Adsorption is one of the most effective technologies in the treatment of colored matter containing wastewater. Graphene related composites display potential to be an effective adsorbent. However, the adsorption mechan...Adsorption is one of the most effective technologies in the treatment of colored matter containing wastewater. Graphene related composites display potential to be an effective adsorbent. However, the adsorption mechanism and their regeneration approach are still demanding more efforts. An effective magnetically separable absorbent, Fe3O4 and reduced graphene oxide(RGO) composite has been prepared by an in situ coprecipitation and reduction method. According to the characterizations of TEM, XRD, XPS, Raman spectra and BET analyses, Fe3O4 nanoparticles in sizes of 10-20 nm are well dispersed over the RGO nanosheets, resulting in a highest specific area of 296.2 m2/g. The rhodamine B adsorption mechanism on the composites was investigated by the adsorption kinetics and isotherms. The isotherms are fitting better by Langmuir model, and the adsorption kinetic rates depend much on the chemical components of RGO. Compared to active carbon, the composite shows 3.7 times higher adsorption capacity and thirty times faster adsorption rates. Furthermore,with Fe3O4 nanoparticles as the in situ catalysts, the adsorption performance of composites can be restored by carrying out a Fenton-like reaction, which could be a promising regeneration way for the adsorbents in the organic pollutant removal of wastewater.展开更多
Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized...Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.展开更多
An efficient visible light driven photocatalyst, gold nanoparticles(NPs) modified Bi VO_4(Au/Bi VO_4), has been synthesized by deposition-precipitation with urea method. Au/Bi VO_4 exhibits enhanced photocatalytic act...An efficient visible light driven photocatalyst, gold nanoparticles(NPs) modified Bi VO_4(Au/Bi VO_4), has been synthesized by deposition-precipitation with urea method. Au/Bi VO_4 exhibits enhanced photocatalytic activity for phenol degradation underλ>400 nm irradiation but negligible activity underλ>535 nm,indicating that the surface plasmon resonance(SPR) effect is too weak for organic photodegradation. According to the photoelectrochemical results of the porous powder electrodes of Bi VO_4 and Au/Bi VO_4, the SPR effect of Au NPs has been assessed. The role of Au NPs as electron sinks or sources, which is controllable by incident photon energy and applied potentials, has been discussed.展开更多
In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performa...In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performance without introducing alien elements.This minireview analyzes the latestprogress in engineering vacancies in photocatalysts,remarks on state‐of‐the‐art characterizationtechniques for vacancies,and reviews the formation chemistry and fundamental benefits of anionand cation vacancies in typical photocatalysts.Although knowledge of these vacancies is increasing,challenges remain in this field,and possible further research is therefore also discussed.展开更多
Catalyst recovery is one of the most important aspects that restrict the application of Ti O_2 photocatalyst. In order to reduce restrictions and improve the photocatalytic efficiency, a hierarchical porous Ti O_2 mon...Catalyst recovery is one of the most important aspects that restrict the application of Ti O_2 photocatalyst. In order to reduce restrictions and improve the photocatalytic efficiency, a hierarchical porous Ti O_2 monolith(PTM) with well-defined macroporous and homogeneous mesoporous structure was prepared by using a sol-gel phase separation method. P123 was used as the mesoporous template and graphene oxide was applied to increase the activity and integrity of the monolithic Ti O_2. According to scanning electron microscopy and the Barrett-Joyner-Halenda measurements, PTM_3 is mainly composed of 10 nm anatase crystallines with3.6 nm mesopores and 2-8 μm macropores. Further characterization suggests carbon and nitrogen have been maintained in the PTM during calcinations so as to induce the visible light activity. The PTM with 0.07 wt%graphene oxide dosage shows high efficiency for methyl orange(MO) decolorization under both full spectrum and visible light irradiation(λ >400 nm). Besides, the monolith remains intact and has good photocatalytic stability after four cyclic experiments.展开更多
Although humic acid(HA)can inhibit TiO2photocatalysis,it can sensitize TiO2and induce significant visible‐light(VL)activity in phenol degradation.This favorable effect of HA was negligible on phosphate‐modified TiO...Although humic acid(HA)can inhibit TiO2photocatalysis,it can sensitize TiO2and induce significant visible‐light(VL)activity in phenol degradation.This favorable effect of HA was negligible on phosphate‐modified TiO2(P‐TiO2),but significantly stronger on Nafion‐modified TiO2(Nf‐TiO2).The reaction rate constants for phenol degradation on Nf‐TiO2increased from(0.003±0.001)to(0.025±0.003)min?1when the reaction was performed in the presence of20mg/L HA.The different effects of HA on P‐TiO2and Nf‐TiO2photocatalysis cannot be attributed to adsorption changes,because the adsorption capacities of P‐TiO2and Nf‐TiO2were only slightly