Successfully generating reactive oxygen species(ROS)in a targeted and efficient manner for the detoxification of chlorinated organic pollutants(CPs)is a significant and demanding challenge.Herein,we present an in-situ...Successfully generating reactive oxygen species(ROS)in a targeted and efficient manner for the detoxification of chlorinated organic pollutants(CPs)is a significant and demanding challenge.Herein,we present an in-situ photoreduction strategy to fabricate a composite of palladium(Pd)nanoparticles anchored few-layer carbon nitride nanosheets(Pd-CN).This innovative Pd-CN is then leveraged to activate peroxymonosulfate(PMS)in pursuit of our objective.The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen,thereby aiding in the cleavage of the O-O bond.This process generates crucial intermediates,including adsorbed hydroxyl radicals(*OH)and adsorbed atomic oxygen(O*),which are essential for the production of ^(1)O_(2).Consequently,the Pd-CN catalyst demonstrates strong preference for ^(1)O_(2) generation during the PMS activation process,successfully degrading over 95%of pollutants such as 4-chlorophenol(4-CP),2,4-dichlorophenol(2,4-DCP),and 2,4,6-trichlorophenol(2,4,6-TCP)within just 20 min.Additionally,the catalyst exhibits total organic carbon(TOC)removal rates ranging from 49.4%to 31.4%,while the rates for de-chlorination fall between 68.6%and 72.7%.A subsequent continuous-flow treatment experiment has confirmed the application potential of this system,demonstrating consistent catalytic activity for up to 8 h.This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.展开更多
Objectives:Photodynamic therapy(PDT)is a minimally invasive method used in the treatment of various cancers and skin diseases,but it is not widely used in bone cancer,where the current therapy is often not effective a...Objectives:Photodynamic therapy(PDT)is a minimally invasive method used in the treatment of various cancers and skin diseases,but it is not widely used in bone cancer,where the current therapy is often not effective and accompanied by side effects.Alternative and more effective therapies like PDT are needed.In this in-vitro study,the effect of the photosensitizer(PS)chlorin e6(Ce6)on cancerous bone tumor cells using PDT was examined.Methods:A total of 27 tissue specimens from patients with primary bone cancers or bone metastases of different origins were genetically characterized and treated with PDT.Following a 24-h incubation,cell viability was determined,and the effect of PDT on cell migration was analyzed over 48 h.Results:We could demonstrate that the effect on proliferation of PDT in combination with the PS Ce6 was best in cells isolated from primary osteosarcoma and in bone metastases from mammary carcinomas.Besides proliferation,PDT was also effective in inhibiting the migration of these cells.A statistically significant correlation between the PDT effect and CD164 gene expression was detected,indicating that a high expression of this gene could result in a higher effectiveness of the photodynamic treatment.Conclusion:This study analyzes for the first time the effect of PDT in bone cancers and metastases and shows the potential of treating these cancer types with Ce6 PDT.展开更多
This study utilizes wet/dry cyclic corrosion testing combined with corrosion big data technology to investigate the mechanism by which chloride ions(Cl^(-))influence the corrosion behavior of 650 MPa high-strength low...This study utilizes wet/dry cyclic corrosion testing combined with corrosion big data technology to investigate the mechanism by which chloride ions(Cl^(-))influence the corrosion behavior of 650 MPa high-strength low-alloy(HSLA)steel in industrially polluted environments.The corrosion process of 650 MPa HSLA steel occurred in two distinct stages:an initial corrosion stage and a stable corrosion stage.During the initial phase,the weight loss rate increased rapidly owing to the instability of the rust layer.Notably,this study demonstrated that 650 MPa HSLA steel exhibited superior corrosion resistance in Cl-containing environments.The formation of a corrosion-product film eventually reduced the weight-loss rate.However,the intrusion of Cl^(-)at increasing concentrations gradually destabilized theα/γ^(*)phases of the rust layer,leading to a looser structure and lower polarization resistance(R_(p)).The application of corrosion big data technology in this study facilitated the validation and analysis of the experimental results,offering new insights into the corrosion mechanisms of HSLA steel in chloride-rich environments.展开更多
Co_(3)O_(4) is a promising catalyst for the chlorine evolution reaction(CER)in seawater;however,its CER selectivity is compromised by the adsorption of the competitive oxygen evolution reaction intermediate(OH^(-))at ...Co_(3)O_(4) is a promising catalyst for the chlorine evolution reaction(CER)in seawater;however,its CER selectivity is compromised by the adsorption of the competitive oxygen evolution reaction intermediate(OH^(-))at Co sites.Inspired by the hard-soft acid-base(HSAB)theory,this study proposes incorporating early transition metal sites(V)with a low degree of electron delocalization into Co_(3)O_(4) to modulate the selective adsorption of reactants on catalytic sites.Experimental and theoretical calculations reveal that V incorporation facilitates the electron accumulation at the Co site,significantly strengthening the interaction between Co and Cl^(-).Meanwhile,the loss of electrons from V sites generates a more localized electronic state that preferentially adsorbs OH^(-),thus reducing the Co-OH interaction and releasing more Co sites for Cl^(-)adsorption.Therefore,Co_(2)VO_(4) exhibits a high CER selectivity of 92.3%and maintains one of the highest stabilities over 300 h in natural seawater.The resulting half-flow cell achieves~100%disinfection efficiency in seawater,validating the HSAB theory-based design strategy and offering new guidance for developing highly selective seawater CER catalysts.展开更多
Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g...Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.展开更多
基金supported by the Natural Science Foundation of Hebei Province(No.B2024203026)the Yanzhao Golden Platform Talent Project(Education Platform)of Hebei Province(No.HJYB202517)+1 种基金the National Natural Science Foundation of China(Nos.U22A20403,22006128)the Open Foundation of MOE Key Laboratory of Resources and Environmental System Optimization,College of Environmental Science and Engineering,North China Electric Power University(No.KLRE-KF202308).
