Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis.However,the traditional problems such as high...Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis.However,the traditional problems such as high recombination rate of photogenerated carriers limit its application.In this work,we introduce nitrogen deficiency into g-C_(3)N_(4)to solve this problem a simple and safe in-situ reduction method.g-C_(3)N_(4)/CaCO_(3)was obtained by a simple and safe one-step calcination method with industrial-grade micron particles CaCO_(3).Cyano group modification was in-situ reduced during the thermal polymerization process,which would change the internal electronic structure of g-C_(3)N_(4).The successful combination of g-C_(3)N_(4)and CaCO_(3)and the introduction of cyanide have been proved by Fourier transform infrared spectroscopy and X-ray photoelectron spectrometer.The formation of the cyano group,an electron-absorbing group,promotes the effective separation of photogenic electron hole pairs and inhibits the recombination of photogenic carriers.These advantages result in the generation of more·O_(2)-and1O_(2)in the catalytic system,which increases the photocatalytic efficiency of nicotine degradation by ten times.Furthermore,the degradation process of nicotine has been studied in this work to provide a basis for the degradation of nicotine organic pollutants in the air.展开更多
Ti_(3)C_(2)T_(x)MXene fiber has shown extraordinary potential for supercapacitor electrode in wearable elec-tronics and textile energy storage,but realizing high energy density and practical-powered applications remai...Ti_(3)C_(2)T_(x)MXene fiber has shown extraordinary potential for supercapacitor electrode in wearable elec-tronics and textile energy storage,but realizing high energy density and practical-powered applications remains a great challenge.Here,we report a covalent-architected molybdenum disulfide-Ti_(3)C_(2)T_(x)(MoS_(2)-Ti_(3)C_(2)T_(x))core-shell fiber for high-performance supercapacitor.Benefiting from the microfluidic and micro-reaction strategies,the ordered MoS_(2)arrays are strongly bridged on Ti_(3)C_(2)T_(x)fiber via Ti-O-Mo bond,re-sulting in large exposed surface,enhanced porosity and excellent interfacial conduction for charges high diffusion and faradaic transfer.The MoS_(2)-Ti_(3)C_(2)T_(x)fiber exhibits ultra-large capacitance of 2028 F cm^(-3)and admirable reversibility in 1 M H_(2)SO_(4)aqueous electrolyte.Meanwhile,MoS_(2)-Ti_(3)C_(2)T_(x)fiber-based solid-state supercapacitor presents high energy density of 23.86 mWh cm^(-3),capacitance of 1073.6 F cm^(-3)and superior cycling ability of 92.13%retention after 20,000 cycles,which can realize stable energy supply for wearable watch,LEDs,electric fans,toy ship and self-powered devices.Our work may provide an insight-ful guidance for the advanced design of structural fiber towards robust new energy and next-generation wearable industry.展开更多
Microplastic pollution has become one of the most concerned focuses in the world.Among many treatment methods,photocatalysis is considered to be one of the most environmentally friendly methods.In this work,the photod...Microplastic pollution has become one of the most concerned focuses in the world.Among many treatment methods,photocatalysis is considered to be one of the most environmentally friendly methods.In this work,the photodegradation behavior of polyamide microplastics is studied by using polyamide 6(PA6)as model microplastics and FeCl_(3) as catalyst.It is hoped that the PA6 fiber can be effectively degraded by utilizing the strong oxidizing active species that can be produced after FeCl_(3) is irradiated in water.The results shows that PA6 fiber can be almost completely degraded after 10 days of irradiation in FeCl_(3) aqueous solution,indicating that it is promising to use this new method to solve the problem of PA6type microplastics.In addition,the chain scission mechanism and degradation process of PA6 are analyzed in detail by ultra-high performance liquid chromatography-tandem mass spectrometry(UPLC-MS),which provides a new insight for the study of polymer degradation mechanism.展开更多
The catalytic conversion of biomass platform chemicals using abundant non-noble metal nanocatalysts is a challenging topic.Here,high-density cobalt oxide nanoparticles loaded on biomass-derived porous N-doped carbon(N...The catalytic conversion of biomass platform chemicals using abundant non-noble metal nanocatalysts is a challenging topic.Here,high-density cobalt oxide nanoparticles loaded on biomass-derived porous N-doped carbon(NC)was fabricated by a tandem hydrothermal pyrolysis and mild nitrate decomposition process,which is a green and cheap preparation method.The Co_(3)O_(4) nanoparticles with the average size of 12 nm were uniformly distributed on the porous NC.The nanocomposites also possessed large surface area,high N content,good dispersibility in isopropanol,and furfural absorbability.Due to these characteristics,the novel cobalt nanocatalyst exhibited high catalytic activity for producing furfuryl alcohol,yielding 98.7%of the conversion and 97.1%of the selectivity at 160℃ for 6 h under 1 bar H2.The control experiments implied that both direct hydrogenation and transfer hydrogenation pathways co-existed in the hydrogenation reaction.The excellent catalytic activity of Co_(3)O_(4)@NC was attributed to the cooperative effects of porous NC and Co_(3)O_(4) nanoparticles.This approach provides a new idea to design effective high-density nonnoble metal oxide nanocatalysts for hydrogenation reactions,which can make full use of sustainable natural biomass.展开更多
