Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway...Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.展开更多
A synthetic wastewater containing phenol as sole substrate was treated in a 2 8 L upflow anaerobic sludge blanket(UASB) reactor at ambient temperature. The operation conditions and phenol removal efficiency were disc...A synthetic wastewater containing phenol as sole substrate was treated in a 2 8 L upflow anaerobic sludge blanket(UASB) reactor at ambient temperature. The operation conditions and phenol removal efficiency were discussed, microbial population in the UASB sludge was identified based on DNA cloning, and pathway of anaerobic phenol degradation was proposed. Phenol in wastewater was degraded in an UASB reactor at loading rate up to 18 gCOD/(L·d), with a 1:1 recycle ratio, at 26±1℃, pH 7 0—7 5. An UASB reactor was able to remove 99% of phenol up to 1226 mg/L in wastewater with 24 h of hydraulic retention time(HRT). For HRT below 24 h, phenol degradation efficiency decreased with HRT, from 95 4% at 16 h to 93 8% at 12 h. It further deteriorated to 88 5% when HRT reached 8 h. When the concentration of influent phenol of the reactor was 1260 mg/L(corresponding COD 3000 mg/L), with the HRT decreasing(from 40 h to 4 h, corresponding COD loading increasing), the biomass yields tended to increase from 0 265 to 3 08 g/(L·d). While at 12 h of HRT, the biomass yield was lower. When HRT was 12 h, the methane yield was 0 308 L/(gCOD removed), which was the highest. Throughout the study, phenol was the sole organic substrate. The effluent contained only residual phenol without any detectable intermediates, such as benzoate, 4 hydrobenzoate or volatile fatty acids(VFAs). Based on DNA cloning analysis, the sludge was composed of five groups of microorganisms. Desulfotomaculum and Clostridium were likely responsible for the conversion of phenol to benzoate, which was further degraded by Syntrophus to acetate and H 2/CO 2. Methanogens lastly converted acetate and H 2/CO 2 to methane. The role of epsilon Proteobacteria was, however, unsure.展开更多
Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe R...Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe River sediments sequentially. The results showed that the anaerobic degradation of γ 666, p,p' DDT and HCB followed pseudo first order kinetics in different sediments. But, the extents and rates of degradation were different, even the other conditions remained the same. Anaerobic degradation rates of γ 666, p,p' DDT and HCB were 0 020 d -1 , 0 009 d -1 and 0 035 month -1 respectively for the sediments without additional carbon resources. However, with addition of carbon resources, the anaerobic degradation rates of γ 666, p, p ' DDT and HCB were 0 071 d -1 , 0 054 d -1 and 0 088 month -1 in the original sediments respectively. After removing NOM, the rates were decreased to 0 047 d -1 , 0 037 d -1 and 0 066 month -1 ; in the sediments removed NOM and HMO, the rates were increased to 0 067 d -1 , 0 059 d -1 and 0 086 month -1 . These results indicated that NOM in the sediments accelerated the anaerobic degradation of γ 666, p,p' DDT and HCB; the HMO inhibited the anaerobic degradation of γ 666, p,p' DDT and HCB.展开更多
Microbial electrochemical technologies have been extensively employed for phenol removal.Yet,previous research has yielded inconsistent results,leaving uncertainties regarding the feasibility of phenol degradation und...Microbial electrochemical technologies have been extensively employed for phenol removal.Yet,previous research has yielded inconsistent results,leaving uncertainties regarding the feasibility of phenol degradation under strictly anaerobic conditions using anodes as sole terminal electron acceptors.In this study,we employed high-performance liquid chromatography and gas chromatography-mass spectrometry to investigate the anaerobic phenol degradation pathway.Our findings provide robust evidence for the purely anaerobic degradation of phenol,as we identified benzoic acid,4-hydroxybenzoic acid,glutaric acid,and other metabolites of this pathway.Notably,no typical intermediates of the aerobic phenol degradation pathway were detected.One-chamber reactors(t0.4 V vs.SHE)exhibited a phenol removal rate of 3.5±0.2 mg L^(-1) d^(-1),while two-chamber reactors showed 3.6±0.1 and 2.6±0.9 mg L^(-1) d^(-1) at anode potentials of t0.4 and t 0.2 V,respectively.Our results also suggest that the reactor configuration certainly influenced the microbial community,presumably leading to different ratios of phenol consumers and microorganisms feeding on degradation products.展开更多
