Mesoporous silica hollow spheres with a homogenous and high content distribution of Fe and Co were synthesized by a facile one-pot hydrothermal process. The sub-nanometer bimetallic components inside the silica framew...Mesoporous silica hollow spheres with a homogenous and high content distribution of Fe and Co were synthesized by a facile one-pot hydrothermal process. The sub-nanometer bimetallic components inside the silica framework facilitate the stable fixation and the open accessibility to active sites. The co-doped Fe/Co in the spheres showed excellent peroxidase-like activity and much higher catalytic performance than their monometallic-supported spheres. The synergistic effect between Fe and Co promotes the continuous formation of functional radicals during the oxidation process and thus accelerates the reaction rate. When used for colorimetric detection of hydrogen peroxide(H_(2)O_(2)), the Fe/Co incorporated silica hollow spheres show the capability of detection of H_(2)O_(2) in a wide range(10-250 μmol/L) and with the low detection limit of 0.012 ppm.展开更多
Lateral two-dimensional(2D)heterostructures have great potential for device engineering at the atomistic scale.Their production is hindered by difficulties in obtaining atomically sharp interface free from intermixtur...Lateral two-dimensional(2D)heterostructures have great potential for device engineering at the atomistic scale.Their production is hindered by difficulties in obtaining atomically sharp interface free from intermixture.Here we report the continuous construction of a lateral heterostructure using blue phosphorene and tetrafluoro-tetracyanoquinodimethane(F_(4)TCNQ)as the building blocks.The lateral heterostructure is achieved by linking the semiconducting F_(4)TCNQ-Au metal organic framework and the metallic blue phosphorene-Au network via Au adatoms.The structural and electronic properties of the heterostructure have been investigated by means of scanning tunneling microscopy and spectroscopy(STM/S),complemented by density functional theory(DFT)calculations,demonstrating a structurally and electrically abrupt interface.Our approach offers the possibility of high flexibility and control that can be extended to other metal-organic species and 2D materials,establishing a foundation for the development of atomically thin in-plane superlattice and devices.展开更多
Fullerene assembling with specific donor molecules would yield multi-functional metamaterials via the collective behavior,wherein linear acenes are widely used as donor molecules to construct the charge‐transfer hete...Fullerene assembling with specific donor molecules would yield multi-functional metamaterials via the collective behavior,wherein linear acenes are widely used as donor molecules to construct the charge‐transfer heterojunction structure with fullerene.However,they are generally prepared by vacuum deposition due to the insoluble property of high‐performance linear acenes molecules in common solvents,which makes the construction of fullerene with insoluble donor molecules still be a big challenge in the solution‐processed method.To this end,chemical modification provides an effective solution‐processed strategy to construct donor and acceptor systems.Here,the C60‐pentacene is assembled into controllable flower‐like superstructures by the surface grafting method.It is found that the nanofeatures of the microflowers could be regulated by temperature,resulting in dense‐flakes morphology at room temperature and loose flakes at high temperatures.Furthermore,the dense‐flakes microflowers structures with less mass but better crystalline structure exhibit better optoelectronic properties.Our results reveal an effective control on the nanofeatures of the self‐assembled fullerenes complex super-structures and their role for the optoelectronic performance,which may promote the exploring of fullerene superstructures as photodetectors.展开更多
Fe-based metallic glasses (Fe–MGs) are potential candidate catalysts for advanced oxidation processes(AOPs) for recalcitrant organic pollutant degradation. However, industrial wastewater and natural contaminated site...Fe-based metallic glasses (Fe–MGs) are potential candidate catalysts for advanced oxidation processes(AOPs) for recalcitrant organic pollutant degradation. However, industrial wastewater and natural contaminated sites usually contain abundant inorganic ions, like the chloride ion (Cl−), which significantly affectAOPs, but their influence on MG-activated AOPs still remains unclear. Through the study of three commonly used oxidants, hydrogen peroxide (H_(2)O_(2)), peroxydisulfate (PDS), and peroxymonosulfate (PMS), theeffect of Cl− on the FeSiB-catalyzed process of degradation of the typical azo dye Orange Ⅱ was investigated. Evidence indicates that the addition of Cl− resulted in the monotonous inhibition of the degradation process when the H_(2)O_(2)/FeSiB and PDS/FeSiB systems were employed, but promoted effect wasdetected with the PMS/FeSiB system, which is different from the previously observed dual effect of Cl−.It is closely relative with FeSiB induced unique variety of degradation pathways, including radicals, nonradicals (^(1)O_(2)), and direct reduction degradation. Moreover, the presence of Cl− significantly affected thesystems’ absorbable organic halogen content and the amount of Fe leached into the solution. The resultsof this work will provide essential references for Fe-based MG used as AOP catalysts in field applicationsand the development of advanced MGs with excellent adaptability to complex environments.展开更多
TiO_(2)-based films are one of the most attractive photocatalysts owing to their highly cost-effective properties.Nevertheless,most TiO_(2)-based photocatalytic films for dye degradation are in the form of robust film...TiO_(2)-based films are one of the most attractive photocatalysts owing to their highly cost-effective properties.Nevertheless,most TiO_(2)-based photocatalytic films for dye degradation are in the form of robust films(without flexibility),TiO_(2)coatings on carbon matrix(with leakage risk),or surface-covered TiO_(2)hybrids(not favorite to contact with external molecules).Therefore,the development of durable and highly efficient TiO_(2)photocatalytic films for dye degradation is still needed.Here,we fabricated soft photocatalytic hybrid membranes(TANFs)from TiO_(2)nanotubes(Ti NT)and aramid nanofiber(ANF)by a facile vacuum filtration process.The similar morphology and dimension of Ti NT and ANF enable them intricately intertwine with each other in the membrane network.Under an appropriate mixing ratio,the TANF exhibited significantly improved optical and mechanical properties.When used for dye degradation,the membrane showed excellent photocatalytic performance and could keep stable activity and integrated state for repeated usage.展开更多
基金financial supports from the Instrument & Equipment Open Funding of Nanjing University of Science and TechnologyNational Natural Science Foundation of China (No. 21875108)the Fundamental Research Funds for the Central Universities (No. 30921013106)。
文摘Mesoporous silica hollow spheres with a homogenous and high content distribution of Fe and Co were synthesized by a facile one-pot hydrothermal process. The sub-nanometer bimetallic components inside the silica framework facilitate the stable fixation and the open accessibility to active sites. The co-doped Fe/Co in the spheres showed excellent peroxidase-like activity and much higher catalytic performance than their monometallic-supported spheres. The synergistic effect between Fe and Co promotes the continuous formation of functional radicals during the oxidation process and thus accelerates the reaction rate. When used for colorimetric detection of hydrogen peroxide(H_(2)O_(2)), the Fe/Co incorporated silica hollow spheres show the capability of detection of H_(2)O_(2) in a wide range(10-250 μmol/L) and with the low detection limit of 0.012 ppm.
基金This work is financially supported by the Natural Science Foundation of Jiangsu Province(No.BK20181297)the National Natural Science Foundation of China(Nos.21875108,21403282,and 51602155)the Fundamental Research Funds for Central Universities(Nos.30919011257,30917015106,and 30918011340)。
文摘Lateral two-dimensional(2D)heterostructures have great potential for device engineering at the atomistic scale.Their production is hindered by difficulties in obtaining atomically sharp interface free from intermixture.Here we report the continuous construction of a lateral heterostructure using blue phosphorene and tetrafluoro-tetracyanoquinodimethane(F_(4)TCNQ)as the building blocks.The lateral heterostructure is achieved by linking the semiconducting F_(4)TCNQ-Au metal organic framework and the metallic blue phosphorene-Au network via Au adatoms.The structural and electronic properties of the heterostructure have been investigated by means of scanning tunneling microscopy and spectroscopy(STM/S),complemented by density functional theory(DFT)calculations,demonstrating a structurally and electrically abrupt interface.Our approach offers the possibility of high flexibility and control that can be extended to other metal-organic species and 2D materials,establishing a foundation for the development of atomically thin in-plane superlattice and devices.