In the research for the safe and efficiently antibacterial cotton fabrics to minimize risk for human health,an organic–inorganic hybrid material of ZnO nanoparticles(NPs)and quaternary ammonium salt(QAS)was employed ...In the research for the safe and efficiently antibacterial cotton fabrics to minimize risk for human health,an organic–inorganic hybrid material of ZnO nanoparticles(NPs)and quaternary ammonium salt(QAS)was employed to modify cotton fabrics by a dipping–padding–drying method.The synergistic effects of ZnO NPs and QAS on the structure and antibacterial properties of cotton fabrics were studied in detail.Results displayed that the QAS and ZnO NPs were immobilized firmly in cotton fabric by the formation of chemical covalent bonds and silica gel structure.ZnO/QAS/cotton had a good inhibitory effect on the growth of E.coli and S.aureus,with superior antibacterial efficiency of>99.99%.ZnO/QAS/cotton preserved good mechanical property,water absorbability,and limpness.We also provided a detailed analysis of antibacterial mechanism for the hybrid materials.The contact mechanism and the Zn2+release were considered as the main mechanisms for the ZnO/QAS/cotton,while the reactive oxygen species(ROS)generation only had a little contribution to the antibacterial activity.In short,the excellent integrated properties endowed the hybrid cotton fabrics as potential application in many fields,like healthcare,food packaging.展开更多
If a person comes into contact with pathogens on public facilities,there is a threat of contact(skin/wound)infections.More urgently,there are also reports about COVID-19 coronavirus contact infection,which once again ...If a person comes into contact with pathogens on public facilities,there is a threat of contact(skin/wound)infections.More urgently,there are also reports about COVID-19 coronavirus contact infection,which once again reminds that contact infection is a very easily overlooked disease exposure route.Herein,we propose an innovative implantation strategy to fabricate a multi-walled carbon nanotube/polyvinyl alcohol(MWCNT/PVA,MCP)interpenetrating interface to achieve flexibility,anti-damage,and non-contact sensing electronic skin(E-skin).Interestingly,the MCP E-skin had a fascinating non-contact sensing function,which can respond to the finger approaching 0−20 mm through the spatial weak field.This non-contact sensing can be applied urgently to human–machine interactions in public facilities to block pathogen.The scratches of the fruit knife did not damage the MCP E-skin,and can resist chemical corrosion after hydrophobic treatment.In addition,the MCP E-skin was developed to real-time monitor the respiratory and cough for exercise detection and disease diagnosis.Notably,the MCP E-skin has great potential for emergency applications in times of infectious disease pandemics.展开更多
Metal phthalocyanine has been extensively studied as a catalyst for degradation of carbamazepine(CBZ).However,metal phthalocyanine tends to undergo their own dimerization or polymerization,thereby reducing their activ...Metal phthalocyanine has been extensively studied as a catalyst for degradation of carbamazepine(CBZ).However,metal phthalocyanine tends to undergo their own dimerization or polymerization,thereby reducing their activity points and affecting their catalytic properties.In this study,a catalytic system consisting of O-bridged iron perfluorophthalocyanine dimers(FePcF16-O-FePcF16),multi-walled carbon nanotubes(MWCNTs)and H2O_(2) was proposed.The results showed MWCNTs loaded with FePcF16-O-FePcF16 can achieve excellent degradation of CBZ with smaller dosages of FePcF16-O-FePcF16 and H2O_(2),and milder reaction temperatures.In addition,the results of experiments revealed the reaction mechanism of non-hydroxyl radicals.The highly oxidized high-valent iron-oxo(Fe(IV)=O)species was the main reactive species in the FePcF16-O-FePcF16/MWCNTs/H2O_(2) system.It is noteworthy that MWCNTs can improve the dispersion of FePcF16-O-FePcF16,contributing to the production of highly oxidized Fe(IV)=O.Then,the pathway of CBZ oxidative degradation was speculated,and the study results also provide new ideas for metal phthalocyanine-loaded carbon materials to degrade emerging pollutants.展开更多
基金supported by the National Natural Science Foundation of China (No.51703201)。
文摘Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis.However,the traditional problems such as high recombination rate of photogenerated carriers limit its application.In this work,we introduce nitrogen deficiency into g-C_(3)N_(4)to solve this problem a simple and safe in-situ reduction method.g-C_(3)N_(4)/CaCO_(3)was obtained by a simple and safe one-step calcination method with industrial-grade micron particles CaCO_(3).Cyano group modification was in-situ reduced during the thermal polymerization process,which would change the internal electronic structure of g-C_(3)N_(4).The successful combination of g-C_(3)N_(4)and CaCO_(3)and the introduction of cyanide have been proved by Fourier transform infrared spectroscopy and X-ray photoelectron spectrometer.The formation of the cyano group,an electron-absorbing group,promotes the effective separation of photogenic electron hole pairs and inhibits the recombination of photogenic carriers.These advantages result in the generation of more·O_(2)-and1O_(2)in the catalytic system,which increases the photocatalytic efficiency of nicotine degradation by ten times.Furthermore,the degradation process of nicotine has been studied in this work to provide a basis for the degradation of nicotine organic pollutants in the air.