In this study, the authors have investigated the effects of various factors on both aerobic and anaerobic degradation of 4-t-octylphenol （4-t-OP） in granular sludge. In comparison, the aerobic degradation rate was m...In this study, the authors have investigated the effects of various factors on both aerobic and anaerobic degradation of 4-t-octylphenol （4-t-OP） in granular sludge. In comparison, the aerobic degradation rate was much higher than that of anaerobic degradation. The optimal pH values for 4-t-OP degradation in granular sludge were 9 and 7 under aerobic and anaerobic conditions, respectively. And the degradation rate decreased with an increase in the initial 4-t-OP concentration. Addition of yeast extract or homologous compounds such as phenol also enhanced the 4-t-OP degradation, especially under the aerobic condition. To investigate the bacterial community in this study, the denaturing gradient gel electrophoresis （DGGE） method was applied, based on the primers, for the 16S rDNA V3 region of bacteria, γ-proteobacteria and bacillus were identified as the major species of sludge.展开更多
A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction...A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction.Clones of Syntrophorhabdaceae and Cryptanaerobacter were observed to be responsible for phenol degradation.For accurate taxonomic assignment of Cryptanaerobacter clones,phylogenetic analysis using nearly full-length 16S ribosomal RNA(rRNA)gene sequences was necessary.Three oligonucleotide probes were designed to detect the following three taxonomic groups:Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus.FISH analysis of thin sections of anaerobic granules showed a random distribution of bacteria and archaea.However,a well-defined distribution of Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus was observed.Cryptanaerobacter and Syntrophus were found on the outer layer of the granules and were closely associated with each other,while Syntrophorhabdaceae was located in the deeper part of the granules.Such specific distribution of the bacteria is most likely due to their metabolic association and affinity for the substrate.Phenol degradation in the granular sludge was observed to be carried out in the following way.First,Cryptanaerobacter converts phenol to benzoate,which is then degraded by Syntrophus into acetate.This syntrophic degradation of phenol occurs near the surface of the granule,where the phenol concen-tration is high.In the deeper part of the granule,where the phenol concentration is lower,Syntrophorhabdaceae degrades phenol into acetate.We observed that Syntrophorhabdaceae is less likely to produce benzoate as an intermediate to feed the neighboring organisms,which contradicts the theo-ries presented by previous studies.展开更多
This study reports an increase in power generation of a MFC （microbial fuel cell） by the addition of Korean ginseng （Panax ginseng）. It was noted that the use of ginseng enhances the microbial anaerobic degradatio...This study reports an increase in power generation of a MFC （microbial fuel cell） by the addition of Korean ginseng （Panax ginseng）. It was noted that the use of ginseng enhances the microbial anaerobic degradation of cellobiose, a disaccharide that was used as a substrate in the anode chamber of the MFC. The power output of the MFC where ginseng was added showed noticeable enhancement compared to the control MFC. The increase slowly ramped at the initial days and became appreciably higher after the 11th day of incubation in an experiment set up for 16 days duration. It is attributed that the ginseng increases the CO2 production by accelerating the fermentation process. Decrease in CH4/CO2 ratio was observed also due to decrease in methane production per digested cellobiose, the proton donor in the current study. Four ring steroid-like structural moiety Ginsenoside of Panax ginseng seemed to play a beneficial role in the electron transfer from ceilobiose to the anode, perhaps by rendering easier electron transfer due to favorable energy level alignments.展开更多
We describe a specific procedure for the synthesis of deuterium-labelled 2-（1-methylalkyl）succinate established via alkylation of diethyl malonate, Krapcho decarboxylation reaction with D20 and hydrolysis reaction. ...We describe a specific procedure for the synthesis of deuterium-labelled 2-（1-methylalkyl）succinate established via alkylation of diethyl malonate, Krapcho decarboxylation reaction with D20 and hydrolysis reaction. Two novel compounds, 2-[^2H]-2-ethylsuccinic acid and 2-[^2H]-2-（1-methylhep- tyl）succinic acid were prepared via this synthetic route and characterized by mass spectrometry and ^1H NMR. The results showed that the 2-（1-methylalkyl）succinic acids were deuterated at the β-position, which is considered as an important reaction centre in the anaerobic degradation of n-alkanes.展开更多
基金the National Natural Science Foundation of China(Nos.41406090,42176045)the Science Foundation of Qingdao Agricultural University(No.631302)+1 种基金the Fujian Key Laboratory of Functional Marine Sensing Materials,Minjiang University(No.MJUKF-FMSM202102)the Natural Science Foundation of Shandong Province(Nos.ZR2019 MB020,ZR2020MB119)。
文摘Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.
