Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key appr...Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key approach to unlocking this potential.In this work,we construct a two-dimensional/twodimensional(2D/2D)FeSe_(2)/protonated carbon nitride(FeSe_(2)/PCN)heterostructure to promote the interfacial charge transfer dynamics,leading to a four-fold improved conversion efficiency of photocatalytic CO_(2)reduction with near 100%CO selectivity.Combining in situ X-ray photoelectron spectroscopy,in situ soft X-ray absorption spectroscopy,and femtosecond transient absorption spectroscopy,it is revealed that FeSe_(2)acts as an electron acceptor upon photoexcitation,introducing an additional electron transfer pathway from PCN to FeSe_(2)that suppresses radiative recombination and promotes charge transfer.In situ X-ray absorption fine structure spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy,and density functional theory calculation further unravel that the electron-enriched FeSe_(2)functions as the active sites for CO_(2)activation and significantly reduces the energy barrier of key intermediate COOH*formation,which is the rate-determined step for CO generation.This work underscores the importance of regulating photocarrier relaxation pathways to achieve effective spatial charge separation for promoted photocatalytic CO_(2)reduction and demonstrates the powerful functions of in situ spectroscopies in in-depth understanding of the photocatalytic mechanism.展开更多
Autoinducer 2（AI-2）, an important bioactive by-product of the Lux S-catalyzed S-ribosylhomocysteine cleavage reaction in the activated-methyl-cycle, has been suggested to serve as a universal intra- and inter-specie...Autoinducer 2（AI-2）, an important bioactive by-product of the Lux S-catalyzed S-ribosylhomocysteine cleavage reaction in the activated-methyl-cycle, has been suggested to serve as a universal intra- and inter-species signaling molecule. The development of reliable and sensitive methods for quantitative determination of AI-2 is highly desired.However, the chemical properties of AI-2 cause difficulty in its quantitative analysis.Herein, we report a high performance liquid chromatography-tandem mass spectrometric method that enables reproducible and sensitive measurement of AI-2 concentrations in complex matrixes. 4,5-Dimethylbenzene-1,2-diamine（DMBDM）, an easy-to-obtain commercial reagent, was used for the derivatization treatment. The assay was linear in the concentration range of 1.0–1000 ng/m L（R^2= 0.999） and had a lower limit of quantification of0.58 ng/m L. The method exhibited several advantages, e.g., high selectivity, wide linear response range, and good sensitivity. Furthermore, the effectiveness of the method was further validated through measuring AI-2 concentrations in the cell-free culture supernatant from Escherichia coli wild type.展开更多
Interactions between metals and activated sludge can substantially affect the fate and transport of heavy metals in wastewater treatment plants. Therefore, it is important to develop a simple, fast and efficient metho...Interactions between metals and activated sludge can substantially affect the fate and transport of heavy metals in wastewater treatment plants. Therefore, it is important to develop a simple, fast and efficient method to elucidate the interaction. In this study, a modified titration method with a dynamic mode was developed to investigate the binding of Cu（Ⅱ）, a typical heavy metal, onto aerobic granules. The titration results indicated that pH and ionic strength both had a positive effect on the biosorption capacity of the granular sludge. The/-XRF results demonstrated that the distribution of metals on the granular surface was heterogeneous, and Cu showed strong correlations and had the same ＂hot spots＂ positions with other metal ions （e.g., Ca, Mg, Fe etc.）. Ion exchange and complexing were the main mechanisms for the biosorption of Cu（Ⅱ） by aerobic granules. These results would be beneficial for better understanding of Cu（Ⅱ） migration and its fate in wastewater treatment plants.展开更多