lower than that of TiO2at an initial HA concentration of20mg/mL.Scavenger tests,electron paramagnetic resonance spectroscopy,and H2O2detection were taken to understand the low VL activity of the P‐TiO2/HA suspension.The main active species for phenol degradation in the TiO2and Nf‐TiO2suspensions were superoxide radicals.There were negligible amounts of superoxide radicals in the P‐TiO2/HA suspension,possibly because a direct four‐electron oxygen reduction reaction occurred.The better VL activity of Nf‐TiO2was rationalized on the basis of Mott–Schottky and electrochemical impedance plots.Nafion modification resulted in cathodic shifts of the energy band positions,increased electron density,and less resistance to electron transfer across the interface between TiO2and electrolytes.All these factors facilitated electron transfer and improved the production of active species.Phosphate modification therefore did not improve the VL response of HA sensitized TiO2,and low concentrations of HA can facilitate VL photocatalytic degradation of organic pollutants on Nafion surface‐modified TiO2.展开更多
The rapid aggregation and sedimentation,the high toxicity towards bacteria,and the passivation of surfaces hinder the application of zero-valent iron(ZVI)particles in groundwater remediation.To overcome the shortages,...The rapid aggregation and sedimentation,the high toxicity towards bacteria,and the passivation of surfaces hinder the application of zero-valent iron(ZVI)particles in groundwater remediation.To overcome the shortages,ZVI particles were modified using oxalic acid(an environmental-friendly low-molecular-weight organic acid)together with xanthan gum(a safe and cost-effective high-molecular-weight polymer).We found that ZVI modified with both oxalic acid and xanthan gum exhibited superior Cr(VI)removal performance than those modified solely with oxalic acid and unmodified ZVI.Due to the reduced Fe^(2+) release,the toxicity towards Escherichia coli by oxalic acid-xanthan gum modified ZVI was greatly inhibited.Via enhancing electrostatic repulsion through increasing the negative zeta potentials,modification of ZVI by oxalic acid and xanthan gum improved the dispersion of ZVI and reduced their sedimentation in suspension.Moreover,the mobile performance of ZVI in porous media was greatly improved by the modification with oxalic acid and xanthan gum due to the enhanced electrostatic repulsive interaction between ZVI and quartz sand.The observations held true in actual groundwater samples without and with heavy metal contamination.Clearly,the modification of ZVI by using oxalic acid and xanthan gum could be a feasible approach to enhance the practical application potential for the in-situ decontamination of groundwater.展开更多
Hydrogen peroxide(H_(2)O_(2))photosynthesis from H_(2)O and O_(2)remains a significant challenge due to the sluggish hydrogen donation process,which stems from the high O-H bond dissociation energy of water.In this st...Hydrogen peroxide(H_(2)O_(2))photosynthesis from H_(2)O and O_(2)remains a significant challenge due to the sluggish hydrogen donation process,which stems from the high O-H bond dissociation energy of water.In this study,we propose an effective strategy to accelerate the water oxidation reaction(WOR)by anchoring single palladium atoms(Pd-CNO_(2))onto a keto-anthraquinone covalent organic framework(KfAQ-Pd),achieving remarkable H_(2)O_(2)production rates of 3828μmol h^(-1)g^(-1)under visible light irradiation(λ>420 nm)in neutral water.Both experimental observations and theoretical simulations reveal that the Pd-CNO_(2)configuration induces an upward shift in the d-band center and enhances the hydrophilicity of KfAQ.This modification effectively disrupts the hydrogen-bond network within adsorbed water clusters,thereby promoting the cleavage of the dangling O-H bonds in H_(2)O molecules and facilitating efficient hydrogen donation.The generated H_3O~+species are subsequently reduced insitu by photogenerated electrons,leading to the hydrogenation of anthraquinone moieties and ultimately driving efficient H_(2)O_(2)photosynthesis.Overall,these findings highlight the pivotal role of single Pd atoms in enhancing water dissociation and hydrogen transfer,offering a promising new paradigm for solardriven,environmentally friendly H_(2)O_(2)synthesis in neutral aqueous systems.展开更多
Existing strategies for bone defect repair are difficult to monitor.Smart scaffold materials that can quantify the efficiency of new bone formation are important for bone regeneration and monitoring.Carbon nanotubes(C...Existing strategies for bone defect repair are difficult to monitor.Smart scaffold materials that can quantify the efficiency of new bone formation are important for bone regeneration and monitoring.Carbon nanotubes(CNT)have promising bioactivity and electrical conductivity.In this study,a noninvasive and intelligent monitoring scaffold was prepared for bone regeneration and monitoring by integrating carboxylated CNT into chemically cross-linked carboxymethyl chitosan hydrogel.CNT scaffold(0.5%w/v)demonstrated improved mechanical properties with good biocompatibility and electrochemical responsiveness.Cyclic voltammetry and electrochemical impedance spectroscopy of CNT scaffold responded sensitively to seed cell differentiation degree in both cellular and animal levels.Interestingly,the CNT scaffold could make up the easy deactivation shortfall of bone morphogenetic protein 2 by sustainably enhancing stem cell osteogenic differentiation and new bone tissue formation through CNT roles.This research provides new ideas for the development of noninvasive and electrochemically responsive bioactive scaffolds,marking an important step in the development of intelligent tissue engineering.展开更多
