This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced ...This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced oxidation processes (AOPs).The changing characteristics of NOM were evaluated by dissolved organic carbon (DOC),the specific UV absorbance (SUVA),trihalomethanes formation potential (THMFP),organic halogen adsorbable on activated carbon formation potential (AOXFP) and parallel factor analysis of excitation–emission matrices (PARAFAC-EEMs).In the three UV-based AOPs,HPI fraction with low molecular weight and aromaticity was more likely to degradate than HPO and TPI,and the removal efficiency of SUVA for HPO was much higher than TPI and HPI fraction.In terms of the specific THMFP of HPO,TPI and HPI,a reduction was achieved in the UV/H_(2)O_(2)process,and the higest removal rate even reached to 83%.UV/TiO_(2)and UV/PS processes can only decrease the specific THMFP of HPI.The specific AOXFP of HPO,TPI and HPI fractions were all able to be degraded by the three UV-based AOPs,and HPO content is more susceptible to decompose than TPI and HPI content.UV/H_(2)O_(2)was found to be the most effective treatment for the removal of THMFP and AOXFP under given conditions.C1 (microbial or marine derived humic-like substances),C_(2) (terrestrially derived humic-like substances)and C_(3) (tryptophan-like proteins) fluorescent components of HPO fraction were fairly labile across the UV-based AOPs treatment.C_(3) of each fraction of NOM was the most resistant to degrade upon the UV-based AOPs.Results from this study may provide the prediction about the consequence of UV-based AOPs for the degradation of different fractions of NOM with varied characteristics.展开更多
This study evaluated the removal of multiple pollutants,i.e.,polybrominated diphenyl ethers(PBDEs),novel halogenated flame retardants(HFRs),sulfonamide antibiotics(SAs),and heavy metals(HMs),by a fullscale reversed A^...This study evaluated the removal of multiple pollutants,i.e.,polybrominated diphenyl ethers(PBDEs),novel halogenated flame retardants(HFRs),sulfonamide antibiotics(SAs),and heavy metals(HMs),by a fullscale reversed A^(2)/O process in a sewage treatment plant(STP)in Guangzhou,China.The reversed A^(2)/O process demonstrated high removal efficiencies(REs)for total PBDEs(60.5%±4.3%),novel HFRs(98.4%±2.8%)and HMs(70.1%±1.2%),and a relatively low RE for SAs(25.0%±2.3%).BDE 209,the dominant PBDE congener,showed a high residual concentration(13.41±5.18 ng/L)in the suspended particulate matter(SPM)of treated effluents.So me novel HFRs,dechlorane plus(DP)and decabromodiphe nyl ethane(DBDPE),were detected in the SPM of the raw sewage(7.50±4.14 ng/L and 11.52±11.65 ng/L,respectively).The removal ofSAs was mainly through biodegradation in the activated sludge bioreactors(ASBs).Ofthe HMs,Mn and Ni exhibited the lowest REs(47.5%±2.2%and 35.0%±2.6%,respectively),while Cr and Cu showed the highest removal(REs>80%).In terms of treatment units in the reversed A^(2)/O process,ASBs showed the highest RE(27.8%)for the multiple pollutants.The information can aid in our understanding of removal properties of STPs on various pollutants and evaluating the ecological/health risks of STPs as point pollutant sources.展开更多
Multinanoparticles interacting with the phospholipid membranes in solution were studied by dissipative particle dynamics simulation.The selected nanoparticles have spherical or cylindrical shapes,and they have various...Multinanoparticles interacting with the phospholipid membranes in solution were studied by dissipative particle dynamics simulation.The selected nanoparticles have spherical or cylindrical shapes,and they have various initial velocities in the dynamical processes.Several translocation modes are defined according to their characteristics in the dynamical processes,in which the phase diagrams are constructed based on the interaction strengths between the particles and membranes and the initial velocities of particles.Furthermore,several parameters,such as the system energy and radius of gyration,are investigated in the dynamical processes for the various translocation modes.Results elucidate the effects of multiparticles interacting with the membranes in the biological processes.展开更多
