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The spatial distribution of archaeal lipids in a mesoscale subtropical watershed, Southeast China

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Science China Earth Sciences 2016年第7期59卷 1317-1328页

作者： LI Xue Ying ZHENG FengF eng CHEN Yu Fei GUO Wen Ting ZHANG TingT ing HU AnY i YU Chang Ping ZHANG Chuan Lun State key Lab of Marine Geology Tongji University key Lab of urban pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences

Archaea play an important role in global carbon and nitrogen cycles. Archaeal lipids, such as isoprenoid glycerol diakyl glycerol tetraethers(i GDGTs), are important biomarkers tracing change in archaeal community structure and biogeochemical processes in the natural environments. In this research, the spatial distributions of archaeal lipids in the surface sediments of the Jiulong River(JR) and the Jiulong River estuary(JRE) were examined. GDGT-0(containing zero cyclopentyl ring) and crenarchaeol were the most abundant i GDGTs in the JR and JRE. From the rivers to the estuary, the total i GDGTs, GDGT-0, crenarchaeol and archaeol concentrations showed significant spatial variation; in particular, GDGT-0 and archaeol in the river may be predominantly derived in situ from methanogens, whereas crenarchaeol in the estuary mainly derived in situ from Thaumarchaeota. We inferred that archaeal community was dominated by methanogens in the Jiulong River and by Thaumarchaeota in the Jiulong River estuary, which are consistent with change in archaeal community structure observed in other estuarine environments.

关键词： GDGT-0 Crenarchaeol Archaeol Spatial distribution Jiulong River Jiulong River Estuary

Probing the redox process of p-benzoquinone in dimethyl sulphoxide by using fluorescence spectroelectrochemistry

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Frontiers of Environmental Science & Engineering 2017年第1期11卷 137-143页

作者： Rui Lu Wei Chen Wen-Wei Li Guo-Ping Sheng Lian-Jun Wang Han-Qing Yu Jiangsu key laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing 210094 China cas key laboratory of urban pollutant Conversion Department of Chemistry University of Science and Technology of China Hefei 230026 China

Quinones are common organic compounds frequently used as model dissolved organic matters in water, and their redox properties are usually characterized by either electrochemical or spectroscopic methods separately. In this work, electrochemical methodology was combined with two fluorescence spectroelectrochemical techniques, cyclic voltafluorescence spectrometry （CVF） and derivative cyclic voltafluorescence spectrometry （DCVF）, to determine the electrochemical properties of p-benzoQuinone in dimethvl sulfoxide, an aprotic solution. The CVF results show that the electrochemical reduction ofp-benzoquinone resulted in the formation of radical anion and dianion, which exhibited a lower fluorescence intensity and red-shift of the emission spectra compared to that of p-benzoauinone. The fluorescence intensity was found to vary along with the electrochemical oxidation and reduction ofp-benzoquinone. The CVF and DCVF results were in good consistence. Thus, the combined method offers a powerful tool to investigate the electrochemical process of p-benzoquinone and other natural organic compounds.

关键词： p-Benzoquinone Electrochemistry Fluorescence Spectroelectrochemistry Derivative cyclic volta fluorescence

Nitrogen-doped pyrogenic carbonaceous matter facilitates azo dye decolorization by sulfide: The important role of graphitic nitrogen

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Chinese Chemical Letters 2023年第2期34卷 230-235页

作者： Han-Qing Zhao Wen-Qiang Li Nannan Hou Lei Li Yiran Wang Peili Lu Yang Mu cas key laboratory of urban pollutant Conversion Department of Environmental Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China College of Environment and Ecology Chongqing UniversityChongqing 400044China

Pyrogenic carbonaceous matter(PCM) catalyzes azo dye decolorization by sulfide, but the nitrogen doping catalytic mechanisms are poorly understood. In this study, we found that stagnate time of azo dye methyl orange(MO) decolorization was reduced to 0.54-18.28 min in the presence of various nitrogen-doped graphenes(NGs), remarkably lower compared to graphene itself. Particularly, graphitic nitrogen played a critical role in NGs-catalyzed MO decolorization by sulfide. Gas chromatography-mass spectrometry and in-situ surface Raman analysis demonstrated that doping nitrogen, especially graphite one facilitated reactive intermediate polysulfides formation. This is attributed to the improved electron conductivity through graphitic nitrogen doping, and the enhanced interactions between sulfide and carbon atoms bonded to graphitic nitrogen. This study not only provides a better understanding of PCM impact on transformations and fates of organic pollutants in natural environments, but also offer a new regulation strategy for more efficient wastewater treatment processes in PCM-catalyzed engineering systems.