The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,end...The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference ability.Among many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands out.Yet,the activation process often relies on transition metals,suffering from low atom utilization.Here we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen degradation.We highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN.Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions predominating.Notably,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic.The proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite activation.This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.展开更多
Developing visible light responsive(VLR)TiO_(2) photocatalysts is essential and attractive for the consideration of solar energy utilization.A large amount of work have shown TiO_(2) modified with several nonmetal ele...Developing visible light responsive(VLR)TiO_(2) photocatalysts is essential and attractive for the consideration of solar energy utilization.A large amount of work have shown TiO_(2) modified with several nonmetal elements having VLR performance,although according to DFT calculation,Asahi denied the VLR properties of fluorine,carbon,etc.in doping TiO_(2).Therefore,the origins of VLR activity desire further delicate discussion.In this mini-review,several strategies for VLR TiO_(2) modification have been introduced,including N doping or B/N codoping,surface modification with sensitizing matter such as carbonaceous or other organic substances,surface alkoxyls modification via a ligand-to-metal charge transfer(LMCT)process,and enhanced dye sensitization by fluorine modification.Besides doping,there are much more approaches to fabricate VLR TiO_(2) modified with nonmetal elements.However,it is still in demand to explore new methods to obtain more stable and efficient VLR TiO_(2) for practical application.展开更多
In Fenton-like reactions,high-valent cobalt-oxo(Co^(IV)=O)has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the electron re...In Fenton-like reactions,high-valent cobalt-oxo(Co^(IV)=O)has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the electron repulsion between the electron rich oxo-and cobalt centers.Here,we demonstrate Co^(IV)=O generation from peroxymonosulfate(PMS)activation over cobalt single-atom catalysts(Co-SACs)using in-situ Co K-edge X-ray absorption spectra,and discern that Co^(IV)=O generation is dependent on the support work-function(WF)due to the strong electronic metal-support interaction(EMSI).Supports with a high WF value like anatase-TiO_(2)facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Cod electrons,thus decreasing the generation barrier for the critical intermediate(Co-OOSO_(3)^(2-)).The Co atoms anchored on anatase-TiO_(2)(Co-TiO_(2))exhibited enhanced Co^(IV)=O generation and superior activity for sulfamethoxazole(SMX)degradation during PMS activation.The normalized steady-state concentration of Co^(IV)=O in Co-TiO_(2)/PMS system was three orders of magnitude higher than that of free radicals,and 1.3-to 11-fold higher than that generated in other Co-SACs/PMS systems.Co-TiO_(2)/PMS sustained efficient removal of SMX with minimal Co^(2+)leaching under continuous flow operation,suggesting its attractive water purification potential.Overall,these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.展开更多
基金financially supported by National Natural Science Foundation of China (No. 21377084)Shanghai Municipal Natural Science Foundation (No. 13ZR1421000)
文摘Adsorption is one of the most effective technologies in the treatment of colored matter containing wastewater. Graphene related composites display potential to be an effective adsorbent. However, the adsorption mechanism and their regeneration approach are still demanding more efforts. An effective magnetically separable absorbent, Fe3O4 and reduced graphene oxide(RGO) composite has been prepared by an in situ coprecipitation and reduction method. According to the characterizations of TEM, XRD, XPS, Raman spectra and BET analyses, Fe3O4 nanoparticles in sizes of 10-20 nm are well dispersed over the RGO nanosheets, resulting in a highest specific area of 296.2 m2/g. The rhodamine B adsorption mechanism on the composites was investigated by the adsorption kinetics and isotherms. The isotherms are fitting better by Langmuir model, and the adsorption kinetic rates depend much on the chemical components of RGO. Compared to active carbon, the composite shows 3.7 times higher adsorption capacity and thirty times faster adsorption rates. Furthermore,with Fe3O4 nanoparticles as the in situ catalysts, the adsorption performance of composites can be restored by carrying out a Fenton-like reaction, which could be a promising regeneration way for the adsorbents in the organic pollutant removal of wastewater.