There have been considerable investigations into the composition of the microbiota inhabiting various anatomical sites of the human body,including but not limited to the gut and skin.However,the distribution of the mi...There have been considerable investigations into the composition of the microbiota inhabiting various anatomical sites of the human body,including but not limited to the gut and skin.However,the distribution of the microbiota composition and functionality across anatomical sites within the same individual are not yetwell-established,in particular in relation with host health and disease.展开更多
The exact relationship between inflammatory bowel disease(IBD)and gut microbiota(GM)is still unclear.This study aimed to explore the cause-and-effect relationship between IBD and GM by Mendelian randomization analysis...The exact relationship between inflammatory bowel disease(IBD)and gut microbiota(GM)is still unclear.This study aimed to explore the cause-and-effect relationship between IBD and GM by Mendelian randomization analysis.The IBD data used in this study were obtained from Genome-Wide Association Studies.The GM data were from the Dutch Microbiome Project and included 207 taxa and 205 microbiota-associated pathways.Multivariate Mendelian randomization analysis was performed to investigate the relationship between GM and IBD.The results demonstrated that susceptibility to developing IBD is negatively correlated with class Clostridia(OR=0.80,P=0.003),family Sutterellacea(OR=0.87,P=0.014),genus Coprobacter(OR=0.90,P=0.009),order Clostridiales(OR=0.80,P=0.003),phylum Firmicutes(OR=0.82,P=0.002)and Coprobacter fastidiosus(OR=0.90,P=0.009).Conversely,the risk of developing IBD was positively correlated with the phosphopantothenate biosynthesis I pathway(OR=1.17,P=0.006),Bacteroides caccae(OR=1.14,P=0.021)and Bacteroides uniformis(OR=1.26,P=0.003).Reverse causality was found between the phosphopantothenate biosynthesis I pathway and IBD(OR=1.03,P=0.04),but not for the remaining specific GM taxa.In conclusion,our study demonstrated a causal relationship between specific GM features and IBD.展开更多
基金supported by the National Natural Science Foundation of China(12241502,92045301)Fundamental Research Funds for the Central Universities(20720220010)+7 种基金USTC Research Funds of the Double First-Class Initiative(YD2310002012)the Launching Special Funds of Scientific Research for Introduced Talents from University of Science and Technology of China(KY2310000060)National Key Research and Development Program of China(2019YFA0405602)Anhui Provincial Natural Science Foundation(2408085QB049)the Instruments Center for Physical Science and USTC Center for Micro and Nanoscale Research and Fabrication,University of Science and Technology of Chinathe solid supports from the BL03U,BL10B,and BL12B beamlines of the National Synchrotron Radiation Laboratory(NSRL,Hefei)the Shanghai Synchrotron Radiation Facility(SSRF,Shanghai)of BL11B(https://cstr.cn/31124.02.SSRF.BL11B)and BL14W1(https://cstr.cn/31124.02.SSRF.BL14W1)beamlines for the assistance on XAFS measurementsAnhui Chuangpu Instruments Co.,Ltd.for the assistance in the test of Table XAFS。
文摘Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key approach to unlocking this potential.In this work,we construct a two-dimensional/twodimensional(2D/2D)FeSe_(2)/protonated carbon nitride(FeSe_(2)/PCN)heterostructure to promote the interfacial charge transfer dynamics,leading to a four-fold improved conversion efficiency of photocatalytic CO_(2)reduction with near 100%CO selectivity.Combining in situ X-ray photoelectron spectroscopy,in situ soft X-ray absorption spectroscopy,and femtosecond transient absorption spectroscopy,it is revealed that FeSe_(2)acts as an electron acceptor upon photoexcitation,introducing an additional electron transfer pathway from PCN to FeSe_(2)that suppresses radiative recombination and promotes charge transfer.In situ X-ray absorption fine structure spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy,and density functional theory calculation further unravel that the electron-enriched FeSe_(2)functions as the active sites for CO_(2)activation and significantly reduces the energy barrier of key intermediate COOH*formation,which is the rate-determined step for CO generation.This work underscores the importance of regulating photocarrier relaxation pathways to achieve effective spatial charge separation for promoted photocatalytic CO_(2)reduction and demonstrates the powerful functions of in situ spectroscopies in in-depth understanding of the photocatalytic mechanism.