基金This work was financially supported by the National Natu-ral Science Foundation of China(Nos.22278378,22208190,and 21706120)the Natural Science Foundation of Jiangsu Province(No.BK20211592)+2 种基金the National Postdoctoral Program for Innovative Tal-ents(No.BX2021146)the Shuimu Tsinghua Scholar Program(No.2021SM055)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Ti_(3)C_(2)T_(x)MXene fiber has shown extraordinary potential for supercapacitor electrode in wearable elec-tronics and textile energy storage,but realizing high energy density and practical-powered applications remains a great challenge.Here,we report a covalent-architected molybdenum disulfide-Ti_(3)C_(2)T_(x)(MoS_(2)-Ti_(3)C_(2)T_(x))core-shell fiber for high-performance supercapacitor.Benefiting from the microfluidic and micro-reaction strategies,the ordered MoS_(2)arrays are strongly bridged on Ti_(3)C_(2)T_(x)fiber via Ti-O-Mo bond,re-sulting in large exposed surface,enhanced porosity and excellent interfacial conduction for charges high diffusion and faradaic transfer.The MoS_(2)-Ti_(3)C_(2)T_(x)fiber exhibits ultra-large capacitance of 2028 F cm^(-3)and admirable reversibility in 1 M H_(2)SO_(4)aqueous electrolyte.Meanwhile,MoS_(2)-Ti_(3)C_(2)T_(x)fiber-based solid-state supercapacitor presents high energy density of 23.86 mWh cm^(-3),capacitance of 1073.6 F cm^(-3)and superior cycling ability of 92.13%retention after 20,000 cycles,which can realize stable energy supply for wearable watch,LEDs,electric fans,toy ship and self-powered devices.Our work may provide an insight-ful guidance for the advanced design of structural fiber towards robust new energy and next-generation wearable industry.
基金supported by the Natural Science Foundation of Zhejiang Province(No.LDQ23E030001)。
文摘Microplastic pollution has become one of the most concerned focuses in the world.Among many treatment methods,photocatalysis is considered to be one of the most environmentally friendly methods.In this work,the photodegradation behavior of polyamide microplastics is studied by using polyamide 6(PA6)as model microplastics and FeCl_(3) as catalyst.It is hoped that the PA6 fiber can be effectively degraded by utilizing the strong oxidizing active species that can be produced after FeCl_(3) is irradiated in water.The results shows that PA6 fiber can be almost completely degraded after 10 days of irradiation in FeCl_(3) aqueous solution,indicating that it is promising to use this new method to solve the problem of PA6type microplastics.In addition,the chain scission mechanism and degradation process of PA6 are analyzed in detail by ultra-high performance liquid chromatography-tandem mass spectrometry(UPLC-MS),which provides a new insight for the study of polymer degradation mechanism.
基金The work was supported by the Scientific Research Foundation of Zhejiang Sci-Tech University(19212450-Y).
文摘The catalytic conversion of biomass platform chemicals using abundant non-noble metal nanocatalysts is a challenging topic.Here,high-density cobalt oxide nanoparticles loaded on biomass-derived porous N-doped carbon(NC)was fabricated by a tandem hydrothermal pyrolysis and mild nitrate decomposition process,which is a green and cheap preparation method.The Co_(3)O_(4) nanoparticles with the average size of 12 nm were uniformly distributed on the porous NC.The nanocomposites also possessed large surface area,high N content,good dispersibility in isopropanol,and furfural absorbability.Due to these characteristics,the novel cobalt nanocatalyst exhibited high catalytic activity for producing furfuryl alcohol,yielding 98.7%of the conversion and 97.1%of the selectivity at 160℃ for 6 h under 1 bar H2.The control experiments implied that both direct hydrogenation and transfer hydrogenation pathways co-existed in the hydrogenation reaction.The excellent catalytic activity of Co_(3)O_(4)@NC was attributed to the cooperative effects of porous NC and Co_(3)O_(4) nanoparticles.This approach provides a new idea to design effective high-density nonnoble metal oxide nanocatalysts for hydrogenation reactions,which can make full use of sustainable natural biomass.
