to simultaneously facilitate exciton separation/transfer and reduce the energy barrier of two-electron water oxidation in COFs via a dicyano functionalization. The in situ characterization and theoretical calculations reveal that the dicyano functionalization improves the amount of charge transfer channels between donor and acceptor units from two in COF-0CN without cyano functionalization to three in COF-1CN with mono-cyano functionalization and four in COF-2CN with dicyano functionalization, leading to the highest separation/transfer efficiency in COF-2CN. More importantly, the dicyano group activates the neighbouring C atom to produce the key *OH intermediate for effectively reducing the energy barrier of rate-determining two-electron water oxidation in H2 O2 photosynthesis. The simultaneously enhanced exciton separation/transfer and two-electron water oxidation in COF-2CN result in high H2 O2 yield (1601 µmol g-1 h-1 ) from water and oxygen without using sacrificial reagent under visible-light irradiation. COF-2CN can effectively yield H2 O2 in water with wide pH range, in different real water samples, in scaled-up reactor under natural sunlight irradiation, and in continuous-flow reactor for consecutively producing H2 O2 solution for water decontamination.

Morphology-Tailored Hydroxyapatite Nanocarrier for Rhizosphere-Targeted Phosphorus Delivery.

High hydrophilicity and soil fixation collectively hamper the delivery of phosphorus (P) released from conventional chemical phosphorus fertilizers (CPFs) to plant rhizosphere for efficient uptake. Here, a phosphorus nutrient nanocarrier (PNC) based on morphology-tailored nanohydroxyapatite (HAP) is constructed. By virtue of kinetic control of building blocks with designed calcium phosphate intermediates, rod-like and hexagonal prism-like PNCs are synthesized, both having satisfactory hydrophobicity (water contact angle of 105.4- 132.9°) and zeta potential (-17.43 to -58.4 mV at pH range from 3 to 13). Greenhouse experiments demonstrate that the P contents increase by up to 183% in maize rhizosphere and up to 16% in maize biomass when compared to the CPF. Due to the water potential gradient driven by photosynthesis and transpiration, both PNCs are stably transported to maize rhizosphere, and they are capable to counteract soil fixation prior to uptake by plant roots. Within the synergies of the HAP morphological characteristics and triggered phosphate starvation response, root anatomy confirms that two pathways are elucidated to enhance plant P replenishment from the PNCs. Together with structure tunability and facile synthesis, our results offer a new nanodelivery prototype to accommodate plant physiological traits by tailoring the morphology of HAP.

(Fe, Cr)(OH)3 Coprecipitation in Solution and on Soil: Roles of Surface Functional Groups and Solution pH.

The simultaneous precipitation of (Fe, Cr)(OH)3 nanoparticles in solution (homogeneous) and on soil surfaces (heterogeneous), which controls Cr transport in soil and aquatic systems, was quantified for the first time in the presence of model surfaces, i.e., bare and natural organic matter (NOM)-coated SiO2 and Al2O3. Various characterization techniques were combined to explore the surface-ion-precipitate interactions and the controlling mechanisms. (Fe, Cr)(OH)3 accumulation on negatively charged SiO2 was mainly governed by electrostatic interactions between hydrolyzed ion species or homogeneous (Fe, Cr)(OH)3 and surfaces. The elevated pH through protonation of Al2O3 surface hydroxyls resulted in higher Cr/Fe ratios in both homogeneous and heterogeneous coprecipitates. Due to ignorable NOM adsorption onto SiO2, the amounts of (Fe, Cr)(OH)3 precipitates on bare/NOM-SiO2 were similar; contrarily, attributed to favored NOM adsorption onto Al2O3 and consequently carboxyl association with metal ions or (Fe, Cr)(OH)3 nanoparticles, remarkably more heterogeneous precipitates harvested on NOM-Al2O3 than bare-Al2O3. With the same solution supersaturation, the total amounts of homogeneous and heterogeneous precipitates were similar irrespective of the substrate type. With lower pH, decreased electrostatic forces between substrates and precipitates shifted (Fe, Cr)(OH)3 distribution from heterogeneous to homogeneous phases. The quantitative knowledge of (Fe, Cr)(OH)3 distribution and the controlling mechanisms can assist in better Cr sequestration in natural and engineered settings.