文摘A synthetic wastewater containing phenol as sole substrate was treated in a 2 8 L upflow anaerobic sludge blanket(UASB) reactor at ambient temperature. The operation conditions and phenol removal efficiency were discussed, microbial population in the UASB sludge was identified based on DNA cloning, and pathway of anaerobic phenol degradation was proposed. Phenol in wastewater was degraded in an UASB reactor at loading rate up to 18 gCOD/(L·d), with a 1:1 recycle ratio, at 26±1℃, pH 7 0—7 5. An UASB reactor was able to remove 99% of phenol up to 1226 mg/L in wastewater with 24 h of hydraulic retention time(HRT). For HRT below 24 h, phenol degradation efficiency decreased with HRT, from 95 4% at 16 h to 93 8% at 12 h. It further deteriorated to 88 5% when HRT reached 8 h. When the concentration of influent phenol of the reactor was 1260 mg/L(corresponding COD 3000 mg/L), with the HRT decreasing(from 40 h to 4 h, corresponding COD loading increasing), the biomass yields tended to increase from 0 265 to 3 08 g/(L·d). While at 12 h of HRT, the biomass yield was lower. When HRT was 12 h, the methane yield was 0 308 L/(gCOD removed), which was the highest. Throughout the study, phenol was the sole organic substrate. The effluent contained only residual phenol without any detectable intermediates, such as benzoate, 4 hydrobenzoate or volatile fatty acids(VFAs). Based on DNA cloning analysis, the sludge was composed of five groups of microorganisms. Desulfotomaculum and Clostridium were likely responsible for the conversion of phenol to benzoate, which was further degraded by Syntrophus to acetate and H 2/CO 2. Methanogens lastly converted acetate and H 2/CO 2 to methane. The role of epsilon Proteobacteria was, however, unsure.
文摘Effects of natural organic matters(NOM) and hydrated metal oxides(HMO) in sediments on the anaerobic degradation of γ 666, p,p' DDT and HCB were investigated by means of removing NOM and HMO in Liaohe River sediments sequentially. The results showed that the anaerobic degradation of γ 666, p,p' DDT and HCB followed pseudo first order kinetics in different sediments. But, the extents and rates of degradation were different, even the other conditions remained the same. Anaerobic degradation rates of γ 666, p,p' DDT and HCB were 0 020 d -1 , 0 009 d -1 and 0 035 month -1 respectively for the sediments without additional carbon resources. However, with addition of carbon resources, the anaerobic degradation rates of γ 666, p, p ' DDT and HCB were 0 071 d -1 , 0 054 d -1 and 0 088 month -1 in the original sediments respectively. After removing NOM, the rates were decreased to 0 047 d -1 , 0 037 d -1 and 0 066 month -1 ; in the sediments removed NOM and HMO, the rates were increased to 0 067 d -1 , 0 059 d -1 and 0 086 month -1 . These results indicated that NOM in the sediments accelerated the anaerobic degradation of γ 666, p,p' DDT and HCB; the HMO inhibited the anaerobic degradation of γ 666, p,p' DDT and HCB.
基金China Scholarship Council(CSC201804910500)for 4-year granting study abroadsupported by the Helmholtz Association in the frame of the Integration Platform“Tapping nature's potential for sustainable production and a healthy environment”at the UFZ.
文摘Microbial electrochemical technologies have been extensively employed for phenol removal.Yet,previous research has yielded inconsistent results,leaving uncertainties regarding the feasibility of phenol degradation under strictly anaerobic conditions using anodes as sole terminal electron acceptors.In this study,we employed high-performance liquid chromatography and gas chromatography-mass spectrometry to investigate the anaerobic phenol degradation pathway.Our findings provide robust evidence for the purely anaerobic degradation of phenol,as we identified benzoic acid,4-hydroxybenzoic acid,glutaric acid,and other metabolites of this pathway.Notably,no typical intermediates of the aerobic phenol degradation pathway were detected.One-chamber reactors(t0.4 V vs.SHE)exhibited a phenol removal rate of 3.5±0.2 mg L^(-1) d^(-1),while two-chamber reactors showed 3.6±0.1 and 2.6±0.9 mg L^(-1) d^(-1) at anode potentials of t0.4 and t 0.2 V,respectively.Our results also suggest that the reactor configuration certainly influenced the microbial community,presumably leading to different ratios of phenol consumers and microorganisms feeding on degradation products.