基金supported by the National Natural Science Foundation of China(Nos.21261160489,21207031 and51538011)the Program for Changjiang Scholars and Innovative Research Team in University,China
文摘Autoinducer 2（AI-2）, an important bioactive by-product of the Lux S-catalyzed S-ribosylhomocysteine cleavage reaction in the activated-methyl-cycle, has been suggested to serve as a universal intra- and inter-species signaling molecule. The development of reliable and sensitive methods for quantitative determination of AI-2 is highly desired.However, the chemical properties of AI-2 cause difficulty in its quantitative analysis.Herein, we report a high performance liquid chromatography-tandem mass spectrometric method that enables reproducible and sensitive measurement of AI-2 concentrations in complex matrixes. 4,5-Dimethylbenzene-1,2-diamine（DMBDM）, an easy-to-obtain commercial reagent, was used for the derivatization treatment. The assay was linear in the concentration range of 1.0–1000 ng/m L（R^2= 0.999） and had a lower limit of quantification of0.58 ng/m L. The method exhibited several advantages, e.g., high selectivity, wide linear response range, and good sensitivity. Furthermore, the effectiveness of the method was further validated through measuring AI-2 concentrations in the cell-free culture supernatant from Escherichia coli wild type.
基金The authors wish to thank the National Natural Science Foundation of China （Grant Nos. 51322802 and 21377123）, the Program for Changjiang Scholars and Innovative Research Team in University, and the Fundamental Research Funds for the Central Universities （WK2060190040 and WK3530000002） for the partial support of this study. Authors also wish to thank the Shanghai Synchrotron Radiation Facility, Shanghai, China for μ-XRF analysis.
文摘Interactions between metals and activated sludge can substantially affect the fate and transport of heavy metals in wastewater treatment plants. Therefore, it is important to develop a simple, fast and efficient method to elucidate the interaction. In this study, a modified titration method with a dynamic mode was developed to investigate the binding of Cu（Ⅱ）, a typical heavy metal, onto aerobic granules. The titration results indicated that pH and ionic strength both had a positive effect on the biosorption capacity of the granular sludge. The/-XRF results demonstrated that the distribution of metals on the granular surface was heterogeneous, and Cu showed strong correlations and had the same ＂hot spots＂ positions with other metal ions （e.g., Ca, Mg, Fe etc.）. Ion exchange and complexing were the main mechanisms for the biosorption of Cu（Ⅱ） by aerobic granules. These results would be beneficial for better understanding of Cu（Ⅱ） migration and its fate in wastewater treatment plants.
基金supported by the Fundamental Research Funds for the Central Universities(2022ZFJH003)Shandong Provincial Laboratory Project(SYS202202)+1 种基金Research Project of Jinan Microecological Biomedicine Shandong Laboratory(JNL-2022001A)Hangzhou Medical and Health Technology Project(B20200626).
文摘There have been considerable investigations into the composition of the microbiota inhabiting various anatomical sites of the human body,including but not limited to the gut and skin.However,the distribution of the microbiota composition and functionality across anatomical sites within the same individual are not yetwell-established,in particular in relation with host health and disease.
基金the Fundamental Research Funds for the Central Universities(2022ZFJH003)Shandong Provincial Laboratory Project(SYS202202)the Research Project of Jinan Microecological Biomedicine Shandong Laboratory(JNL-2022001A).
文摘The exact relationship between inflammatory bowel disease(IBD)and gut microbiota(GM)is still unclear.This study aimed to explore the cause-and-effect relationship between IBD and GM by Mendelian randomization analysis.The IBD data used in this study were obtained from Genome-Wide Association Studies.The GM data were from the Dutch Microbiome Project and included 207 taxa and 205 microbiota-associated pathways.Multivariate Mendelian randomization analysis was performed to investigate the relationship between GM and IBD.The results demonstrated that susceptibility to developing IBD is negatively correlated with class Clostridia(OR=0.80,P=0.003),family Sutterellacea(OR=0.87,P=0.014),genus Coprobacter(OR=0.90,P=0.009),order Clostridiales(OR=0.80,P=0.003),phylum Firmicutes(OR=0.82,P=0.002)and Coprobacter fastidiosus(OR=0.90,P=0.009).Conversely,the risk of developing IBD was positively correlated with the phosphopantothenate biosynthesis I pathway(OR=1.17,P=0.006),Bacteroides caccae(OR=1.14,P=0.021)and Bacteroides uniformis(OR=1.26,P=0.003).Reverse causality was found between the phosphopantothenate biosynthesis I pathway and IBD(OR=1.03,P=0.04),but not for the remaining specific GM taxa.In conclusion,our study demonstrated a causal relationship between specific GM features and IBD.