Flagella and Their Properties Affect the Transport and Deposition Behaviors of Escherichia coli in Quartz Sand.

The effects of flagella and their properties on bacterial transport and deposition behaviors were examined by using four types of Escherichia coli (E. coli) with or without flagella, as well as with normal or sticky flagella. Packed column, quartz crystal microbalance with dissipation, visible parallel-plate flow chamber system, and visible flow chamber packed with porous media system were employed to investigate the deposition mechanisms of bacteria with different properties of flagella. We found that the presence of flagella favored E. coli deposition onto quartz sand/silica surfaces. Moreover, by changing the porous media porosity and directly observing the bacterial deposition process, local sites with high roughness, narrow flow channels, and grain-to-grain contacts were found to be the major sites for bacterial deposition. Particularly, flagella could help bacteria swim near and then deposit at these sites. In addition, we found that due to the stronger adhesive forces, sticky flagella could further enhance bacterial deposition onto quartz sand/silica surfaces. Elution experiments indicated that flagella could help bacteria attach onto sand surfaces more irreversibly. Clearly, flagella and their properties would have obvious impacts on the transport/deposition behaviors of bacteria in porous media.

Differences in quinone redox system of humic substances between endemic and disease-free areas in Kashin-Beck disease-affected Changdu Region, Tibet, China.

Kashin-Beck disease (KBD) is an endemic disease in China with the highest incidence rate in Tibet region. Promoted generation of oxygen free radicals by semiquinone structure of humic substance (HS) in drinking water was considered to be one of its pathogeneses. Therefore, detailed analysis of HS was performed in water and sediment samples collected from three endemic and three disease-free areas in Changdu Region, Tibet, China. After purification of the HS in the samples, the fractions of HS were characterized using electron paramagnetic resonance, 13C nuclear magnetic resonance, fluorescence spectroscopy with parallel factor analysis and Fourier transform infrared spectroscopy (FTIR). The organic carbon content of HS did not show a significant difference between endemic and disease-free areas or correlation with KBD-associated morbidity. Except FTIR, all techniques succeeded in characterization of the quinone redox system, indicating their validity and consistency. The quinone redox system in aquatic HS exhibited significantly higher level of the following indexes in endemic areas than disease-free areas: semiquinone radical content of fulvic acid (FA) (p < 0.05), aromaticity of FA (p < 0.05), fluorescence intensity (per gram carbon) of reduced quinone-like component of FA (p < 0.05) and humic acid (HA) (p < 0.1). Semiquinone radical content (r = 0.781, p < 0.1), aromaticity of FA (r = 0.891, p < 0.05), intensity of oxidized quinone-like component (r = 0.875, p < 0.05) and reduced quinone-like component of FA (r = 0.793 p < 0.1) showed medium to strong correlation with KBD-associated morbidity. Generally, the content of reduced quinone and aquatic FA showed stronger differences between endemic and disease-free areas than oxidized quinone and aquatic HA, respectively. The quinone redox system in sediment HS did not show any significant relationship with KBD. The present study is a successful attempt to combine the three indexes, semiquinone radical content, aromaticity and fluorescence intensity, in characterizing quinone redox system in HS, facilitating more comprehensive understanding of the characteristics of HS in KBD-affected regions.

Enrichment of antibiotics in an inland lake water.