基金financially support by an Australian Research Council (ARC) Discovery Project (No. DP200100965)a Griffith University Postdoctoral Fellowship
文摘Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.
基金financially supported by National Natural Science Foundation of China(No.20907031)the SSRF pro ject(No.10sr0175)Natural Science Foundation of Shanghai(No.09ZR1414800)
文摘An efficient visible light driven photocatalyst, gold nanoparticles(NPs) modified Bi VO_4(Au/Bi VO_4), has been synthesized by deposition-precipitation with urea method. Au/Bi VO_4 exhibits enhanced photocatalytic activity for phenol degradation underλ>400 nm irradiation but negligible activity underλ>535 nm,indicating that the surface plasmon resonance(SPR) effect is too weak for organic photodegradation. According to the photoelectrochemical results of the porous powder electrodes of Bi VO_4 and Au/Bi VO_4, the SPR effect of Au NPs has been assessed. The role of Au NPs as electron sinks or sources, which is controllable by incident photon energy and applied potentials, has been discussed.
基金supported by the National Natural Science Foundation of China (21377084)Special Fund for Agro-scientific Research in the Public Interest (201503107)~~
文摘In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performance without introducing alien elements.This minireview analyzes the latestprogress in engineering vacancies in photocatalysts,remarks on state‐of‐the‐art characterizationtechniques for vacancies,and reviews the formation chemistry and fundamental benefits of anionand cation vacancies in typical photocatalysts.Although knowledge of these vacancies is increasing,challenges remain in this field,and possible further research is therefore also discussed.
基金financially supported by the National Natural Science Foundation of China (No. 20907031)
文摘Catalyst recovery is one of the most important aspects that restrict the application of Ti O_2 photocatalyst. In order to reduce restrictions and improve the photocatalytic efficiency, a hierarchical porous Ti O_2 monolith(PTM) with well-defined macroporous and homogeneous mesoporous structure was prepared by using a sol-gel phase separation method. P123 was used as the mesoporous template and graphene oxide was applied to increase the activity and integrity of the monolithic Ti O_2. According to scanning electron microscopy and the Barrett-Joyner-Halenda measurements, PTM_3 is mainly composed of 10 nm anatase crystallines with3.6 nm mesopores and 2-8 μm macropores. Further characterization suggests carbon and nitrogen have been maintained in the PTM during calcinations so as to induce the visible light activity. The PTM with 0.07 wt%graphene oxide dosage shows high efficiency for methyl orange(MO) decolorization under both full spectrum and visible light irradiation(λ >400 nm). Besides, the monolith remains intact and has good photocatalytic stability after four cyclic experiments.