文摘Successfully generating reactive oxygen species(ROS)in a targeted and efficient manner for the detoxification of chlorinated organic pollutants(CPs)is a significant and demanding challenge.Herein,we present an in-situ photoreduction strategy to fabricate a composite of palladium(Pd)nanoparticles anchored few-layer carbon nitride nanosheets(Pd-CN).This innovative Pd-CN is then leveraged to activate peroxymonosulfate(PMS)in pursuit of our objective.The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen,thereby aiding in the cleavage of the O-O bond.This process generates crucial intermediates,including adsorbed hydroxyl radicals(*OH)and adsorbed atomic oxygen(O*),which are essential for the production of ^(1)O_(2).Consequently,the Pd-CN catalyst demonstrates strong preference for ^(1)O_(2) generation during the PMS activation process,successfully degrading over 95%of pollutants such as 4-chlorophenol(4-CP),2,4-dichlorophenol(2,4-DCP),and 2,4,6-trichlorophenol(2,4,6-TCP)within just 20 min.Additionally,the catalyst exhibits total organic carbon(TOC)removal rates ranging from 49.4%to 31.4%,while the rates for de-chlorination fall between 68.6%and 72.7%.A subsequent continuous-flow treatment experiment has confirmed the application potential of this system,demonstrating consistent catalytic activity for up to 8 h.This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.
文摘Objectives:Photodynamic therapy(PDT)is a minimally invasive method used in the treatment of various cancers and skin diseases,but it is not widely used in bone cancer,where the current therapy is often not effective and accompanied by side effects.Alternative and more effective therapies like PDT are needed.In this in-vitro study,the effect of the photosensitizer(PS)chlorin e6(Ce6)on cancerous bone tumor cells using PDT was examined.Methods:A total of 27 tissue specimens from patients with primary bone cancers or bone metastases of different origins were genetically characterized and treated with PDT.Following a 24-h incubation,cell viability was determined,and the effect of PDT on cell migration was analyzed over 48 h.Results:We could demonstrate that the effect on proliferation of PDT in combination with the PS Ce6 was best in cells isolated from primary osteosarcoma and in bone metastases from mammary carcinomas.Besides proliferation,PDT was also effective in inhibiting the migration of these cells.A statistically significant correlation between the PDT effect and CD164 gene expression was detected,indicating that a high expression of this gene could result in a higher effectiveness of the photodynamic treatment.Conclusion:This study analyzes for the first time the effect of PDT in bone cancers and metastases and shows the potential of treating these cancer types with Ce6 PDT.
基金financially supported by the National Natural Science Foundation of China(Nos.52104319 and 52374323)。
文摘This study utilizes wet/dry cyclic corrosion testing combined with corrosion big data technology to investigate the mechanism by which chloride ions(Cl^(-))influence the corrosion behavior of 650 MPa high-strength low-alloy(HSLA)steel in industrially polluted environments.The corrosion process of 650 MPa HSLA steel occurred in two distinct stages:an initial corrosion stage and a stable corrosion stage.During the initial phase,the weight loss rate increased rapidly owing to the instability of the rust layer.Notably,this study demonstrated that 650 MPa HSLA steel exhibited superior corrosion resistance in Cl-containing environments.The formation of a corrosion-product film eventually reduced the weight-loss rate.However,the intrusion of Cl^(-)at increasing concentrations gradually destabilized theα/γ^(*)phases of the rust layer,leading to a looser structure and lower polarization resistance(R_(p)).The application of corrosion big data technology in this study facilitated the validation and analysis of the experimental results,offering new insights into the corrosion mechanisms of HSLA steel in chloride-rich environments.
基金supported by the Guangxi Science and Technology Program(2023AB38061)the National Natural Science Foundation of China(22162004,22479031)the High-performance Computing Platform of Guangxi University。
文摘Co_(3)O_(4) is a promising catalyst for the chlorine evolution reaction(CER)in seawater;however,its CER selectivity is compromised by the adsorption of the competitive oxygen evolution reaction intermediate(OH^(-))at Co sites.Inspired by the hard-soft acid-base(HSAB)theory,this study proposes incorporating early transition metal sites(V)with a low degree of electron delocalization into Co_(3)O_(4) to modulate the selective adsorption of reactants on catalytic sites.Experimental and theoretical calculations reveal that V incorporation facilitates the electron accumulation at the Co site,significantly strengthening the interaction between Co and Cl^(-).Meanwhile,the loss of electrons from V sites generates a more localized electronic state that preferentially adsorbs OH^(-),thus reducing the Co-OH interaction and releasing more Co sites for Cl^(-)adsorption.Therefore,Co_(2)VO_(4) exhibits a high CER selectivity of 92.3%and maintains one of the highest stabilities over 300 h in natural seawater.The resulting half-flow cell achieves~100%disinfection efficiency in seawater,validating the HSAB theory-based design strategy and offering new guidance for developing highly selective seawater CER catalysts.
基金supported by Natural Science Foundation of China(Nos.U23B20165 and 52170085)National Key R&D Program International Cooperation Project(No.2023YFE0108100)+1 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
