Inefficient photo-carrier separation and sluggish photoreaction dynamics appreciably undermine the photocatalytic decontamination efficacy of photocatalysts.Herein,an S-scheme Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)heterojunc...Inefficient photo-carrier separation and sluggish photoreaction dynamics appreciably undermine the photocatalytic decontamination efficacy of photocatalysts.Herein,an S-scheme Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)heterojunction with interfacial Mo-S chemical bond is designed as an efficient photocatalyst.In this integrated photosystem,Bi2MoO6 and Mn_(0.5)Cd_(0.5)S function as oxidation and reduction centers of Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)microspheres,respectively.Importantly,the unique charge transfer mechanism in the chemically bonded S-scheme heterojunction with Mo-S bond as atom-scale charge transport highway effectively inhibits the photocorrosion of Mn_(0.5)Cd_(0.5)S and the recombination of photo-generated electron-hole pairs,endowing Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)photocatalyst with excellent photocatalytic decontamination performance and stability.Besides,integration of Mn_(0.5)Cd_(0.5)S nanocrystals into Bi2MoO6 improves hydrophilicity,conducive to the photoreactions.Strikingly,compared with Mn_(0.5)Cd_(0.5)S and Bi2MoO6,the Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)unveils much augmented photoactivity in tetracycline eradication,among which Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)-2 possesses the highest activity with the rate constant up to 0.0323 min-1,prominently outperforming other counterparts.This research offers a chemical bonding engineering combining with S-scheme heterojunction strategy for constructing extraordinary photocatalysts for environmental purification.展开更多
Devising robust S-scheme photocatalysts is of central importance for achieving high-efficient micropollu-tant decontamination.However,the conscious optimization of S-scheme system with high performance remains a prime...Devising robust S-scheme photocatalysts is of central importance for achieving high-efficient micropollu-tant decontamination.However,the conscious optimization of S-scheme system with high performance remains a prime challenge.Herein,carbon quantum dots(CDs)and Mn_(0.5)Cd_(0.5)S(MCS)are mounted on BiOBr(BOB)microspheres,establishing an advanced S-scheme heterojunction with interfacial Bi-S bond.The interfacial Bi-S bonds function as superb channels at atomic-scale to abate the energy barrier for S-scheme charge transportation.Meanwhile,CDs serve as electron collectors to preserve highly reductive electrons from MCS,further augmenting the spatial separation of photo-carriers.Therefore,the optimized CDs/MCS/BOB(MBC)heterojunction manifests significantly strengthened tetracycline hydrochloride(TC)destruction activity and its reaction rate constant is approximately 3.1,2.2,2.1,and 1.5 folds that than that of MCS,BOB,BOB/CDs and MCS/BOB.In addition,MBC exhibits high stability and significant resistance to environmental interferences.The toxicology evaluation confirms the effective abatement of toxicity of TC after treatment.This achievement demonstrates the benefits of CDs-optimized S-scheme photosystems with chemical bonds for photocatalytic water decontamination.展开更多
Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution.In this work,a chemic...Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution.In this work,a chemically bonded Mn0.5Cd_(0.5)S/BiOBr S-scheme heterostructure with oxygen vacancies is ingeniously developed through a facile in-situ solvothermal synthesis.The designed Mn0.5Cd_(0.5)S/BiOBr heterojunction exhibits eminently reinforced photo-activity for destruction of tetracycline hydrochloride and Cr(VI)as compared with its individual components.This substantial photo-redox performance amelioration is benefitted from the creation of an intense internal electric field(IEF)via supplying powerful driving force and migration highway by interfacial chemical bond to foster the S-scheme electron/hole disintegration.More intriguingly,the IEF at the hetero-interface drives the fast consumption of the photo-induced holes in Mn0.5Cd_(0.5)S by the photoelectrons from BiOBr,profoundly boosting the enrichment of active photo-carriers and sparing the photo-corrosion of Mn0.5Cd_(0.5)S.Furthermore,Mn0.5Cd_(0.5)S/BiOBr with exceptional anti-interference property can work efficiently in real water matrices.Multiple uses of the recycled Mn0⋅5Cd0⋅5S/BiOBr evidence its prominent robustness and stability.This achievement indicates the vast potential of chemically bonded S-scheme photosystems with structural defects in the design of photo-responsive materials for effective wastewater treatment.展开更多