关键词： Azo dye Decolorization Graphitic N Nitrogen doped graphene Sulfide

Redox-active humics support interspecies syntrophy and shift microbial community

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Science China(Technological Sciences) 2019年第10期62卷 1695-1702页

作者： ZHENG Yue KAPPLER Andreas XIAO Yong YANG Fan MAHADEVA Gurumurthy Dummi ZHAO Feng cas key laboratory of urban pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China University of Chinese Academy of Sciences Beijing100049China Geomicrobiology Center for Applied GeosciencesUniversity of TuebingenTuebingen72076Germany

The network of microbial electron transfer can establish a syntrophic association of microbes by connecting interspecies metabolisms, and a variety of redox-active shuttles in environment have been proved to accelerate the electron flow in a microbial community. Using humic substances as models, we investigated how different redox-active shuttles with different electrochemical properties influence interspecies electron transfer, and affect the shift of microbial communities. The co-culture of two species was constructed with supplements of humics, and the electron transfer between these two strains was found to be linked by humic acid with a wider window of redox potential and multi-peaks of redox reactions. Based on the shift of microbial composition, the humic substances with a wide potential window and multi-peaks of redox reactions for accepting and donating electrons could increase the biodiversity(Chao 1 and phylogenetic diversity) with a large extent. The mechanism by which redox-active shuttles mediate the microbial electron transfer network could facilitate our understanding of syntrophic interactions between microbes.

关键词： humic acid fulvic acid redox-active shuttle microbial diversity interspecies electron transfer

Next generation desalination membrane with exceptional chlorine resistance

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Science China Chemistry 2024年第11期67卷 3500-3502页

作者： Shihong Lin Xinglin Lu Department of Civil and Environmental Engineering Vanderbilt UniversityNashville TN 37235USA cas key laboratory of urban pollutant Conversion Department of Environmental Science and EngineeringNational Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

This highlight draws inspiration from a recent publication in Science where Zhang and co-workers [1] from Nanjing University of Science and Technology reported a novel multifunctional polyester reverse osmosis(RO) membrane and its application in seawater desalination. This research represents a notable advancement in the field, as polyester membranes may potentially compete with state-of-the-art polyamide RO membranes in the mainstream market.

关键词： polyester exceptional chlorine

A mechanistic study on the regioselective Ni-catalyzed methylation–alkenylation of alkyne with AlMe3 and allylic alcohol

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Organic Chemistry Frontiers 2022年第1期9卷 163-172页

作者： Jiao Liu Deguang Liu Wan Nie Haizhu Yu Jing Shi Hefei National laboratory for Physical Sciences at the Microscale iChEMCAS Key Laboratory of Urban Pollutant ConversionAnhui Province Key Laboratory of Biomass Clean EnergyDepartment of ChemistryUniversity of Science and Technology of ChinaHefeiAnhui 230026China Department of Chemistry Anhui UniversityHefeiAnhui 230026China

The recently reported Ni-catalyzed methylation–allylation of alkynes with allylic alcohols and AlMe3 reagents delivers valuable tetrasubstituted alkene units in a highly regioselective *** by the experimental significance and the mechanistic ambiguity(*** details of C–O bond activation,the function of the Lewis acid AlMe3,etc.),we conducted a detailed mechanistic study using density functional theory(DFT)*** reaction was found to occur via the C–O bond activation of allylic alcohol,allylation of alkyne,transmetalation,reductive elimination and catalyst regeneration ***3 could easily react with the allylic alcohol to form a cyclodialuminoxane species bearing two groups of Lewis acid–base *** this regard,the C(allyl)–O bond is remarkably activated,resulting in a relatively facile C–O activation(compared to the typical Lewis-acid mediated reactions).In addition,the Al–Me interaction is a double-edged sword to the methylation step:the cyclodialuminoxane group functions as the methyl resource,while the full dissociation of the Al–Me interaction(via a cis-to-trans isomerization)is a requisite to fully release the methyl *** this context,the“Me-relay”pathway involving the[Ni]–Me intermediate is found to be more plausible than all other mechanistic possibilities(such as the typical concerted Me-transfer mechanism in previous studies).

关键词： alcohol catalyzed allyl

Removal of tetracycline from aqueous solution by a Fe_3O_4 incorporated PAN electrospun nanofiber mat

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Journal of Environmental Sciences 2015年第2期27卷 29-36页

作者： Qing Liu Yuming Zheng Lubin Zhong Xiaoxia Cheng key laboratory of urban pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences College of Resources and Environment University of Chinese Academy of Sciences College of Environmental and Municipal Engineering Xi'an University of Architecture and Technology

