Owing to the ppb-level detection standard toward the toxic and harmful gas,the detection of trace gases has become an important subject in the field of indoor environment management.However,the traditional resistive g...Owing to the ppb-level detection standard toward the toxic and harmful gas,the detection of trace gases has become an important subject in the field of indoor environment management.However,the traditional resistive gas sensors hardly meet the requirement due to the weak signal generated by trace gas molecules that are difficult to capture.Herein,a visible-light-assisted Pd/TiO_(2)gas sensor is proposed to endow the effective detection of trace formaldehyde(HCHO)gas without heating temperature.Benefiting from the enhanced photocatalytic properties of TiO_(2)by Pd decoration,the visible-light-assisted Pd/TiO_(2)gas sensor can detect the HCHO gas as low as80×10^(–9)at room temperature.The successful preparation of nanoscale TiO_(2)sensing layer is facilitated by the ultrathin carbon nanotube interdigital electrode in the gas sensor,which avoids the discontinuity of the sensing layer caused by the excessive thickness of the traditional metal electrode.In addition,the whole preparation process of the Pd/TiO_(2)gas sensor with carbon nanotube electrodes is compatible with mainstream CMOS fabrication technology,which is expected to realize the batch fabrication and micro-integrated application of gas sensors.It is expected that our work can provide a new strategy for the batch preparation of high-performance trace HCHO gas sensors and their future applications in portable electronic devices such as smartphones.展开更多
The state-of-the-art anion-exchange membrane water electrolyzers(AEMWEs)require highly stable electrodes for prolonged operation.The stability of the electrode is closely linked to the effective evacuation of H_(2) or...The state-of-the-art anion-exchange membrane water electrolyzers(AEMWEs)require highly stable electrodes for prolonged operation.The stability of the electrode is closely linked to the effective evacuation of H_(2) or O_(2) gas generated from electrode surface during the electrolysis.In this study,we prepared a superhydrophilic electrode by depositing porous nickel–iron nanoparticles on annealed TiO_(2) nanotubes(NiFe/ATNT)for rapid outgassing of such nonpolar gases.The super-hydrophilic NiFe/ATNT electrode exhibited an overpotential of 235 mV at 10 mA cm^(−2) for oxygen evolution reaction in 1.0 M KOH solution,and was utilized as the anode in the AEMWE to achieve a current density of 1.67 A cm^(−2) at 1.80 V.In addition,the AEMWE with NiFe/ATNT electrode,which enables effective outgassing,showed record stability for 1500 h at 0.50 A cm^(−2) under harsh temperature conditions of 80±3℃.展开更多
TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed ...TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed to characterize the TiNT electrodes. The linear voltammetry results under irradiation showed that the TiNT electrode annealed at 450℃ presented the highest photoelectrochemical activity. By combining photocatalytic with electrochemical process, a significantly synergetic effect on ammonia degradation was observed with Na2SO4 as supporting electrolyte at pH 10.7. Furthermore, the photoelectrocatalytic efficiency on the ammonia degradation was greatly enhanced in presence of chloride ions without the limitation ofpH. The degradation rate was improved by 14.8 times reaching 4.98 × 10^-2 min^-1 at pH 10.7 and a faster degradation rate of 6.34 × 10^-2 min^-1 was obtained at pH 3.01. The in situ photoelectrocatalytic generated active chlorine was proposed to be responsible for the improved efficiency. On the other hand, an enhanced degradation of ammonia using TiNT electrode fabricated in fluorinated organic solution was also confirmed compared to TiNT electrode anodized in fluorinated water solution and TiO2 film electrode fabricated by sol-gel method. Finally, the effect of chloride concentration was also discussed.展开更多
Pd-MnO2/TiO2 nanotube arrays（NTAs） photo-electrodes were successfully fabricated via anodization and electro deposition subsequently; the obtained Pd-MnO2/TiO2 NTAs photo electrodes were analyzed by scanning electro...Pd-MnO2/TiO2 nanotube arrays（NTAs） photo-electrodes were successfully fabricated via anodization and electro deposition subsequently; the obtained Pd-MnO2/TiO2 NTAs photo electrodes were analyzed by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and characterized accordingly. Moreover, the light harvesting and absorption properties were investigated via ultraviolet–visible diffuse reflectance spectrum（DRS）; photo degradation efficiency was investigated via analyzing the photo catalytic degradation of Rhodamine B under visible illumination（xenon light）. The performed analyses illustrated that Pd-MnO2 codoped particles were successfully deposited onto the surface of the TiO2 nanotube arrays;DRS results showed significant improvement in visible light absorption which was between400 and 700 nm. Finally, the photo catalytic degradation efficiency results of the designated organic pollutant（Rhodamine B） illustrated a superior photocatalytic（PC） efficiency of approximately 95% compared to the bare TiO2 NTAs, which only exhibited a photo catalytic degradation efficiency of approximately 61%, thus it indicated the significant enhancement of the light absorption properties of fabricated photo electrodes and their yield of UOH radicals.展开更多