基金This work was supported by the Scientific Research Foundation of Zhejiang Sci-Tech University(19212450-Y).
文摘In the research for the safe and efficiently antibacterial cotton fabrics to minimize risk for human health,an organic–inorganic hybrid material of ZnO nanoparticles(NPs)and quaternary ammonium salt(QAS)was employed to modify cotton fabrics by a dipping–padding–drying method.The synergistic effects of ZnO NPs and QAS on the structure and antibacterial properties of cotton fabrics were studied in detail.Results displayed that the QAS and ZnO NPs were immobilized firmly in cotton fabric by the formation of chemical covalent bonds and silica gel structure.ZnO/QAS/cotton had a good inhibitory effect on the growth of E.coli and S.aureus,with superior antibacterial efficiency of>99.99%.ZnO/QAS/cotton preserved good mechanical property,water absorbability,and limpness.We also provided a detailed analysis of antibacterial mechanism for the hybrid materials.The contact mechanism and the Zn2+release were considered as the main mechanisms for the ZnO/QAS/cotton,while the reactive oxygen species(ROS)generation only had a little contribution to the antibacterial activity.In short,the excellent integrated properties endowed the hybrid cotton fabrics as potential application in many fields,like healthcare,food packaging.
基金Zhejiang Provincial Natural Science Key Foundation of China(No.LZ20E030003)National Science Foundation of China(No.51673121)+1 种基金Candidates of Young and Middle Aged Academic Leader of Zhejiang Province,the Young Elite Scientists Sponsorship Program by CAST(No.2018QNRC001)Excellent Doctoral Thesis Cultivation Fund(No.2019D01).
文摘If a person comes into contact with pathogens on public facilities,there is a threat of contact(skin/wound)infections.More urgently,there are also reports about COVID-19 coronavirus contact infection,which once again reminds that contact infection is a very easily overlooked disease exposure route.Herein,we propose an innovative implantation strategy to fabricate a multi-walled carbon nanotube/polyvinyl alcohol(MWCNT/PVA,MCP)interpenetrating interface to achieve flexibility,anti-damage,and non-contact sensing electronic skin(E-skin).Interestingly,the MCP E-skin had a fascinating non-contact sensing function,which can respond to the finger approaching 0−20 mm through the spatial weak field.This non-contact sensing can be applied urgently to human–machine interactions in public facilities to block pathogen.The scratches of the fruit knife did not damage the MCP E-skin,and can resist chemical corrosion after hydrophobic treatment.In addition,the MCP E-skin was developed to real-time monitor the respiratory and cough for exercise detection and disease diagnosis.Notably,the MCP E-skin has great potential for emergency applications in times of infectious disease pandemics.
基金the National Natural Science Foundation of China(No.51703201)Zhejiang Provincial Natural Science Foundation of China(No.LQ17E030003)。
文摘Metal phthalocyanine has been extensively studied as a catalyst for degradation of carbamazepine(CBZ).However,metal phthalocyanine tends to undergo their own dimerization or polymerization,thereby reducing their activity points and affecting their catalytic properties.In this study,a catalytic system consisting of O-bridged iron perfluorophthalocyanine dimers(FePcF16-O-FePcF16),multi-walled carbon nanotubes(MWCNTs)and H2O_(2) was proposed.The results showed MWCNTs loaded with FePcF16-O-FePcF16 can achieve excellent degradation of CBZ with smaller dosages of FePcF16-O-FePcF16 and H2O_(2),and milder reaction temperatures.In addition,the results of experiments revealed the reaction mechanism of non-hydroxyl radicals.The highly oxidized high-valent iron-oxo(Fe(IV)=O)species was the main reactive species in the FePcF16-O-FePcF16/MWCNTs/H2O_(2) system.It is noteworthy that MWCNTs can improve the dispersion of FePcF16-O-FePcF16,contributing to the production of highly oxidized Fe(IV)=O.Then,the pathway of CBZ oxidative degradation was speculated,and the study results also provide new ideas for metal phthalocyanine-loaded carbon materials to degrade emerging pollutants.