N^(6)-methyldeoxyadenosine(6 mdA) modification is considered as a new epigenetic mark that may play important roles in various biological processes.However,it remains unclear about the effect of 6 mdA on DNA replicati...N^(6)-methyldeoxyadenosine(6 mdA) modification is considered as a new epigenetic mark that may play important roles in various biological processes.However,it remains unclear about the effect of 6 mdA on DNA replication in human cells.Herein,we combined next-generation sequencing with shuttle vector technology to explore how 6 mdA affects the efficiency and accuracy of DNA replication in human cells.Our results showed that 6 mdA neither blocked DNA replication nor induced mutations in human cells.Moreover,we found that the depletion of translesion synthesis DNA polymerase(Pol) κ,Pol η,Pol ι or Pol ζ did not significantly change the biological consequences of 6 mdA during replication in human cells.The negligible impact of 6 mdA on DNA replication is consistent with its potential role in epigenetic gene expression.展开更多
DNA methylation represents a major type of DNA modifications that play key roles in diverse biological processes.With the recent development of highly selective and sensitive bioanalytical techniques,N^(6)-methyladeni...DNA methylation represents a major type of DNA modifications that play key roles in diverse biological processes.With the recent development of highly selective and sensitive bioanalytical techniques,N^(6)-methyladenine(6mA)has been characterized as an important internal DNA modification dynamically occurring in multiple eukaryotes including humans.Increasing evidence has indicated that 6mA may act as a novel epigenetic modification involved in regulation of development,stress response and diseases such as cancer and neurodegenerative disorders.We review herein the recent advances in the detection and functional studies of 6mA modification,with special emphasis on its biological consequences and human health relevance as well as its dynamic regulation by various types of methyltransferases,demethylases and 6mA-binding proteins.It can be envisaged that further chemical and biological studies of 6mA modification will lead to a better understanding about its potentially important roles in normal and pathological biological processes.展开更多
Recent studies have shown that CTP may act as a ligand to regulate the activity of its target proteins in many biological processes.However,proteome-wide identification of CTP-binding proteins remains challenging.Here...Recent studies have shown that CTP may act as a ligand to regulate the activity of its target proteins in many biological processes.However,proteome-wide identification of CTP-binding proteins remains challenging.Here,we employed a biotinylated CTP affinity probe coupled with stable isotope labeling by amino acids in cell culture(SILAC)-based quantitative proteomics approach to capture,identify and quantify CTP-binding proteins in human cells.By performing two types of competitive SILAC experiments with high vs.low concentrations of CTP probe(100 vs.10µmol/L)or with CTP probe in the presence of free CTP,we identified 90 potential CTP-binding proteins which are involved in a variety of biological processes,including protein folding,nucleotide binding and cell-cell adhesion.Together,we developed a chemical proteomic method for uncovering the CTP-binding proteins in human cells,which could be widely applicable for profiling CTP-binding proteins in other biological samples.展开更多
N1-methyladenosine(m1A)is an important RNA modification that functions in various biological processes by interacting with cellular proteins.However,the binding proteins of N1-methyldeoxyadenosine(1mdA)in DNA remain l...N1-methyladenosine(m1A)is an important RNA modification that functions in various biological processes by interacting with cellular proteins.However,the binding proteins of N1-methyldeoxyadenosine(1mdA)in DNA remain largely unknown.Herein,we employed a quantitative proteomics strategy to identify the potential binding proteins of 1mdA in human cells.Our results revealed that serine–threonine kinase receptor-associated protein(STRAP)can bind to 1mdA-carrying DNA.We further demonstrated that STRAP participates in alkylating agent-induced DNA damage response and can promote the repair of 1mdA embedded in DNA.Moreover,we investigated the effects of STRAP on 1mdA-induced perturbation in transcription using a shuttle vector-and next-generation sequencing-based assay,and found that STRAP is involved in the transcriptional bypass of 1mdA in human cells.Together,our study revealed STRAP as a novel 1mdA-binding protein in human cells and provided new insight into the biological implications of STRAP and 1mdA modification in human diseases.展开更多