The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra bind...The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization,a complex fabrication process,and weak conductivity.Herein,a three-dimensional(3D)porous electrode was fabricated in-situ on a Ni foam(NF)substrate integrated with nitrogen-doped carbon nanotubes(N@C)derived from carbonization of zeolitic imidazolate framework-8(ZIF-8)without any binder.The resulting 900/N@C-NF cathode(synthesized at 900℃)was high in surface area,N content,and degree of graphitization,achieved high performance of H_(2)O_(2)production(2.58 mg L^(−1)h^(−1)H_(2)O_(2)/mg catalyst)at-0.7 V(vs.SCE),and enabled prompt regeneration of Fe^(2+).The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants,including rhodamine B(Rh B),phenol,bisphenol A(BPA),nitroben-zene(NB),and Cu-ethylenediaminetetraacetic acid(EDTA),and significantly attenuating the concentration of chemical oxygen demand(COD)in the real acid wastewater,exhibiting superior activity and stability.This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment,particularly those rich in organics,acids,and Fe^(3+)/Fe^(2+).展开更多
Electrical double-layer capacitors(EDLCs)consist of energy storage devices that present high-power and moderate energy density.The electrolyte and electrode physicochemical properties are crucial for improving their o...Electrical double-layer capacitors(EDLCs)consist of energy storage devices that present high-power and moderate energy density.The electrolyte and electrode physicochemical properties are crucial for improving their overall energy storage capabilities.Therefore,the stability of the EDLCs’materials is the primary focus of this study.Since energy storage depends on the specific capacitance,and also on the square of the maximum capacitive cell voltage(UMCV).Thus,electrodes with high specific surface area(SSA)and electrolytes with excellent electrochemical stability are commonly reported in the literature.Aqueous electrolytes are safer and green devices compared to other organic-based solutions.On the other hand,their UMCVis reduced compared to other electrolytes(e.g.,organic-based and ionic liquids).In this sense,spanning the UMCVfor aqueous-based electrolytes is a’hot topic’research.Unfortunately,the lack of protocols to establish reliable UMCVvalues has culminated in the publishing of several conflicting results.Herein,we confirm that multiwalled carbon nanotubes(MWCNTs)housed in cells degrade and produce CO_(2) under abusive polarisation conditions.It is probed by employing electrochemical techniques,in-situ FTIR and in-situ Raman spectroscopies.From these considerations,the current study uses spectro-electrochemical techniques to support the correct determination of the electrode and electrolyte stability conditions as a function of the operating electrochemical parameters.展开更多
Thin titanium oxide nanotube arrays (TNAs) films were synthesized by anodization of titanium foil in an aqueous dimethyl sulfoxide solution using a platinum foil counter electrode.TNAs up to 6.8 μm in length,120 nm i...Thin titanium oxide nanotube arrays (TNAs) films were synthesized by anodization of titanium foil in an aqueous dimethyl sulfoxide solution using a platinum foil counter electrode.TNAs up to 6.8 μm in length,120 nm in inner pore diameter,and 20 nm in wall thickness were obtained by 40 V potentials anodization for 24 h.Their microstructures and surface morphologies were characterized by XRD,TEM,SAED and UV-vis spectroscopy.The photoelectrochemical properties of as-prepared unsensitized and dye-sensitized TNAs electrodes were examined under simulated solar light (AM 1.5,100 mW/cm2) illumination.The results showed that the photocurrent of the dye-sensitized TNAs electrodes reached 6.9 mA/cm2,which was 6 times more than that of the dye-sensitized TiO2 nanoparticles (TNPs) electrodes.It implied that the electron transport process and the charge recombination suppression within TNAs electrodes were much more favorable in comparison with that in the TNPs electrodes.Electrodes applying such kind of titania nanotubes will have a potential to further enhance the efficiencies of TNAs-based dye-sensitized solar cells.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.62071410 and 62101477)Hunan Provincial Natural Science Foundation(No.2021JJ40542)the Postgraduate Scientific Research Innovation Project of Hunan Province(No.CX20210627)。
文摘Owing to the ppb-level detection standard toward the toxic and harmful gas,the detection of trace gases has become an important subject in the field of indoor environment management.However,the traditional resistive gas sensors hardly meet the requirement due to the weak signal generated by trace gas molecules that are difficult to capture.Herein,a visible-light-assisted Pd/TiO_(2)gas sensor is proposed to endow the effective detection of trace formaldehyde(HCHO)gas without heating temperature.Benefiting from the enhanced photocatalytic properties of TiO_(2)by Pd decoration,the visible-light-assisted Pd/TiO_(2)gas sensor can detect the HCHO gas as low as80×10^(–9)at room temperature.The successful preparation of nanoscale TiO_(2)sensing layer is facilitated by the ultrathin carbon nanotube interdigital electrode in the gas sensor,which avoids the discontinuity of the sensing layer caused by the excessive thickness of the traditional metal electrode.In addition,the whole preparation process of the Pd/TiO_(2)gas sensor with carbon nanotube electrodes is compatible with mainstream CMOS fabrication technology,which is expected to realize the batch fabrication and micro-integrated application of gas sensors.It is expected that our work can provide a new strategy for the batch preparation of high-performance trace HCHO gas sensors and their future applications in portable electronic devices such as smartphones.