Inland water is very susceptible to the input of pollutants. However, little is known about the occurrence of antibiotics in inland lakes. In this study, a total of 83 target antibiotics were quantified in water and sediment samples collected from the Qinghai Lake, the largest inland lake of China located on the northeast of Qinghai-Tibet plateau, and its inflowing rivers. The results showed that 27 and 25 antibiotics were detected in water and sediments, respectively, with the summed concentrations (SUM) of 1.14-17.3 ng/L and 0.72-8.31 ng/g. Compared with the input rivers, significantly higher levels of sulfonamides (SAs), quinolones (QNs), polyethers (PEs), and SUM in water samples were observed in Qinghai Lake water. The average proportions of SAs (50.9-52.7%) and QNs (22.0-28.3%) in Qinghai Lake water nearly doubled compared to those in input rivers. An enrichment factor (EF) was proposed to reveal the enrichment degree of antibiotics in Qinghai Lake compared to its input river water. Sulfaguanidine (SGD), flumequine (FLU), and nalidixic acid (NDA) were enriched in Qinghai Lake up to several ten times based on the calculated EF values, due to their persistence in such a cold saline lake. Risk assessment showed that most antibiotics except anhydrochlortetracycline (ACTC) had insignificant risks to aquatic organisms and antibiotic resistance selection in Qinghai Lake water. This study was the first to reveal the enrichment of antibiotics in Qinghai Lake water, and suggests the urgent need to investigate the possible long-term enrichment and environmental risks of antibiotics in inland lakes.

Dispersal limitation drives biogeographical patterns of anammox bacterial communities across the Yangtze River.

Over the past few decades, anaerobic ammonium oxidation (anammox) has been extensively documented at different scales in natural ecosystems. Previous studies have stated that the community composition of anammox bacteria is shaped mainly by environmental factors, whereas spatial factors have been largely overlooked. This study investigated biogeographical patterns of anammox bacterial communities using 42 sediment samples along a 4300-km stretch of the Yangtze River, the longest river in Asia. A significant distance-decay relationship was observed for anammox bacterial community similarity, which was significantly influenced by mean dendritic distance rather than environmental factors. This implied that dispersal limitation plays an important role in shaping biogeographical pattern of anammox community. Furthermore, our results revealed that neutral processes played vital role in shaping community assembly of anammox bacteria, and their communities were seriously dispersal limited. These findings contrast with previous studies on community similarities between broad taxonomic groups, which are mainly determined by niche-based selection owing to greater niche distances within broad taxonomic groups than in anammox bacteria. Importantly, the slope of the distance-decay curve was much steeper than previously reported for whole bacteria, which indicating the species turnover rate of anammox bacterial community was significantly higher than that of the whole bacterial community. Anammox bacteria harbor strong adhesion ability and low dispersal potential, and ultimately exhibited a high species turnover rate. Together, in the context of biogeography, our results highlight the importance of dispersal limitation in shaping the biogeographical pattern of anammox bacterial community.

Redistribution of Electron Equivalents between Magnetite and Aqueous Fe2+ Induced by a Model Quinone Compound AQDS.

The complex interactions between magnetite and aqueous Fe2+ (Fe2+(aq)) pertain to many biogeochemical redox processes in anoxic subsurface environments. The effect of natural organic matter, abundant in these same environments, on Fe2+(aq)-magnetite interactions is an additional complex that remains poorly understood. We investigated the influence of a model quinone molecule anthraquinone-2,6-disulfonate (AQDS) on Fe2+(aq)-magnetite interactions by systematically studying equilibrium Fe2+(aq) concentrations, rates and extents of AQDS reduction, and structural versus surface-localized Fe(II)/Fe(III) ratios in magnetite under different controlled experimental conditions. The equilibrium concentration of Fe2+(aq) in Fe2+-amended magnetite suspensions with AQDS proportionally changes with solution pH or initial AQDS concentration, but independent of magnetite loadings through the solid concentrations that were studied here. The rates and extents of AQDS reduction by Fe2+-amended magnetite proportionally increased with solution pH, magnetite loading, and initial Fe2+(aq) concentration, which correlates with the corresponding change of reduction potentials for the Fe2+-magnetite system. AQDS reduction by surface-associated Fe(II) in the Fe2+-magnetite suspensions induces solid-state migration of electron equivalents from particle interiors to the near-surface region and the production of nonmagnetic Fe(II)-containing species, which inhibits Fe2+(aq) incorporation or electron injection into the magnetite structure. This study demonstrates the significant influence of quinones on reductive activity of the Fe2+-magnetite system.