Living cells are constantly threatened by endogenous and environmental agents that can induce various DNA lesions including 8-oxoguanine(8-oxoG).Increasing evidence has suggested that 8-oxoG is not only a biomarker of...Living cells are constantly threatened by endogenous and environmental agents that can induce various DNA lesions including 8-oxoguanine(8-oxoG).Increasing evidence has suggested that 8-oxoG is not only a biomarker of oxidative stress,but also a novel epigenetic-like modification involved in transcriptional regulation in mammalian cells.Measurement of DNA damage and repair is useful for both basic research and clinical applications,but current methods for 8-oxoG detection still suffer from some problems such as poor selectivity,time consuming and being expensive.Here,we developed a fast and simple biosensing approach for quantitative analysis of 8-oxoG in DNA,which was based on the selective chemical biotinylation of 8-oxoG in conjunction with biotin-streptavidin enzyme-linked immunosorbent assay.We have also successfully applied this method to achieve efficient detection of the repair activities of DNA glycosylases Fpg and hOGG1 toward 8-oxoG in vitro and in human cells.This newly developed biosensing assay should be generally applicable for rapid detection of 8-oxoG and its repair in other organisms.展开更多
文摘Inefficient photo-carrier separation and sluggish photoreaction dynamics appreciably undermine the photocatalytic decontamination efficacy of photocatalysts.Herein,an S-scheme Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)heterojunction with interfacial Mo-S chemical bond is designed as an efficient photocatalyst.In this integrated photosystem,Bi2MoO6 and Mn_(0.5)Cd_(0.5)S function as oxidation and reduction centers of Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)microspheres,respectively.Importantly,the unique charge transfer mechanism in the chemically bonded S-scheme heterojunction with Mo-S bond as atom-scale charge transport highway effectively inhibits the photocorrosion of Mn_(0.5)Cd_(0.5)S and the recombination of photo-generated electron-hole pairs,endowing Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)photocatalyst with excellent photocatalytic decontamination performance and stability.Besides,integration of Mn_(0.5)Cd_(0.5)S nanocrystals into Bi2MoO6 improves hydrophilicity,conducive to the photoreactions.Strikingly,compared with Mn_(0.5)Cd_(0.5)S and Bi2MoO6,the Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)unveils much augmented photoactivity in tetracycline eradication,among which Mn_(0.5)Cd_(0.5)S/Bi_(2)MoO_(6)-2 possesses the highest activity with the rate constant up to 0.0323 min-1,prominently outperforming other counterparts.This research offers a chemical bonding engineering combining with S-scheme heterojunction strategy for constructing extraordinary photocatalysts for environmental purification.
基金supported by the NSFC-Zhejiang Joint Fund for Integration of Industrialization and Diversification(No.U1809214)the Natural Science Foundation of Zhejiang Province(Nos.LTGN23E080001 and LY20E080014)+1 种基金the Science and Technology Project of Zhoushan(No.2022C41011)the National Natural Science Foundation of China(No.22201251).
文摘Devising robust S-scheme photocatalysts is of central importance for achieving high-efficient micropollu-tant decontamination.However,the conscious optimization of S-scheme system with high performance remains a prime challenge.Herein,carbon quantum dots(CDs)and Mn_(0.5)Cd_(0.5)S(MCS)are mounted on BiOBr(BOB)microspheres,establishing an advanced S-scheme heterojunction with interfacial Bi-S bond.The interfacial Bi-S bonds function as superb channels at atomic-scale to abate the energy barrier for S-scheme charge transportation.Meanwhile,CDs serve as electron collectors to preserve highly reductive electrons from MCS,further augmenting the spatial separation of photo-carriers.Therefore,the optimized CDs/MCS/BOB(MBC)heterojunction manifests significantly strengthened tetracycline hydrochloride(TC)destruction activity and its reaction rate constant is approximately 3.1,2.2,2.1,and 1.5 folds that than that of MCS,BOB,BOB/CDs and MCS/BOB.In addition,MBC exhibits high stability and significant resistance to environmental interferences.The toxicology evaluation confirms the effective abatement of toxicity of TC after treatment.This achievement demonstrates the benefits of CDs-optimized S-scheme photosystems with chemical bonds for photocatalytic water decontamination.