基金supported by the National Research Foundation of Korea(RS-2023-00207831,RS-2024-00346153).
文摘The state-of-the-art anion-exchange membrane water electrolyzers(AEMWEs)require highly stable electrodes for prolonged operation.The stability of the electrode is closely linked to the effective evacuation of H_(2) or O_(2) gas generated from electrode surface during the electrolysis.In this study,we prepared a superhydrophilic electrode by depositing porous nickel–iron nanoparticles on annealed TiO_(2) nanotubes(NiFe/ATNT)for rapid outgassing of such nonpolar gases.The super-hydrophilic NiFe/ATNT electrode exhibited an overpotential of 235 mV at 10 mA cm^(−2) for oxygen evolution reaction in 1.0 M KOH solution,and was utilized as the anode in the AEMWE to achieve a current density of 1.67 A cm^(−2) at 1.80 V.In addition,the AEMWE with NiFe/ATNT electrode,which enables effective outgassing,showed record stability for 1500 h at 0.50 A cm^(−2) under harsh temperature conditions of 80±3℃.
基金supported by the National Natural Science Foundation of China (Nos. 21277134, 21107103)the State Key Laboratory of Environmental, Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences
文摘TiO2 nanotube （TINT） electrodes anodized in fluorinated organic solutions were successfully prepared on Ti sheets. Field-emission scanning electron microscopy （FE-SEM） and X-ray diffraction （XRD） were performed to characterize the TiNT electrodes. The linear voltammetry results under irradiation showed that the TiNT electrode annealed at 450℃ presented the highest photoelectrochemical activity. By combining photocatalytic with electrochemical process, a significantly synergetic effect on ammonia degradation was observed with Na2SO4 as supporting electrolyte at pH 10.7. Furthermore, the photoelectrocatalytic efficiency on the ammonia degradation was greatly enhanced in presence of chloride ions without the limitation ofpH. The degradation rate was improved by 14.8 times reaching 4.98 × 10^-2 min^-1 at pH 10.7 and a faster degradation rate of 6.34 × 10^-2 min^-1 was obtained at pH 3.01. The in situ photoelectrocatalytic generated active chlorine was proposed to be responsible for the improved efficiency. On the other hand, an enhanced degradation of ammonia using TiNT electrode fabricated in fluorinated organic solution was also confirmed compared to TiNT electrode anodized in fluorinated water solution and TiO2 film electrode fabricated by sol-gel method. Finally, the effect of chloride concentration was also discussed.
基金supported by the National Natural Science Foundation of China (No. 51178138)the National Creative Research Groups of China (No. 51121062)the State Key Laboratory of Urban Water Resources and Environment (No. 2010DX03)
文摘Pd-MnO2/TiO2 nanotube arrays（NTAs） photo-electrodes were successfully fabricated via anodization and electro deposition subsequently; the obtained Pd-MnO2/TiO2 NTAs photo electrodes were analyzed by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and characterized accordingly. Moreover, the light harvesting and absorption properties were investigated via ultraviolet–visible diffuse reflectance spectrum（DRS）; photo degradation efficiency was investigated via analyzing the photo catalytic degradation of Rhodamine B under visible illumination（xenon light）. The performed analyses illustrated that Pd-MnO2 codoped particles were successfully deposited onto the surface of the TiO2 nanotube arrays;DRS results showed significant improvement in visible light absorption which was between400 and 700 nm. Finally, the photo catalytic degradation efficiency results of the designated organic pollutant（Rhodamine B） illustrated a superior photocatalytic（PC） efficiency of approximately 95% compared to the bare TiO2 NTAs, which only exhibited a photo catalytic degradation efficiency of approximately 61%, thus it indicated the significant enhancement of the light absorption properties of fabricated photo electrodes and their yield of UOH radicals.