Lateral transport of soil carbon and land-atmosphere CO2 flux induced by water erosion in China.

Soil erosion by water impacts soil organic carbon stocks and alters CO2 fluxes exchanged with the atmosphere. The role of erosion as a net sink or source of atmospheric CO2 remains highly debated, and little information is available at scales larger than small catchments or regions. This study attempts to quantify the lateral transport of soil carbon and consequent land-atmosphere CO2 fluxes at the scale of China, where severe erosion has occurred for several decades. Based on the distribution of soil erosion rates derived from detailed national surveys and soil carbon inventories, here we show that water erosion in China displaced 180 ± 80 Mt C⋅y(-1) of soil organic carbon during the last two decades, and this resulted a net land sink for atmospheric CO2 of 45 ± 25 Mt C⋅y(-1), equivalent to 8-37% of the terrestrial carbon sink previously assessed in China. Interestingly, the "hotspots," largely distributed in mountainous regions in the most intensive sink areas (>40 g C⋅m(-2)⋅y(-1)), occupy only 1.5% of the total area suffering water erosion, but contribute 19.3% to the national erosion-induced CO2 sink. The erosion-induced CO2 sink underwent a remarkable reduction of about 16% from the middle 1990s to the early 2010s, due to diminishing erosion after the implementation of large-scale soil conservation programs. These findings demonstrate the necessity of including erosion-induced CO2 in the terrestrial budget, hence reducing the level of uncertainty.

Dominant role of ammonia-oxidizing bacteria in nitrification due to ammonia accumulation in sediments of Danjiangkou reservoir, China.

Surface sediments are the inner source of contaminations in aquatic systems and usually maintain aerobic conditions. As the key participators of nitrification process, little is known about the activities and contributions of ammonia-oxidizing archaea (AOA) and bacteria (AOB) in the surface sediments. In this study, we determined the net and potential nitrification rates and used 1-octyne as an AOB specific inhibitor to detect the contributions of AOA and AOB to nitrification in surface sediments of Danjiangkou reservoir, which is the water source area of the middle route of South-to-North Water Diversion Project in China. Quantitative PCR and Illumina high-throughput sequencing were used to evaluate the abundance and diversity of the amoA gene. The net and potential nitrification rates ranged from 0.42 to 1.93 and 2.06 to 8.79 mg N kg-1 dry sediments d-1, respectively. AOB dominated in both net and potential nitrification, whose contribution accounted for 52.7-78.6% and 59.9-88.1%, respectively. The cell-specific ammonia oxidation rate calculation also revealed the cell-specific rates of AOB were higher than that of AOA. The Spearman's rank correlation analysis suggested that ammonia accumulation led to the AOB predominant role in net nitrification activity, and AOB abundance played the key role in potential nitrification activity. Furthermore, phylogenetic analysis suggested AOB were predominantly characterized by the Nitrosospira cluster, while AOA by the Nitrososphaera and Nitrososphaera sister clusters. This study will help us to better understand the contributions and characteristics of AOA and AOB in aquatic sediments and provide improved strategies for nitrogen control in large reservoirs.

Molecular Insights into the Transformation of Dissolved Organic Matter in Landfill Leachate Concentrate during Biodegradation and Coagulation Processes Using ESI FT-ICR MS.

