Layered materials are particularly attractive for supercapacitors because of their unique physical,electrical and chemical properties.Here,we demonstrate a facile and scalable electrochemical deposition method for waf...Layered materials are particularly attractive for supercapacitors because of their unique physical,electrical and chemical properties.Here,we demonstrate a facile and scalable electrochemical deposition method for wafer-scale synthesis of quasilayered tungstate-doped polypyrrole films(named TALPy)with controllable thickness and size.The as-prepared TALPy film exhibits a high gravimetric density and excellent volumetric capacitance,exceeding many high-performing carbon-and polymerbased film electrodes.Based on combined results of ex-situ X-ray diffraction(XRD),Raman and X-ray photoelectron spectroscopy(XPS),it is determined that TALPy stores charge through an ion intercalation process accompanied by change in oxidation states of polypyrrole backbone,which is referred as intercalation pseudocapacitance.All these results suggest the great promise of electrochemical deposition as a scalable and controllable bottom-up approach for synthesizing quasi-layered conductive organic-inorganic hybrid films for electrochemical energy storage applications with high volumetric performance.展开更多
Scanning electrochemical cell microscopy(SECCM)is increasingly applied to determine the intrinsic catalytic activity of single electrocatalyst particle.This is especially feasible if the catalyst nanoparticles are lar...Scanning electrochemical cell microscopy(SECCM)is increasingly applied to determine the intrinsic catalytic activity of single electrocatalyst particle.This is especially feasible if the catalyst nanoparticles are large enough that they can be found and counted in post-SECCM scanning electron microscopy images.Evidently,this becomes impossible for very small nanoparticles and hence,a catalytic current measured in one landing zone of the SECCM droplet cannot be correlated to the exact number of catalyst particles.We show,that by introducing a ruler method employing a carbon nanoelectrode decorated with a countable number of the same catalyst particles from which the catalytic activity can be determined,the activity determined using SECCM from many spots can be converted in the intrinsic catalytic activity of a certain number of catalyst nanoparticles.展开更多
基金supported by the Australian Research Council Discovery Project(No.DP190101008)Future Fellowship(No.FT190100058)the UNSW Scientia Program.H.B.L.acknowledges the University International Postgraduate Award(UIPA)PhD Scholarship from UNSW Sydney.
文摘Layered materials are particularly attractive for supercapacitors because of their unique physical,electrical and chemical properties.Here,we demonstrate a facile and scalable electrochemical deposition method for wafer-scale synthesis of quasilayered tungstate-doped polypyrrole films(named TALPy)with controllable thickness and size.The as-prepared TALPy film exhibits a high gravimetric density and excellent volumetric capacitance,exceeding many high-performing carbon-and polymerbased film electrodes.Based on combined results of ex-situ X-ray diffraction(XRD),Raman and X-ray photoelectron spectroscopy(XPS),it is determined that TALPy stores charge through an ion intercalation process accompanied by change in oxidation states of polypyrrole backbone,which is referred as intercalation pseudocapacitance.All these results suggest the great promise of electrochemical deposition as a scalable and controllable bottom-up approach for synthesizing quasi-layered conductive organic-inorganic hybrid films for electrochemical energy storage applications with high volumetric performance.
基金funding from the European Research Council(ERC)under the European Unions Horizon 2020 research and innovation programme(grant agreement CasCat[833408])well as from the European Unions Horizon 2020 research and innovation program under the Marie Sktodowska-Curie MSCA-ITN Single-Entity Nanoelectrochemistry,Sentinel[812398]+2 种基金S.S.and C.A.acknowledge the Deutsche Forschungsgemeinschaft(DFG,German Research Foundation)within the project[440951282]X.X.C.acknowledges financial support from the Liaoning BaiQianWan Talents Program,China(No.2019B042)the Excellent Young Scientific and Technological Talents Project of Educational Department of Liaoning Province,China(No.2020LNQN07).
文摘Scanning electrochemical cell microscopy(SECCM)is increasingly applied to determine the intrinsic catalytic activity of single electrocatalyst particle.This is especially feasible if the catalyst nanoparticles are large enough that they can be found and counted in post-SECCM scanning electron microscopy images.Evidently,this becomes impossible for very small nanoparticles and hence,a catalytic current measured in one landing zone of the SECCM droplet cannot be correlated to the exact number of catalyst particles.We show,that by introducing a ruler method employing a carbon nanoelectrode decorated with a countable number of the same catalyst particles from which the catalytic activity can be determined,the activity determined using SECCM from many spots can be converted in the intrinsic catalytic activity of a certain number of catalyst nanoparticles.