基金supported by the National Natural Science Foundation of China(21377084)Special Fund for Agro-Scientific Research in the Public Interest(201503107)Shanghai Municipal International Cooperation Foundation(15230724600)~~
文摘Although humic acid(HA)can inhibit TiO2photocatalysis,it can sensitize TiO2and induce significant visible‐light(VL)activity in phenol degradation.This favorable effect of HA was negligible on phosphate‐modified TiO2(P‐TiO2),but significantly stronger on Nafion‐modified TiO2(Nf‐TiO2).The reaction rate constants for phenol degradation on Nf‐TiO2increased from(0.003±0.001)to(0.025±0.003)min?1when the reaction was performed in the presence of20mg/L HA.The different effects of HA on P‐TiO2and Nf‐TiO2photocatalysis cannot be attributed to adsorption changes,because the adsorption capacities of P‐TiO2and Nf‐TiO2were only slightly lower than that of TiO2at an initial HA concentration of20mg/mL.Scavenger tests,electron paramagnetic resonance spectroscopy,and H2O2detection were taken to understand the low VL activity of the P‐TiO2/HA suspension.The main active species for phenol degradation in the TiO2and Nf‐TiO2suspensions were superoxide radicals.There were negligible amounts of superoxide radicals in the P‐TiO2/HA suspension,possibly because a direct four‐electron oxygen reduction reaction occurred.The better VL activity of Nf‐TiO2was rationalized on the basis of Mott–Schottky and electrochemical impedance plots.Nafion modification resulted in cathodic shifts of the energy band positions,increased electron density,and less resistance to electron transfer across the interface between TiO2and electrolytes.All these factors facilitated electron transfer and improved the production of active species.Phosphate modification therefore did not improve the VL response of HA sensitized TiO2,and low concentrations of HA can facilitate VL photocatalytic degradation of organic pollutants on Nafion surface‐modified TiO2.
基金supported by the National Key Research and Development Program of China(Grant Nos.2023YFC3708001,2022YFC3702103)the National Natural Science Foundation of China(Grant No.42025706)。
文摘The rapid aggregation and sedimentation,the high toxicity towards bacteria,and the passivation of surfaces hinder the application of zero-valent iron(ZVI)particles in groundwater remediation.To overcome the shortages,ZVI particles were modified using oxalic acid(an environmental-friendly low-molecular-weight organic acid)together with xanthan gum(a safe and cost-effective high-molecular-weight polymer).We found that ZVI modified with both oxalic acid and xanthan gum exhibited superior Cr(VI)removal performance than those modified solely with oxalic acid and unmodified ZVI.Due to the reduced Fe^(2+) release,the toxicity towards Escherichia coli by oxalic acid-xanthan gum modified ZVI was greatly inhibited.Via enhancing electrostatic repulsion through increasing the negative zeta potentials,modification of ZVI by oxalic acid and xanthan gum improved the dispersion of ZVI and reduced their sedimentation in suspension.Moreover,the mobile performance of ZVI in porous media was greatly improved by the modification with oxalic acid and xanthan gum due to the enhanced electrostatic repulsive interaction between ZVI and quartz sand.The observations held true in actual groundwater samples without and with heavy metal contamination.Clearly,the modification of ZVI by using oxalic acid and xanthan gum could be a feasible approach to enhance the practical application potential for the in-situ decontamination of groundwater.
基金supported by the National Natural Science Foundation of China(22206125 and 22376138)the Fundamental Research Funds for the Central Universities(2682025CX064)。
文摘Hydrogen peroxide(H_(2)O_(2))photosynthesis from H_(2)O and O_(2)remains a significant challenge due to the sluggish hydrogen donation process,which stems from the high O-H bond dissociation energy of water.In this study,we propose an effective strategy to accelerate the water oxidation reaction(WOR)by anchoring single palladium atoms(Pd-CNO_(2))onto a keto-anthraquinone covalent organic framework(KfAQ-Pd),achieving remarkable H_(2)O_(2)production rates of 3828μmol h^(-1)g^(-1)under visible light irradiation(λ>420 nm)in neutral water.Both experimental observations and theoretical simulations reveal that the Pd-CNO_(2)configuration induces an upward shift in the d-band center and enhances the hydrophilicity of KfAQ.This modification effectively disrupts the hydrogen-bond network within adsorbed water clusters,thereby promoting the cleavage of the dangling O-H bonds in H_(2)O molecules and facilitating efficient hydrogen donation.The generated H_3O~+species are subsequently reduced insitu by photogenerated electrons,leading to the hydrogenation of anthraquinone moieties and ultimately driving efficient H_(2)O_(2)photosynthesis.Overall,these findings highlight the pivotal role of single Pd atoms in enhancing water dissociation and hydrogen transfer,offering a promising new paradigm for solardriven,environmentally friendly H_(2)O_(2)synthesis in neutral aqueous systems.
基金supported by the National Natural Science Foundation of China(81972530,62171275,82000879)the National Key R&D Project(2018YFC1106100 and 2018YFC1106101)+1 种基金Fund for Excellent Young Scholars of Shanghai Ninth People’s Hospital,Shanghai Jiao Tong University School of Medicine(JYYQ001)the Science and Technology Commission of Shanghai(20DZ2270800).