Background Seasonal freeze-thaw(FT)processes alter soil formation and cause changes in soil microbial communi-ties,which regulate the decomposition of organic matter in alpine ecosystems.Soil aggregates are basic stru...Background Seasonal freeze-thaw(FT)processes alter soil formation and cause changes in soil microbial communi-ties,which regulate the decomposition of organic matter in alpine ecosystems.Soil aggregates are basic structural units and play a critical role in microbial habitation.However,the impact of seasonal FT processes on the distribution of microbial communities associated with soil pores in different aggregate fractions under climate change has been overlooked.In this study,we sampled soil aggregates from two typical alpine ecosystems(alpine meadow and alpine shrubland)during the seasonal FT processes(UFP:unstable freezing period,SFP:stable frozen period,UTP:unstable thawing period and STP:stable thawed period).The phospholipid fatty acid(PLFA)method was used to determine the biomass of living microbes in different aggregate fractions.Results The microbial biomass of 0.25–2 mm and 0.053–0.25 mm aggregates did not change significantly dur-ing the seasonal FT process while the microbial biomass of>2 mm aggregates presented a significant difference between the STP and UTP.Bacterial communities dominated the microbes in aggregates,accounting for over 80%of the total PLFAs.The microbial communities of soil aggregates in the surface layer were more sensitive to the sea-sonal FT process than those in other soil layers.In the thawing period,Gram positive bacteria(GP)was more dominant.In the freezing period,the ratio of Gram-positive to Gram-negative bacterial PLFAs(GP/GN)was low because the enrichment of plant litter facilitated the formation of organic matter.In the freezing process,pores of 30–80μm(mesopores)favored the habitation of fungal and actinobacterial communities while total PLFAs and bacterial PLFAs were negatively correlated with mesopores in the thawing process.Conclusions The freezing process caused a greater variability in microbial biomass of different aggregate fractions.The thawing process increased the differences in microbial biomass among soil horizons.Mesopores of aggregates supported the habitation of actinobacterial and fungal communities while they were not conducive to bacterial growth.These findings provide a further comprehension of biodiversity and accurate estimation of global carbon cycle.展开更多
Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number ...Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.展开更多
Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.La...Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.Layer‐by‐layer(LbL)processing with a p–i–n configuration offers an innovative solution by enabling precise control over donor–acceptor distribution and interfacial characteristics.Here,we systematically investigate nine halogen‐functionalized additives across three categories—methyl halides,thiophene halides,and benzene halides—for optimizing LbL device performance.These additives,distinguished by their diverse thermal properties and solid–liquid transformation capabilities below 100°C,are functionalized as both nucleation centers and morphology‐modulating plasticizers during thermal treatment.Among them,2‐bromo‐5‐iodothiophene(BIT)demonstrates superior performance through synergistic effects of its bromine–iodine combination and thiophene core in mediating donor–acceptor interactions.LbL devices processed with BIT achieve exceptional metrics in the PM6/L8‐BO system,including a open‐circuit voltage of 0.916 V,a short‐circuit current density of 27.12 mA cm−2,and an fill factor of 80.97%,resulting in an impressive power conversion efficiency of 20.12%.This study establishes a molecular design strategy for halogen‐functionalized additives that simultaneously optimizes both donor and acceptor layers while maintaining processing simplicity for potential industrial applications.展开更多
A research team led by Dr.GE Ziyi from the Ningbo Institute of Materials Technology and Engineering(NIMTE)of the Chinese Academy of Sciences has developed novel giant acceptors with an oxygenated linker,enabling the c...A research team led by Dr.GE Ziyi from the Ningbo Institute of Materials Technology and Engineering(NIMTE)of the Chinese Academy of Sciences has developed novel giant acceptors with an oxygenated linker,enabling the creation of highly efficient non-halogen-processed organic solar cells(OSCs),with a power conversion efficiency(PCE)up to 20.02%.展开更多
Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosyn...Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosynthesis and separation strategy for halogenation reagents—N-chlorosuccinimide(NCS)and N-bromosuccinimide(NBS)—at high current densities.Faradic efficiency(FE)of 91.0%and 81.3%was achieved for NCS and NBS generation on RuO_(x)/TiO_(2)/Ti in a batch cell,respectively.Electrosynthesis of NCS likely involves both heterogeneous catalytic and homogeneous tandem pathways,while NBS is likely formed in a Langmuir-Hinshelwood mechanism with a proton-coupled electron transfer as the rate-determining step.A coupled continuous electrocatalytic synthesis and in situ separation setup was developed for the efficient production of NCS and NBS,which yielded 0.77 g of NCS in 12000 s and 0.81 g of NBS in 15000 s,both with relative purity exceeding 95%.The halogenation of acetone using NCS and NBS enabled gram-scale production of the key intermediate in organic synthesis,1-halogenacetone,with over 95%recovery of succinimide.展开更多
