Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartme...Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.展开更多
Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the h...Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the high surface-contact resistance and result in energy losses.Thus,a mechanism for improving the conductivity and interface stability of the GDL is an urgent issue.In this work,we have prepared a hydrophilic and corrosion resistant conductive composite protective coating.The polydopamine(PDA)film on the Ti surface,which was obtained via the solution oxidation method,ensured that neither micropores nor pinholes existed in the final hybrid coatings.In-situ reduced gold nanoparticles(AuNPs)improved the conductivity to achieve the desired interfacial contact resistance and further enhanced the corrosion resistance.The surface composition of the treated samples was investigated using scanning electron microscopy(SEM),transmis-sion electron microscopy(TEM),X-ray diffraction(XRD),and Fourier transform infrared spectroscopy(FTIR).The results indicated that the optimized reaction conditions included a pH value of 3 of HAuCl_(4) solution with PDA deposition(48 h)on papers and revealed the lowest con-tact resistance(0.5 mΩ·cm^(2))and corrosion resistance(0.001μA·cm^(−2))in a 0.5 M H_(2)SO_(4)+2 ppm F−solution(1.7 V vs.RHE)among all the modified specimens,where RHE represents reversible hydrogen electrode.These findings indicated that the Au-PDA coating is very appropriate for the modification of Ti GDLs in PEM WE systems.展开更多
基金support from the DFG through SFB 951 Hybrid Inorganic/Organic Systems for OptoElectronics(HIOS)funding by the European Research Council(ERC)Consolidator Grant with Project Number 646659-NANOREACTORthe Joint Lab for Structural Research at the Integrative Research Institute for the Sciences(IRIS Adlershof).
文摘Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.
基金supported by the National Key Research and Development Program of China(No.2018 YFB1502403)。
文摘Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the high surface-contact resistance and result in energy losses.Thus,a mechanism for improving the conductivity and interface stability of the GDL is an urgent issue.In this work,we have prepared a hydrophilic and corrosion resistant conductive composite protective coating.The polydopamine(PDA)film on the Ti surface,which was obtained via the solution oxidation method,ensured that neither micropores nor pinholes existed in the final hybrid coatings.In-situ reduced gold nanoparticles(AuNPs)improved the conductivity to achieve the desired interfacial contact resistance and further enhanced the corrosion resistance.The surface composition of the treated samples was investigated using scanning electron microscopy(SEM),transmis-sion electron microscopy(TEM),X-ray diffraction(XRD),and Fourier transform infrared spectroscopy(FTIR).The results indicated that the optimized reaction conditions included a pH value of 3 of HAuCl_(4) solution with PDA deposition(48 h)on papers and revealed the lowest con-tact resistance(0.5 mΩ·cm^(2))and corrosion resistance(0.001μA·cm^(−2))in a 0.5 M H_(2)SO_(4)+2 ppm F−solution(1.7 V vs.RHE)among all the modified specimens,where RHE represents reversible hydrogen electrode.These findings indicated that the Au-PDA coating is very appropriate for the modification of Ti GDLs in PEM WE systems.