文摘Existing strategies for bone defect repair are difficult to monitor.Smart scaffold materials that can quantify the efficiency of new bone formation are important for bone regeneration and monitoring.Carbon nanotubes(CNT)have promising bioactivity and electrical conductivity.In this study,a noninvasive and intelligent monitoring scaffold was prepared for bone regeneration and monitoring by integrating carboxylated CNT into chemically cross-linked carboxymethyl chitosan hydrogel.CNT scaffold(0.5%w/v)demonstrated improved mechanical properties with good biocompatibility and electrochemical responsiveness.Cyclic voltammetry and electrochemical impedance spectroscopy of CNT scaffold responded sensitively to seed cell differentiation degree in both cellular and animal levels.Interestingly,the CNT scaffold could make up the easy deactivation shortfall of bone morphogenetic protein 2 by sustainably enhancing stem cell osteogenic differentiation and new bone tissue formation through CNT roles.This research provides new ideas for the development of noninvasive and electrochemically responsive bioactive scaffolds,marking an important step in the development of intelligent tissue engineering.
基金Financial support from the National Natural Science Foundation of China(52270068)the open Project of the State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(QG202225)+1 种基金the Heilongjiang Touyan Innovation Team Program was highly appreciatedWe would also like to thank Dr.Shibo Xi of Singapore Synchrotron Light Source for his help in catalyst characterization.
文摘The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference ability.Among many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands out.Yet,the activation process often relies on transition metals,suffering from low atom utilization.Here we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen degradation.We highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN.Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions predominating.Notably,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic.The proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite activation.This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.
基金This work was supported by the National Natural Science Foundation of China(Grant No.20907031)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Dong Hua University(Grant No.LK0907)the Specialized Research Fund for the Doctoral Program of Higher Education(Grant No.20090073120042).
文摘Developing visible light responsive(VLR)TiO_(2) photocatalysts is essential and attractive for the consideration of solar energy utilization.A large amount of work have shown TiO_(2) modified with several nonmetal elements having VLR performance,although according to DFT calculation,Asahi denied the VLR properties of fluorine,carbon,etc.in doping TiO_(2).Therefore,the origins of VLR activity desire further delicate discussion.In this mini-review,several strategies for VLR TiO_(2) modification have been introduced,including N doping or B/N codoping,surface modification with sensitizing matter such as carbonaceous or other organic substances,surface alkoxyls modification via a ligand-to-metal charge transfer(LMCT)process,and enhanced dye sensitization by fluorine modification.Besides doping,there are much more approaches to fabricate VLR TiO_(2) modified with nonmetal elements.However,it is still in demand to explore new methods to obtain more stable and efficient VLR TiO_(2) for practical application.
基金supported by the National Natural Science Foundation of China(22376138 and 52070128)the National Key R&D Program of China(2023YFC3708005)National Science Foundation Engineering Research Centers on Nanotechnology-Enabled Water Treatment(EEC-1449500)。
文摘In Fenton-like reactions,high-valent cobalt-oxo(Co^(IV)=O)has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the electron repulsion between the electron rich oxo-and cobalt centers.Here,we demonstrate Co^(IV)=O generation from peroxymonosulfate(PMS)activation over cobalt single-atom catalysts(Co-SACs)using in-situ Co K-edge X-ray absorption spectra,and discern that Co^(IV)=O generation is dependent on the support work-function(WF)due to the strong electronic metal-support interaction(EMSI).Supports with a high WF value like anatase-TiO_(2)facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Cod electrons,thus decreasing the generation barrier for the critical intermediate(Co-OOSO_(3)^(2-)).The Co atoms anchored on anatase-TiO_(2)(Co-TiO_(2))exhibited enhanced Co^(IV)=O generation and superior activity for sulfamethoxazole(SMX)degradation during PMS activation.The normalized steady-state concentration of Co^(IV)=O in Co-TiO_(2)/PMS system was three orders of magnitude higher than that of free radicals,and 1.3-to 11-fold higher than that generated in other Co-SACs/PMS systems.Co-TiO_(2)/PMS sustained efficient removal of SMX with minimal Co^(2+)leaching under continuous flow operation,suggesting its attractive water purification potential.Overall,these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.