基金supported by the “Central leading local” Science and Technology Development Fund Project of Shandong Province (No.YDZX202037 00001642)the Key Research and Development Plan of Shandong Province(NO.2020CXGC011406),the Natural Science Foundation of Shandong Province (No.ZR2021ME166)the Special Project of Taishan Scholar Construction Engineering (No.ts201712084)。
文摘This study examined the effectiveness for degradation of hydrophobic (HPO),transphilic(TPI) and hydrophilic (HPI) fractions of natural organic matter (NOM) during UV/H_(2)O_(2),UV/TiO_(2)and UV/K2S2O8(UV/PS) advanced oxidation processes (AOPs).The changing characteristics of NOM were evaluated by dissolved organic carbon (DOC),the specific UV absorbance (SUVA),trihalomethanes formation potential (THMFP),organic halogen adsorbable on activated carbon formation potential (AOXFP) and parallel factor analysis of excitation–emission matrices (PARAFAC-EEMs).In the three UV-based AOPs,HPI fraction with low molecular weight and aromaticity was more likely to degradate than HPO and TPI,and the removal efficiency of SUVA for HPO was much higher than TPI and HPI fraction.In terms of the specific THMFP of HPO,TPI and HPI,a reduction was achieved in the UV/H_(2)O_(2)process,and the higest removal rate even reached to 83%.UV/TiO_(2)and UV/PS processes can only decrease the specific THMFP of HPI.The specific AOXFP of HPO,TPI and HPI fractions were all able to be degraded by the three UV-based AOPs,and HPO content is more susceptible to decompose than TPI and HPI content.UV/H_(2)O_(2)was found to be the most effective treatment for the removal of THMFP and AOXFP under given conditions.C1 (microbial or marine derived humic-like substances),C_(2) (terrestrially derived humic-like substances)and C_(3) (tryptophan-like proteins) fluorescent components of HPO fraction were fairly labile across the UV-based AOPs treatment.C_(3) of each fraction of NOM was the most resistant to degrade upon the UV-based AOPs.Results from this study may provide the prediction about the consequence of UV-based AOPs for the degradation of different fractions of NOM with varied characteristics.
基金the National Natural Science Foundation of China(No.91851110)Guangzhou University’s 2017 Training Program for Young Top-Notch Personnels(No.BJ201713)+1 种基金Scientific Research Project of Guangzhou University(No.YK2020017)Guizhou Provincial Department of Education Youth Science and Technology Talents Growth Project(No.KY[2017]300)。
文摘This study evaluated the removal of multiple pollutants,i.e.,polybrominated diphenyl ethers(PBDEs),novel halogenated flame retardants(HFRs),sulfonamide antibiotics(SAs),and heavy metals(HMs),by a fullscale reversed A^(2)/O process in a sewage treatment plant(STP)in Guangzhou,China.The reversed A^(2)/O process demonstrated high removal efficiencies(REs)for total PBDEs(60.5%±4.3%),novel HFRs(98.4%±2.8%)and HMs(70.1%±1.2%),and a relatively low RE for SAs(25.0%±2.3%).BDE 209,the dominant PBDE congener,showed a high residual concentration(13.41±5.18 ng/L)in the suspended particulate matter(SPM)of treated effluents.So me novel HFRs,dechlorane plus(DP)and decabromodiphe nyl ethane(DBDPE),were detected in the SPM of the raw sewage(7.50±4.14 ng/L and 11.52±11.65 ng/L,respectively).The removal ofSAs was mainly through biodegradation in the activated sludge bioreactors(ASBs).Ofthe HMs,Mn and Ni exhibited the lowest REs(47.5%±2.2%and 35.0%±2.6%,respectively),while Cr and Cu showed the highest removal(REs>80%).In terms of treatment units in the reversed A^(2)/O process,ASBs showed the highest RE(27.8%)for the multiple pollutants.The information can aid in our understanding of removal properties of STPs on various pollutants and evaluating the ecological/health risks of STPs as point pollutant sources.
基金the National Natural Science Foundation of China(No.21973070,No.21474076,No.21674082,and No.11875205)。
文摘Multinanoparticles interacting with the phospholipid membranes in solution were studied by dissipative particle dynamics simulation.The selected nanoparticles have spherical or cylindrical shapes,and they have various initial velocities in the dynamical processes.Several translocation modes are defined according to their characteristics in the dynamical processes,in which the phase diagrams are constructed based on the interaction strengths between the particles and membranes and the initial velocities of particles.Furthermore,several parameters,such as the system energy and radius of gyration,are investigated in the dynamical processes for the various translocation modes.Results elucidate the effects of multiparticles interacting with the membranes in the biological processes.