文摘In this study, the authors have investigated the effects of various factors on both aerobic and anaerobic degradation of 4-t-octylphenol （4-t-OP） in granular sludge. In comparison, the aerobic degradation rate was much higher than that of anaerobic degradation. The optimal pH values for 4-t-OP degradation in granular sludge were 9 and 7 under aerobic and anaerobic conditions, respectively. And the degradation rate decreased with an increase in the initial 4-t-OP concentration. Addition of yeast extract or homologous compounds such as phenol also enhanced the 4-t-OP degradation, especially under the aerobic condition. To investigate the bacterial community in this study, the denaturing gradient gel electrophoresis （DGGE） method was applied, based on the primers, for the 16S rDNA V3 region of bacteria, γ-proteobacteria and bacillus were identified as the major species of sludge.
基金supported by Grant-in-Aids for Scientific Research(B)(JP18H01564)from the Japan Society for the Promotion of Science.
文摘A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction.Clones of Syntrophorhabdaceae and Cryptanaerobacter were observed to be responsible for phenol degradation.For accurate taxonomic assignment of Cryptanaerobacter clones,phylogenetic analysis using nearly full-length 16S ribosomal RNA(rRNA)gene sequences was necessary.Three oligonucleotide probes were designed to detect the following three taxonomic groups:Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus.FISH analysis of thin sections of anaerobic granules showed a random distribution of bacteria and archaea.However,a well-defined distribution of Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus was observed.Cryptanaerobacter and Syntrophus were found on the outer layer of the granules and were closely associated with each other,while Syntrophorhabdaceae was located in the deeper part of the granules.Such specific distribution of the bacteria is most likely due to their metabolic association and affinity for the substrate.Phenol degradation in the granular sludge was observed to be carried out in the following way.First,Cryptanaerobacter converts phenol to benzoate,which is then degraded by Syntrophus into acetate.This syntrophic degradation of phenol occurs near the surface of the granule,where the phenol concen-tration is high.In the deeper part of the granule,where the phenol concentration is lower,Syntrophorhabdaceae degrades phenol into acetate.We observed that Syntrophorhabdaceae is less likely to produce benzoate as an intermediate to feed the neighboring organisms,which contradicts the theo-ries presented by previous studies.
文摘This study reports an increase in power generation of a MFC （microbial fuel cell） by the addition of Korean ginseng （Panax ginseng）. It was noted that the use of ginseng enhances the microbial anaerobic degradation of cellobiose, a disaccharide that was used as a substrate in the anode chamber of the MFC. The power output of the MFC where ginseng was added showed noticeable enhancement compared to the control MFC. The increase slowly ramped at the initial days and became appreciably higher after the 11th day of incubation in an experiment set up for 16 days duration. It is attributed that the ginseng increases the CO2 production by accelerating the fermentation process. Decrease in CH4/CO2 ratio was observed also due to decrease in methane production per digested cellobiose, the proton donor in the current study. Four ring steroid-like structural moiety Ginsenoside of Panax ginseng seemed to play a beneficial role in the electron transfer from ceilobiose to the anode, perhaps by rendering easier electron transfer due to favorable energy level alignments.
基金supported by the National Natural Science Foundation of China(No.41373070,51174092)the National Natural Science Foundation of China/Research Grants Council Joint Research Fund(No.41161160560)
文摘We describe a specific procedure for the synthesis of deuterium-labelled 2-（1-methylalkyl）succinate established via alkylation of diethyl malonate, Krapcho decarboxylation reaction with D20 and hydrolysis reaction. Two novel compounds, 2-[^2H]-2-ethylsuccinic acid and 2-[^2H]-2-（1-methylhep- tyl）succinic acid were prepared via this synthetic route and characterized by mass spectrometry and ^1H NMR. The results showed that the 2-（1-methylalkyl）succinic acids were deuterated at the β-position, which is considered as an important reaction centre in the anaerobic degradation of n-alkanes.