Landfill leachate concentrate is a type of refractory organic wastewater with high environmental risk. Identification of refractory components and insights into the molecular transformations of the organics are essential for the development of efficient treatment process. In this report, molecular compositions of dissolved organic matter (DOM) in leachate concentrate, as well as changes after anaerobic/aerobic biodegradation and coagulation with salts, were characterized using electrospray ionization (ESI) coupled with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). DOM in leachate concentrate were more saturated and less oxidized with more nitrogen and sulfur-containing substances (accounting for 50.0%), comparing with natural organic matter in Suwannee River. Selectivity for different classes of organics during biodegradation and coagulation processes was observed. Substances with low oxidation degree (O/C < 0.3) were more reactive during biodegradation process, leading to the formation of highly oxidized molecules (O/C > 0.5). Unsaturated (H/C < 1.0) and oxidized (O/C > 0.4) substances containing carboxyl groups were preferentially removed after coagulation with Al or Fe sulfate. The complementary functions of biodegradation and coagulation in the treatment of DOM in leachate concentrate were verified at the molecular level. Lignin-derived compounds and sulfur-containing substances in leachate concentrate were resistant to biodegradation and coagulation treatments. To treat leachate concentrate more effectively, processes aimed at removal of such DOM should be developed.

Effect of NaCl on aerobic denitrification by strain Achromobacter sp. GAD-3.

This paper presents the effect of NaCl on aerobic denitrification by a novel aerobic denitrifier strain Achromobacter sp. GAD-3. Results indicated that the aerobic denitrification process was inhibited by NaCl concentrations ≥20 g L-1, leading to lower nitrate removal rates (1.67∼4.0 mg L-1 h-1), higher nitrite accumulation (50.2∼87.4 mg L-1), and increasing N2O emission ratios (13∼72 mg L-1/mg L-1). Poor performance of aerobic denitrification at high salinity was attributed to the suppression of active microbial biomass and electron donating capacity of strain GAD-3. Further studies on the corresponding inhibition of the denitrifying gene expression by higher salinities revealed the significant sensitivity order of nosZ (for N2O reductase) > cnorB (for NO reductase) ≈ nirS (for cytochrome cd(1) nitrite reductase) > napA (for periplasmic nitrate reductase), accompanied with a time-lapse expression between nosZ and cnorB based on reverse transcription and real-time quantitative polymerase chain reaction (RT-qPCR) analysis. The insights into the effect of NaCl on aerobic denitrification are of great significance to upgrade wastewater treatment plants (WWTPs) containing varying levels of salinity.

Effects of heavy metals on aerobic denitrification by strain Pseudomonas stutzeri PCN-1.

Effects of heavy metals on aerobic denitrification have been poorly understood compared with their impacts on anaerobic denitrification. This paper presented effects of four heavy metals (Cd(II), Cu(II), Ni(II), and Zn(II)) on aerobic denitrification by a novel aerobic denitrifying strain Pseudomonas stutzeri PCN-1. Results indicated that aerobic denitrifying activity decreased with increasing heavy metal concentrations due to their corresponding inhibition on the denitrifying gene expression characterized by a time lapse between the expression of the nosZ gene and that of the cnorB gene by PCN-1, which led to lower nitrate removal rate (1.67∼6.67 mg L-1 h-1), higher nitrite accumulation (47.3∼99.8 mg L-1), and higher N2O emission ratios (5∼283 mg L-1/mg L-1). Specially, promotion of the nosZ gene expression by increasing Cu(II) concentrations (0∼0.05 mg L-1) was found, and the absence of Cu resulted in massive N2O emission due to poor synthesis of N2O reductase. The inhibition effect for both aerobic denitrifying activity and denitrifying gene expression was as follows from strongest to least: Cd(II) (0.5∼2.5 mg L-1) > Cu(II) (0.5∼5 mg L-1) > Ni(II) (2∼10 mg L-1) > Zn(II) (25∼50 mg L-1). Furthermore, sensitivity of denitrifying gene to heavy metals was similar in order of nosZ > nirS ≈ cnorB > napA. This study is of significance in understanding the potential application of aerobic denitrifying bacteria in practical wastewater treatment.

Novel Ion-Exchange Coagulants Remove More Low Molecular Weight Organics than Traditional Coagulants.