基金financially supported by the National Natural Science Founda-tion of China(Grant number:42371107)the Project Supported by State Key Laboratory of Earth Surface Processes and Resource Ecology(2022-TS-03)
文摘Background Seasonal freeze-thaw(FT)processes alter soil formation and cause changes in soil microbial communi-ties,which regulate the decomposition of organic matter in alpine ecosystems.Soil aggregates are basic structural units and play a critical role in microbial habitation.However,the impact of seasonal FT processes on the distribution of microbial communities associated with soil pores in different aggregate fractions under climate change has been overlooked.In this study,we sampled soil aggregates from two typical alpine ecosystems(alpine meadow and alpine shrubland)during the seasonal FT processes(UFP:unstable freezing period,SFP:stable frozen period,UTP:unstable thawing period and STP:stable thawed period).The phospholipid fatty acid(PLFA)method was used to determine the biomass of living microbes in different aggregate fractions.Results The microbial biomass of 0.25–2 mm and 0.053–0.25 mm aggregates did not change significantly dur-ing the seasonal FT process while the microbial biomass of>2 mm aggregates presented a significant difference between the STP and UTP.Bacterial communities dominated the microbes in aggregates,accounting for over 80%of the total PLFAs.The microbial communities of soil aggregates in the surface layer were more sensitive to the sea-sonal FT process than those in other soil layers.In the thawing period,Gram positive bacteria(GP)was more dominant.In the freezing period,the ratio of Gram-positive to Gram-negative bacterial PLFAs(GP/GN)was low because the enrichment of plant litter facilitated the formation of organic matter.In the freezing process,pores of 30–80μm(mesopores)favored the habitation of fungal and actinobacterial communities while total PLFAs and bacterial PLFAs were negatively correlated with mesopores in the thawing process.Conclusions The freezing process caused a greater variability in microbial biomass of different aggregate fractions.The thawing process increased the differences in microbial biomass among soil horizons.Mesopores of aggregates supported the habitation of actinobacterial and fungal communities while they were not conducive to bacterial growth.These findings provide a further comprehension of biodiversity and accurate estimation of global carbon cycle.
基金financially supported by the National Natural Science Foundation of China(22176059,21777042,and 22076045)the authors would also like to acknowledge support from the Science and Technology Commission of Shanghai Municipality’s Yangfan Special Project(23YF1408400)the Fundamental Research Funds for the Central Universities.
文摘Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB4200500)National Natural Science Foundation of China(NSFC,22379101 and 22422904)Sichuan Natural Science Foundation(2024NSFSC0001 and 2025ZNSFSC0960).
文摘Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.Layer‐by‐layer(LbL)processing with a p–i–n configuration offers an innovative solution by enabling precise control over donor–acceptor distribution and interfacial characteristics.Here,we systematically investigate nine halogen‐functionalized additives across three categories—methyl halides,thiophene halides,and benzene halides—for optimizing LbL device performance.These additives,distinguished by their diverse thermal properties and solid–liquid transformation capabilities below 100°C,are functionalized as both nucleation centers and morphology‐modulating plasticizers during thermal treatment.Among them,2‐bromo‐5‐iodothiophene(BIT)demonstrates superior performance through synergistic effects of its bromine–iodine combination and thiophene core in mediating donor–acceptor interactions.LbL devices processed with BIT achieve exceptional metrics in the PM6/L8‐BO system,including a open‐circuit voltage of 0.916 V,a short‐circuit current density of 27.12 mA cm−2,and an fill factor of 80.97%,resulting in an impressive power conversion efficiency of 20.12%.This study establishes a molecular design strategy for halogen‐functionalized additives that simultaneously optimizes both donor and acceptor layers while maintaining processing simplicity for potential industrial applications.
文摘A research team led by Dr.GE Ziyi from the Ningbo Institute of Materials Technology and Engineering(NIMTE)of the Chinese Academy of Sciences has developed novel giant acceptors with an oxygenated linker,enabling the creation of highly efficient non-halogen-processed organic solar cells(OSCs),with a power conversion efficiency(PCE)up to 20.02%.
文摘Existing organic halide synthesis routes typically employ elemental halogens(X_(2),X=Cl or Br),leading to low atom economy and significant environmental pollution.In this work,we developed an atom efficient electrosynthesis and separation strategy for halogenation reagents—N-chlorosuccinimide(NCS)and N-bromosuccinimide(NBS)—at high current densities.Faradic efficiency(FE)of 91.0%and 81.3%was achieved for NCS and NBS generation on RuO_(x)/TiO_(2)/Ti in a batch cell,respectively.Electrosynthesis of NCS likely involves both heterogeneous catalytic and homogeneous tandem pathways,while NBS is likely formed in a Langmuir-Hinshelwood mechanism with a proton-coupled electron transfer as the rate-determining step.A coupled continuous electrocatalytic synthesis and in situ separation setup was developed for the efficient production of NCS and NBS,which yielded 0.77 g of NCS in 12000 s and 0.81 g of NBS in 15000 s,both with relative purity exceeding 95%.The halogenation of acetone using NCS and NBS enabled gram-scale production of the key intermediate in organic synthesis,1-halogenacetone,with over 95%recovery of succinimide.