基金financial support from the Guangdong Special Support Plan for Innovation Teams (No.2019BT02L218)the Science and Technology Planning Project of Guangdong Province,China (No.2019A050510009)+3 种基金the Guangdong Special Support Plan for Young Top-notch Talents (No.2019TQ05L179)the National Natural Science Foundation of China (No.21876052)the Science and Technology Program of Guangzhou,China (No.201904010293)the Fundamental Research Funds for the Central Universities,SCUT (No.2020ZYGXZR055)。
文摘The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization,a complex fabrication process,and weak conductivity.Herein,a three-dimensional(3D)porous electrode was fabricated in-situ on a Ni foam(NF)substrate integrated with nitrogen-doped carbon nanotubes(N@C)derived from carbonization of zeolitic imidazolate framework-8(ZIF-8)without any binder.The resulting 900/N@C-NF cathode(synthesized at 900℃)was high in surface area,N content,and degree of graphitization,achieved high performance of H_(2)O_(2)production(2.58 mg L^(−1)h^(−1)H_(2)O_(2)/mg catalyst)at-0.7 V(vs.SCE),and enabled prompt regeneration of Fe^(2+).The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants,including rhodamine B(Rh B),phenol,bisphenol A(BPA),nitroben-zene(NB),and Cu-ethylenediaminetetraacetic acid(EDTA),and significantly attenuating the concentration of chemical oxygen demand(COD)in the real acid wastewater,exhibiting superior activity and stability.This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment,particularly those rich in organics,acids,and Fe^(3+)/Fe^(2+).
基金the financial support from the Brazilian funding agencies CNPq(301486/2016-6)FAEPEX(2426/17)+7 种基金FAPESP(2020/04431-0,2020/04281-8,2016/25082-8,2017/11986-5,2017/11958-1,2014/02163-7,2018/20756-6,2018/02713-8)CAPES(1740195)the financial support from CNPq(Processes 131234/2020-0 and 130741/2021-3)the Fundação ao AmparoàPesquisa do Estado de Minas Gerais(FAPEMIGCNPq for the PQ-2 grant(Process 310544/20190)the support of Shell,the strategic importance of the support given by Brazil’s National Oil,Natural Gas,and Biofuels Agency(ANP)through the R&D levy regulationthe Center for Innovation on New Energies(CINE)the LNLS/CNPEM。
文摘Electrical double-layer capacitors(EDLCs)consist of energy storage devices that present high-power and moderate energy density.The electrolyte and electrode physicochemical properties are crucial for improving their overall energy storage capabilities.Therefore,the stability of the EDLCs’materials is the primary focus of this study.Since energy storage depends on the specific capacitance,and also on the square of the maximum capacitive cell voltage(UMCV).Thus,electrodes with high specific surface area(SSA)and electrolytes with excellent electrochemical stability are commonly reported in the literature.Aqueous electrolytes are safer and green devices compared to other organic-based solutions.On the other hand,their UMCVis reduced compared to other electrolytes(e.g.,organic-based and ionic liquids).In this sense,spanning the UMCVfor aqueous-based electrolytes is a’hot topic’research.Unfortunately,the lack of protocols to establish reliable UMCVvalues has culminated in the publishing of several conflicting results.Herein,we confirm that multiwalled carbon nanotubes(MWCNTs)housed in cells degrade and produce CO_(2) under abusive polarisation conditions.It is probed by employing electrochemical techniques,in-situ FTIR and in-situ Raman spectroscopies.From these considerations,the current study uses spectro-electrochemical techniques to support the correct determination of the electrode and electrolyte stability conditions as a function of the operating electrochemical parameters.
基金supported by the National Natural Science Foundation of China (10904128)the Zhejiang Provincial Natural Science Foundation (Y6100171 and Y6110467)Start-up Research Foundation of Zhejiang University of Science and Technology (F501108C01)
文摘Thin titanium oxide nanotube arrays (TNAs) films were synthesized by anodization of titanium foil in an aqueous dimethyl sulfoxide solution using a platinum foil counter electrode.TNAs up to 6.8 μm in length,120 nm in inner pore diameter,and 20 nm in wall thickness were obtained by 40 V potentials anodization for 24 h.Their microstructures and surface morphologies were characterized by XRD,TEM,SAED and UV-vis spectroscopy.The photoelectrochemical properties of as-prepared unsensitized and dye-sensitized TNAs electrodes were examined under simulated solar light (AM 1.5,100 mW/cm2) illumination.The results showed that the photocurrent of the dye-sensitized TNAs electrodes reached 6.9 mA/cm2,which was 6 times more than that of the dye-sensitized TiO2 nanoparticles (TNPs) electrodes.It implied that the electron transport process and the charge recombination suppression within TNAs electrodes were much more favorable in comparison with that in the TNPs electrodes.Electrodes applying such kind of titania nanotubes will have a potential to further enhance the efficiencies of TNAs-based dye-sensitized solar cells.