Low molecular weight (MW) charged organic matter is poorly removed by conventional coagulants but contributes to disinfection byproduct formation during chlorination of drinking waters. We hypothesized that CIEX, a new Al-based hybrid coagulant with ion-exchange functional groups, would be new mechanistic approach to remove low MW organic matter during coagulation and would perform better than polyaluminum chloride (PACl) or metal-salt based coagulants. We measured coagulation performance using dissolved organic carbon (DOC) in a high hardness surface water. CIEX achieved excellent turbidity removal and removed 20% to 46% more DOC than FeCl3, Al2(SO4)3, or PACl, depending on dose. The improved DOC removal was attributable to better removal of low MW organic matter (<2 kDa). We further studied removal mechanisms in a model water containing a low MW organic acid (salicylic acid (SA)). CIEX achieved high removal of organic acids (>90% of SA) independent of pH, whereas removal by metal salts was lower (<15%) and was strongly pH dependent. CIEX ion-exchange capability is facilitated by its covalently bound quaternary ammonium group, which conventional coagulants lack. Plus, unlike other cationic polymers that react with chloramines to form N-nitrosodimethylamine (NDMA), CIEX has a low molar yield (9.3 × 10(-7) mol NDMA per mol CIEX-N).

Simultaneous denitrification and phosphorus removal by Agrobacterium sp. LAD9 under varying oxygen concentration.

Although efficient aerobic denitrification has received increasing attention, few studies have been made on simultaneous denitrification and phosphorus removal (SDPR) under aerobic condition. In this study, SDPR by an efficient aerobic denitrifier, Agrobacterium sp. LAD9, was firstly demonstrated. High nitrate and phosphorus removal rates of 7.50 and 1.02 mg L(-1) h(-1) were achieved in wide range of O2 concentration from 5.92 to 20.02 mg L(-1). The N2O production would be inhibited as O2 concentration exceeded 11.06 mg L(-1), while the phosphorus removal efficiency would be generally improved with increasing O2 concentration. (15)N mass spectrometry revealed that nitrogen removal accorded with the typical aerobic denitrification pathway, while (31)P nuclear magnetic resonance spectroscopy ((31)P NMR) indicated the fate of phosphorus to cells, extracellular polymeric substances (EPS), and polyphosphate (poly-P) of the denitrifier. EPS acted as a reservoir of phosphorus and the transformation of poly-P was dynamic and depended on initial orthophosphate (ortho-P) content. The aerobic SDPR would greatly simplify the conventional wastewater treatment processes which required separated considerations of nitrogen and phosphorus removal.

Nitrite interference and elimination in diphenylcarbazide (DPCI) spectrophotometric determination of hexavalent chromium.

Cr(VI) is highly noted as a carcinogenic, mutagenic, and teratogenic pollutant. However, accurate determination of Cr(VI) in aqueous samples is difficult using the conventional diphenylcarbazide (DPCI) spectrophotometric method upon being interfered by co-existed nitrite. This paper illustrates how to eliminate the nitrite influence in a simple but efficient method based on a detailed analysis of interference mechanism. High-performance liquid chromatography analysis revealed that under acidic condition, DPCI was oxidized by nitrite to other substrates, which could not react with Cr(VI). The final oxidation product of DPCI was further purified by thin-layer chromatography and identified as diaryl carbodiazone by Fourier Transform Ion Cyclotron Resonance-Mass Spectrometry (FTICR-MS) and nuclear magnetic resonance. Consequently, an improved method was proposed by simply adding sulfamic acid for eliminating the nitrite interference in Cr(VI) determination. The proposed method was successfully confirmed by the accurate recovery of Cr(VI) from spiked water samples and further proven with inductively coupled plasma-atomic emission spectroscopy, which demonstrated a great potential for determining Cr(VI) concentration in aqueous samples containing nitrite.

Investigation on the mechanisms for biotransformation of saponins to diosgenin.