Pollution of antibiotics, a type of emerging contaminant, has become an issue of concern,due to their overuse in human and veterinary application, persistence in environment and great potential risk to human and animal health even at trace level. In this work, a novel adsorbent, Fe3O4 incorporated polyacrylonitrile nanofiber mat（Fe-NFM）, was successfully fabricated via electrospinning and solvothermal method, targeting to remove tetracycline（TC）, a typical class of antibiotics, from aqueous solution. Field emission scanning electron microscopy and X-ray diffraction spectroscopy were used to characterize the surface morphology and crystal structure of the Fe-NFM, and demonstrated that Fe-NFM was composed of continuous, randomly distributed uniform nanofibers with surface coating of Fe3O4 nanoparticles. A series of adsorption experiments were carried out to evaluate the removal efficiency of TC by the Fe-NFM. The pseudo-second-order kinetics model fitted better with the experimental data. The highest adsorption capacity was observed at initial solution p H 4 while relative high adsorption performance was obtained from initial solution p H 4 to 10. The adsorption of TC on Fe-NFM was a combination effect of both electrostatic interaction and complexation between TC and Fe-NFM. Freundlich isotherm model could better describe the adsorption isotherm. The maximum adsorption capacity calculated from Langmuir isotherm model was 315.31 mg/g. Compared to conventional nanoparticle adsorbents which have difficulties in downstream separation, the novel nanofiber mat can be simply installed as a modular compartment and easily separated from the aqueous medium, promising its huge potential in drinking and wastewater treatment for micro-pollutant removal.

关键词： Adsorption Antibiotics Electrospinning Composite nanomaterial

Formaldehyde oxidation on Pd/USY catalysts at room temperature: The effect of acid pretreatment on supports

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Journal of Environmental Sciences 2023年第3期125卷 811-822页

作者： Xiaofeng Liu Chunying Wang Yumin Chen Qi Qin Yaobin Li Hong He Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionChinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China Zhejiang key laboratory of urban Environmental Processes and Pollution Control Chinese Academy of SciencesNingbo Urban Environment Observation and Research Station-NUEORSNingbo 315800China State key Joint laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing 100085China Xiamen key laboratory of Materials for Gaseous pollutant Control Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

The complete catalytic oxidation of formaldehyde (HCHO) to CO_(2)and H_(2)O at room temperature is a green route for indoor HCHO *** is an excellent carrier material for HCHO oxidation due to its large surface area,intricate pores and high adsorption ***,the zeolite-supported noble metal catalysts have currently shown relatively low activity especially at room *** this work,we present a facile acid treatment strategy for zeolite catalysts to improve the hydroxyl concentration and further enhance their catalytic activity for HCHO *** tests illustrated that HCHO could be completely oxidized to CO_(2)and H_(2)O at a nearly 100%conversion rate with a weight hourly space velocity (WHSV) of 150,000 mL/(g·hr) at 25℃,when the support of Pd/USY catalysts was pretreated by hydrochloric acid with a concentration of 0.20 mol/*** characterization results revealed that the active hydroxyl groups originated from the dealumination in the acid treatment play a key role in the HCHO oxidation *** deduced reaction mechanism suggests that bridging hydroxyl groups may oxidize HCHO to dioxymethylene(DOM) species and terminal hydroxyl groups are responsible for the transformation of DOM groups to formate (HCOO) species.

关键词： Formaldehyde oxidation USY zeolite Acid treatment Hydroxyl groups

Influence of hydraulic retention time on behavior of antibiotics and antibiotic resistance genes in aerobic granular reactor treating biogas slurry

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Frontiers of Environmental Science & Engineering 2019年第3期13卷 59-67页

作者： Jie Liao Chaoxiang Liu Lin Liu Jie Li Hongyong Fan Jiaqi Ye Zhichao Zeng key laboratory of Environmental Biotechnology Fujian Province University Xiamen University of Technology Xiamen 361024 China key laboratory of urban pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China Fujian Institute of Innovation Chinese Academy of Sciences Fuzhou 350002 China

The behavior of antibiotics and the corresponding resistance genes in aerobic granular reactors for treating biogas slurry under different hydraulic retention times (10.7 h, Rl;8 h, R2) was investigated in this study. The results indicated that the hydraulic retention time could affect the effluent concentrations and removal efficiencies of sulfonamides. The average removal rates of tetracyclines, fluoroquinolones, and sulfonamides were 63%, 46%, and 90% in Rl, and 62%, 46%, and 86% in R2, respectively. Although the removal efficiencies of tetracyclines and fluoroquinolones were similar in both reactors, the respective accumulated concentrations of tetracyclines and fluoroquinolones in R1 were 7.00 and 11.15μg/g SS, which were lower than those in R2 (8.92 and 13.37μg/g SS, respectively). The difference in the relative abundance of target antibiotic resistance genes between both reactors was not significant, yet the average relative abundances of all target resistance genes in R1 were higher than those in R2 after 45 days of operation. The results of this study suggested that a longer hydraulic retention time could enhance the antibiotic removal ability of aerobic granular sludge, yet it may also increase the risk of surplus sludge utilization from a resistance genes point of view.

关键词： Aerobic granules Swine wastewater Tetracyclines Fluoroquinolones Sulfonamides