To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium p...To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH3 production with excellent selectivity.The high Faradaic efficiency of 22%with a large NH3 yield of 8.35×10^(−11) mol·s^(−1)·cm^(−2)was obtained at 0 V vs.the reversible hydrogen electrode in acid solution,superior to all previously studied V-based NRR catalysts.Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.展开更多
Colloidal core/shell quantum dots(QDs)with environment-friendly feature and controllable optoelectronic properties are promising building blocks in emerging solar technologies.In this work,we rationally design and tai...Colloidal core/shell quantum dots(QDs)with environment-friendly feature and controllable optoelectronic properties are promising building blocks in emerging solar technologies.In this work,we rationally design and tailor the eco-friendly CuInSe(CISe)/ZnSe core/shell QDs by Mn doping and stoichiometric optimization(i.e.,molar ratios of Cu/In).It is demonstrated that Mn doping in In-rich CISe/ZnSe core/shell QDs can effectively engineer the charge kinetics inside the QDs,enabling efficient photogenerated electrons transfer into the shell for retarded charge recombination.As a result,a solar-driven photoelectrochemical(PEC)device fabricated using the optimized Mn-doped In-rich CISe/ZnSe core/shell QDs(Cu/In ratio of 1/2)exhibits improved charge extraction and injection,showing a~3.5-fold higher photocurrent density than that of the pristine CISe/ZnSe core/shell QDs under 1 sun AM 1.5G illumination.The findings indicate that transition metal doping in“green”nonstoichiometric core/shell QDs may offer a new strategy for achieving high-efficiency solar energy conversion applications.展开更多
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH3 production with excellent selectivity.The high Faradaic efficiency of 22%with a large NH3 yield of 8.35×10^(−11) mol·s^(−1)·cm^(−2)was obtained at 0 V vs.the reversible hydrogen electrode in acid solution,superior to all previously studied V-based NRR catalysts.Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.
基金X.T.acknowledges the support from the National Key Research and Development Program of China(No.2019YFE0121600)the National Natural Science Foundation of China(Nos.22105031 and 62011530131)+2 种基金Sichuan Science and Technology Program(No.2021YFH0054)Innovation Group Project of Sichuan Province(No.20CXTD0090)Z.M.W.acknowledges the National Key Research and Development Program of China(No.2019YFB2203400)and the“111 Project”(No.B20030).
文摘Colloidal core/shell quantum dots(QDs)with environment-friendly feature and controllable optoelectronic properties are promising building blocks in emerging solar technologies.In this work,we rationally design and tailor the eco-friendly CuInSe(CISe)/ZnSe core/shell QDs by Mn doping and stoichiometric optimization(i.e.,molar ratios of Cu/In).It is demonstrated that Mn doping in In-rich CISe/ZnSe core/shell QDs can effectively engineer the charge kinetics inside the QDs,enabling efficient photogenerated electrons transfer into the shell for retarded charge recombination.As a result,a solar-driven photoelectrochemical(PEC)device fabricated using the optimized Mn-doped In-rich CISe/ZnSe core/shell QDs(Cu/In ratio of 1/2)exhibits improved charge extraction and injection,showing a~3.5-fold higher photocurrent density than that of the pristine CISe/ZnSe core/shell QDs under 1 sun AM 1.5G illumination.The findings indicate that transition metal doping in“green”nonstoichiometric core/shell QDs may offer a new strategy for achieving high-efficiency solar energy conversion applications.