In order to improve the efficiency of biotransformation of saponins in Dioscorea zingiberensis to diosgenin, a new enzymatic model was developed to investigate the mechanism of the metabolic systems. Four main saponin hydrolases (E1, E2, E3 and E4) were purified from Trichoderma reesei. Using progracillin as substrate, the enzymatic hydrolysis experiments with E1, E2, E3 and E4 were carried out respectively. Saponin concentrations during each biotransformation reaction were constructed with a kinetic model consisting of a few Michaelis-Menten equations. During biotransformation, C-26 glycoside and C-3 terminal glycoside were cleaved sequentially from saponins by E1, E2, E3 and E4. Then C-3 terminal rhamnoside and C-3 glycoside were released from the aglycone stepwisely by E2 and E3, to yield diosgenin. E2 and E3 were the key enzymes in the system, and cleavage of the C-3 glycoside from saponins was the rate-limiting step in the biotransformation process. The proposed enzymatic model might be used to analyze the mechanism for biotransformation of saponins to diosgenin.

The mystery of rich human gut antibiotic resistome in the Yellow River with hyper-concentrated sediment-laden flow.

Human gut antibiotic resistome widely occur in anoxic environments characterized by high density of bacterial cells and frequent transmission of antibiotic resistance genes (ARGs). Such resistome is greatly diluted, degraded, and restrained in the aerobic habitats within most natural rivers (regarded as "terrestrial guts") connecting continents and the oceans. Here we implemented a large-scale monitoring campaign extending 5,200 km along the Yellow River, and provide the first integral biogeographic pattern for both ARGs and their hosts. We identified plentiful ARGs (24 types and 809 subtypes) and their hosts (24 phyla and 757 MAGs) in three media (water, suspended particulate matter (SPM), and sediment). Unexpectedly, we found diverse human gut bacteria (HGB) acting as supercarriers of ARGs in this oxygen-rich river. We further discovered that numerous microhabitats were created within stratified biofilms that surround SPMs, particularly regarding the aggregation of anaerobic HGB. These microhabitats provide numerous ideal sinks for anaerobic bacteria and facilitate horizontal transfer of ARGs within the stratified biofilms, Furthermore, the stratification of biofilms surrounding SPMs has facilitated synergy between human gut flora and denitrifiers for propagation of ARGs in the anoxic atmospheres, leading to high occurrence of human gut antibiotic resistome. SPMs play active roles in the dynamic interactions of river water and sediment, thus accelerating the evolution of riverine resistome and transmission of human gut antibiotic resistome. This study revealed the special contribution of SPMs to the propagation of ARGs, and highlighted the necessity of making alternative strategies for sustainable management of large rivers with hyper-concentrated sediment-laden flows.

6PPD-quinone affects the photosynthetic carbon fixation in cyanobacteria by extracting photosynthetic electrons.

Photosynthetic carbon fixation by cyanobacteria plays a pivotal role in the global carbon cycle but is threatened by environmental pollutants. To date, the impact of quinones, with electron shuttling properties, on cyanobacterial photosynthesis is unknown. Here, we present the first study investigating the effects of an emerging quinone pollutant, i.e., 6PPD-Q (N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine-quinone), on the cyanobacterium Synechocystis sp. over a 400-generation exposure period. Synechocystis sp. exhibited distinct sequential phases, including hormesis, toxicity, and eventual recovery, throughout this exposure. Extensive evidence, including results of thylakoid membrane morphological and photosynthetic responses, carbon fixation rate, and key gene/protein analyses, strongly indicates that 6PPD-Q is a potent disruptor of photosynthesis. 6PPD-Q accepts photosynthetic electrons at the plastoquinone QB site in photosystem II (PSII) and the phylloquinone A1 site in PSI, leading to a sustained decrease in the carbon fixation of cyanobacteria after an ephemeral increase. This work revealed the specific mechanism by which 6PPD-Q interferes with photosynthetic carbon fixation in cyanobacteria, which is highly important for the global carbon cycle.