Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction...Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.展开更多
To enhance the solubility of polyanilines(PANI),polymeric ionic liquid(PIL)was introduced into the polymerization synthesis of PANI with various proportions.The structure and properties of the modified PANIs were char...To enhance the solubility of polyanilines(PANI),polymeric ionic liquid(PIL)was introduced into the polymerization synthesis of PANI with various proportions.The structure and properties of the modified PANIs were characterized by 1H NMR,Fourier transform infrared spectroscopy,thermogravimetric analysis,ultraviolet-visible spectrum,etc.It was found that the obtained PANIs doped with PILs were soluble in various organic solvents such as N,N-dimethyl formamide and acetonitrile.Compared with the pure PANI,the PANIs doped by PILs showed remarkable solubility and their chemical structure and conductivity kept integrated.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52173055 and 21961132024)the Natural Science Foundation of Shanghai(No.19ZR1401100)+3 种基金the International Cooperation Fund of Science and Technology Commission of Shanghai Municipality(No.21130750100)the Innovation Program of Shanghai Municipal Education Commission(No.2017-01-07-00-03-E00024)the Fundamental Research Funds for the Central Universities(No.18D310109)the DHU Distinguished Young Professor Program(No.LZA2020001).
文摘Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.
基金The authors gratefully acknowledge the valuable help and great support from the Fundamental Research Funds for the Central Universities(Nos.2232018D3-07,2232018D3-24 and 2232019G-02)China Postdoctoral Science Foundation(No.2016M591573)+1 种基金the National Natural Science Foundation of China(Grant No.21404024)Changsha Science and Technology Project.
文摘To enhance the solubility of polyanilines(PANI),polymeric ionic liquid(PIL)was introduced into the polymerization synthesis of PANI with various proportions.The structure and properties of the modified PANIs were characterized by 1H NMR,Fourier transform infrared spectroscopy,thermogravimetric analysis,ultraviolet-visible spectrum,etc.It was found that the obtained PANIs doped with PILs were soluble in various organic solvents such as N,N-dimethyl formamide and acetonitrile.Compared with the pure PANI,the PANIs doped by PILs showed remarkable solubility and their chemical structure and conductivity kept integrated.