基金Beijing National Laboratory for Molecular Sciences,Grant/Award Number:BNLMS202006National Natural Science Foundation of China,Grant/Award Numbers:21875108,62004138+1 种基金Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20191289Instrument&Equipment Open Funding of Nanjing University of Science and Technology。
文摘Fullerene assembling with specific donor molecules would yield multi-functional metamaterials via the collective behavior,wherein linear acenes are widely used as donor molecules to construct the charge‐transfer heterojunction structure with fullerene.However,they are generally prepared by vacuum deposition due to the insoluble property of high‐performance linear acenes molecules in common solvents,which makes the construction of fullerene with insoluble donor molecules still be a big challenge in the solution‐processed method.To this end,chemical modification provides an effective solution‐processed strategy to construct donor and acceptor systems.Here,the C60‐pentacene is assembled into controllable flower‐like superstructures by the surface grafting method.It is found that the nanofeatures of the microflowers could be regulated by temperature,resulting in dense‐flakes morphology at room temperature and loose flakes at high temperatures.Furthermore,the dense‐flakes microflowers structures with less mass but better crystalline structure exhibit better optoelectronic properties.Our results reveal an effective control on the nanofeatures of the self‐assembled fullerenes complex super-structures and their role for the optoelectronic performance,which may promote the exploring of fullerene superstructures as photodetectors.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52101195,51871120)the Natural Science Foundation of Jiangsu Province(Nos.BK20190480,BK20200019)+1 种基金the Fundamental Research Funds for the Central Universities(Nos.30920021156,30920010004)the GuangdongHong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technology。
文摘Fe-based metallic glasses (Fe–MGs) are potential candidate catalysts for advanced oxidation processes(AOPs) for recalcitrant organic pollutant degradation. However, industrial wastewater and natural contaminated sites usually contain abundant inorganic ions, like the chloride ion (Cl−), which significantly affectAOPs, but their influence on MG-activated AOPs still remains unclear. Through the study of three commonly used oxidants, hydrogen peroxide (H_(2)O_(2)), peroxydisulfate (PDS), and peroxymonosulfate (PMS), theeffect of Cl− on the FeSiB-catalyzed process of degradation of the typical azo dye Orange Ⅱ was investigated. Evidence indicates that the addition of Cl− resulted in the monotonous inhibition of the degradation process when the H_(2)O_(2)/FeSiB and PDS/FeSiB systems were employed, but promoted effect wasdetected with the PMS/FeSiB system, which is different from the previously observed dual effect of Cl−.It is closely relative with FeSiB induced unique variety of degradation pathways, including radicals, nonradicals (^(1)O_(2)), and direct reduction degradation. Moreover, the presence of Cl− significantly affected thesystems’ absorbable organic halogen content and the amount of Fe leached into the solution. The resultsof this work will provide essential references for Fe-based MG used as AOP catalysts in field applicationsand the development of advanced MGs with excellent adaptability to complex environments.
基金the financial supports from the Instrument&Equipment Open Funding of Nanjing University of Science and TechnologyNational Natural Science Foundation of China(Nos.21875108 and 22105103)+3 种基金the Natural Science Foundation of Jiangsu Province(No.BK20200471)the Fundamental Research Funds for the Central Universities(No.30921013106)the technical cooperation project with Nantong Junjiang Material Science and Technology Co.,Ltd.(No.2022320104001955)the Key R&D Project of Shanxi Province(No.2022JBGS3–12)。
文摘TiO_(2)-based films are one of the most attractive photocatalysts owing to their highly cost-effective properties.Nevertheless,most TiO_(2)-based photocatalytic films for dye degradation are in the form of robust films(without flexibility),TiO_(2)coatings on carbon matrix(with leakage risk),or surface-covered TiO_(2)hybrids(not favorite to contact with external molecules).Therefore,the development of durable and highly efficient TiO_(2)photocatalytic films for dye degradation is still needed.Here,we fabricated soft photocatalytic hybrid membranes(TANFs)from TiO_(2)nanotubes(Ti NT)and aramid nanofiber(ANF)by a facile vacuum filtration process.The similar morphology and dimension of Ti NT and ANF enable them intricately intertwine with each other in the membrane network.Under an appropriate mixing ratio,the TANF exhibited significantly improved optical and mechanical properties.When used for dye degradation,the membrane showed excellent photocatalytic performance and could keep stable activity and integrated state for repeated usage.