A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐cry...A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐crystal X‐ray analysis,Fourier transform infrared spectroscopy,thermogravimetric analyses,CNH elemental analysis and UV‐Vis diffuse reflectance spectroscopy.BUC‐21exhibited an excellent performance for photocatalytic Cr(VI)reduction with a conversion efficiency of96%,better than that of commercial P25(39%),under UV light irradiation for30min.BUC‐21could also be used to conduct photocatalytic degradation of organic dyes including methylene blue,rhodamine B,methyl orange and reactive red X‐3B.Also,the photocatalytic activity of BUC‐21remained high across a wide pH range from2.0to12.0.It is interesting to note,however,that BUC‐21was unable to achieve simultaneous reduction of Cr(VI)and degradation of an organic pollutant in a mixed matrix,which can be attributed to the competition between Cr(VI)and the organic dyes for access to the photo‐excited electrons.展开更多
X-ray photoelectron spectroscopy(XPS)and Raman spectroscopy were used to analyze the complexes in LiCl−KCl eutectic salt containing VCl_(3) and KF.The additional fluoride ions would replace chloride ions and combine w...X-ray photoelectron spectroscopy(XPS)and Raman spectroscopy were used to analyze the complexes in LiCl−KCl eutectic salt containing VCl_(3) and KF.The additional fluoride ions would replace chloride ions and combine with V(Ⅲ)to form VF_(6)^(3-).The electrochemical behavior of V(Ⅲ)was evaluated under condition of the molar concentration ratio of F−to Vn+(α)equal to 0:1,1:1,2:1,5:1,20:1 and 50:1,respectively.The results showed that a new reduction step appeared:VF_(6)^(3-)→V^(2+),and the reduction mechanism of vanadium ions became more complicated.The metallic vanadium was deposited on the tungsten electrode at−2.90 V in the LiCl−KCl melts for 6 h,and the products were characterized by SEM−EDS.It was indicated that the particle size of the product decreased with adding fluoride ions for the forming of the coordination compound VF_(6)^(3-).展开更多
Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loadin...Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging.Herein,we report a high-loading(7.5 wt%)Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes.Both the nitrogen-doped porous carbon(NPC)support with high specific surface area and ο-phenylenediamine(o-PD)play key roles role in the preparation of high-loading Fe-SA/NPC catalysts.The results of X-ray photoelectron spectroscopy,high-angle annular dark-field scanning transmission electron microscopy,and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates(Fe-N_(4)).The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading.The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V.Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.展开更多
基金supported by the National Natural Science Foundation of China(51578034)the Beijing Natural Science Foundation&Scientific Research Key Program of Beijing Municipal Commission of Education(KZ201410016018)+1 种基金Beijing Talent Project(2016023)Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(IDHT20170508)~~
文摘A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐crystal X‐ray analysis,Fourier transform infrared spectroscopy,thermogravimetric analyses,CNH elemental analysis and UV‐Vis diffuse reflectance spectroscopy.BUC‐21exhibited an excellent performance for photocatalytic Cr(VI)reduction with a conversion efficiency of96%,better than that of commercial P25(39%),under UV light irradiation for30min.BUC‐21could also be used to conduct photocatalytic degradation of organic dyes including methylene blue,rhodamine B,methyl orange and reactive red X‐3B.Also,the photocatalytic activity of BUC‐21remained high across a wide pH range from2.0to12.0.It is interesting to note,however,that BUC‐21was unable to achieve simultaneous reduction of Cr(VI)and degradation of an organic pollutant in a mixed matrix,which can be attributed to the competition between Cr(VI)and the organic dyes for access to the photo‐excited electrons.
基金supports from the National Key Research and Development Program of China (No.2021YFC2901600)supported by the State Key Laboratory of Special Rare Metal Materials (No.SKL2020K004)。
文摘X-ray photoelectron spectroscopy(XPS)and Raman spectroscopy were used to analyze the complexes in LiCl−KCl eutectic salt containing VCl_(3) and KF.The additional fluoride ions would replace chloride ions and combine with V(Ⅲ)to form VF_(6)^(3-).The electrochemical behavior of V(Ⅲ)was evaluated under condition of the molar concentration ratio of F−to Vn+(α)equal to 0:1,1:1,2:1,5:1,20:1 and 50:1,respectively.The results showed that a new reduction step appeared:VF_(6)^(3-)→V^(2+),and the reduction mechanism of vanadium ions became more complicated.The metallic vanadium was deposited on the tungsten electrode at−2.90 V in the LiCl−KCl melts for 6 h,and the products were characterized by SEM−EDS.It was indicated that the particle size of the product decreased with adding fluoride ions for the forming of the coordination compound VF_(6)^(3-).
文摘Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging.Herein,we report a high-loading(7.5 wt%)Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes.Both the nitrogen-doped porous carbon(NPC)support with high specific surface area and ο-phenylenediamine(o-PD)play key roles role in the preparation of high-loading Fe-SA/NPC catalysts.The results of X-ray photoelectron spectroscopy,high-angle annular dark-field scanning transmission electron microscopy,and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates(Fe-N_(4)).The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading.The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V.Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.