基金supported by the National Natural Science Foundation of China(U1809214)the Natural Science Foundation of Zhejiang Province(LY20E080014 and LTGN23E080001)the Science and Technology Project of Zhoushan(2022C41011).
文摘Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution.In this work,a chemically bonded Mn0.5Cd_(0.5)S/BiOBr S-scheme heterostructure with oxygen vacancies is ingeniously developed through a facile in-situ solvothermal synthesis.The designed Mn0.5Cd_(0.5)S/BiOBr heterojunction exhibits eminently reinforced photo-activity for destruction of tetracycline hydrochloride and Cr(VI)as compared with its individual components.This substantial photo-redox performance amelioration is benefitted from the creation of an intense internal electric field(IEF)via supplying powerful driving force and migration highway by interfacial chemical bond to foster the S-scheme electron/hole disintegration.More intriguingly,the IEF at the hetero-interface drives the fast consumption of the photo-induced holes in Mn0.5Cd_(0.5)S by the photoelectrons from BiOBr,profoundly boosting the enrichment of active photo-carriers and sparing the photo-corrosion of Mn0.5Cd_(0.5)S.Furthermore,Mn0.5Cd_(0.5)S/BiOBr with exceptional anti-interference property can work efficiently in real water matrices.Multiple uses of the recycled Mn0⋅5Cd0⋅5S/BiOBr evidence its prominent robustness and stability.This achievement indicates the vast potential of chemically bonded S-scheme photosystems with structural defects in the design of photo-responsive materials for effective wastewater treatment.
基金supported by the National Natural Science Foundation of China (Nos. 21807030, 21907028)the Science and Technology Innovation Program of Hunan Province(No. 2019RS2020)+1 种基金Natural Science Foundation of Hunan Province(No. 2020JJ5046)the Fundamental Research Funds for the Central Universities (Nos. 531118010061, 531118010259)。
文摘N^(6)-methyldeoxyadenosine(6 mdA) modification is considered as a new epigenetic mark that may play important roles in various biological processes.However,it remains unclear about the effect of 6 mdA on DNA replication in human cells.Herein,we combined next-generation sequencing with shuttle vector technology to explore how 6 mdA affects the efficiency and accuracy of DNA replication in human cells.Our results showed that 6 mdA neither blocked DNA replication nor induced mutations in human cells.Moreover,we found that the depletion of translesion synthesis DNA polymerase(Pol) κ,Pol η,Pol ι or Pol ζ did not significantly change the biological consequences of 6 mdA during replication in human cells.The negligible impact of 6 mdA on DNA replication is consistent with its potential role in epigenetic gene expression.
基金supported by the National Natural Science Foun-dation of China(Nos.21807030,21907028)the Science and Tech-nology Innovation Program of Hunan Province(No.2019RS2020),Natural Science Foundation of Hunan Province(No.2020JJ5046)the Fundamental Research Funds for the Central Universities(Nos.531118010061,531118010259).
文摘DNA methylation represents a major type of DNA modifications that play key roles in diverse biological processes.With the recent development of highly selective and sensitive bioanalytical techniques,N^(6)-methyladenine(6mA)has been characterized as an important internal DNA modification dynamically occurring in multiple eukaryotes including humans.Increasing evidence has indicated that 6mA may act as a novel epigenetic modification involved in regulation of development,stress response and diseases such as cancer and neurodegenerative disorders.We review herein the recent advances in the detection and functional studies of 6mA modification,with special emphasis on its biological consequences and human health relevance as well as its dynamic regulation by various types of methyltransferases,demethylases and 6mA-binding proteins.It can be envisaged that further chemical and biological studies of 6mA modification will lead to a better understanding about its potentially important roles in normal and pathological biological processes.
基金supported by the National Natural Science Foundation of China(Nos.21807030,21907028)the Science and Technology Innovation Program of Hunan Province(No.2019RS2020)+1 种基金Natural Science Foundation of Hunan Province(No.2020JJ5046)the Fundamental Research Funds for the Central Universities(Nos.531118010061,531118010259).
文摘Recent studies have shown that CTP may act as a ligand to regulate the activity of its target proteins in many biological processes.However,proteome-wide identification of CTP-binding proteins remains challenging.Here,we employed a biotinylated CTP affinity probe coupled with stable isotope labeling by amino acids in cell culture(SILAC)-based quantitative proteomics approach to capture,identify and quantify CTP-binding proteins in human cells.By performing two types of competitive SILAC experiments with high vs.low concentrations of CTP probe(100 vs.10µmol/L)or with CTP probe in the presence of free CTP,we identified 90 potential CTP-binding proteins which are involved in a variety of biological processes,including protein folding,nucleotide binding and cell-cell adhesion.Together,we developed a chemical proteomic method for uncovering the CTP-binding proteins in human cells,which could be widely applicable for profiling CTP-binding proteins in other biological samples.
基金supported by the National Natural Science Foundation of China(Nos.21907028 and 21807030)Natural Science Foundation of Hunan Province(No.2023JJ30119)+1 种基金the Science and Technology Innovation Program of Hunan Province(No.2019RS2020)the Fundamental Research Funds for the Central Universities(Nos.531118010061 and 531118010259)。
文摘N1-methyladenosine(m1A)is an important RNA modification that functions in various biological processes by interacting with cellular proteins.However,the binding proteins of N1-methyldeoxyadenosine(1mdA)in DNA remain largely unknown.Herein,we employed a quantitative proteomics strategy to identify the potential binding proteins of 1mdA in human cells.Our results revealed that serine–threonine kinase receptor-associated protein(STRAP)can bind to 1mdA-carrying DNA.We further demonstrated that STRAP participates in alkylating agent-induced DNA damage response and can promote the repair of 1mdA embedded in DNA.Moreover,we investigated the effects of STRAP on 1mdA-induced perturbation in transcription using a shuttle vector-and next-generation sequencing-based assay,and found that STRAP is involved in the transcriptional bypass of 1mdA in human cells.Together,our study revealed STRAP as a novel 1mdA-binding protein in human cells and provided new insight into the biological implications of STRAP and 1mdA modification in human diseases.
基金This work was supported by the National Natural Science Foundation of China(Nos.21907028,21807030)the Science and Technology Innovation Programof Hunan Province(No.2019RS2020)+1 种基金the Special Funds for the Construction of Innovative Provinces in Hunan Province(No.2019RS1031)the Fundamental Research Funds for the Central Universities(Nos.531118010061,531118010259).
文摘Living cells are constantly threatened by endogenous and environmental agents that can induce various DNA lesions including 8-oxoguanine(8-oxoG).Increasing evidence has suggested that 8-oxoG is not only a biomarker of oxidative stress,but also a novel epigenetic-like modification involved in transcriptional regulation in mammalian cells.Measurement of DNA damage and repair is useful for both basic research and clinical applications,but current methods for 8-oxoG detection still suffer from some problems such as poor selectivity,time consuming and being expensive.Here,we developed a fast and simple biosensing approach for quantitative analysis of 8-oxoG in DNA,which was based on the selective chemical biotinylation of 8-oxoG in conjunction with biotin-streptavidin enzyme-linked immunosorbent assay.We have also successfully applied this method to achieve efficient detection of the repair activities of DNA glycosylases Fpg and hOGG1 toward 8-oxoG in vitro and in human cells.This newly developed biosensing assay should be generally applicable for rapid detection of 8-oxoG and its repair in other organisms.
