The photocatalytic activity of cobalt octakis（butylthio） porphyrazine（CoPz（BuS）8） was assessed through photodegradation of the dye rhodamine B（RhB） in water under irradiation with a Xe lamp and aerated conditi...The photocatalytic activity of cobalt octakis（butylthio） porphyrazine（CoPz（BuS）8） was assessed through photodegradation of the dye rhodamine B（RhB） in water under irradiation with a Xe lamp and aerated conditions.The photocatalytic activity of CoPz（BuS）8 loaded on Al2O3 or SiO2@Fe3O4nanoparticles or coordinated with an axial azide ligand was also investigated.The results demonstrated that the photocatalytic activity of CoPz（BuS）8 loaded on Al2O3 was higher than that loaded on SiO2@Fe3O4.The kinetic curves of RhB degradation in aqueous solutions at different pH indicated the pseudo first-order kinetics of the reaction.The highest degradation rate for CoPz（BuS）8 loaded Al2O3 at pH = 4 after 160 min was 84.6%.However,the advantages of easier separation and recycling as well as the ability to terminate the reaction at any time for the CoPz（BuS）8 loaded SiO2@Fe3O4 cannot be ignored.When electron-rich NaN3 was coordinated with CoPz（BuS）8 as an axial ligand and loaded on Al2O3,the resulting catalyst produced more active oxygen species such as O2^- and HO· to promote the quicker degradation of RhB than that by the other catalysts.For the N3-coordinated CoPz（BuS）8 loaded on Al2O3,the reactions at pH = 4 and 7 distinctly deviated from first-order kinetics,and the degradation rate reached 77.6%after 80 min at pH = 4.展开更多
In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBC...In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBCs).For this purpose,polyethyleneimine(PEI) was added onto the reduced graphene oxide and CoPc composite(RGO/CoPc) to create abundant NH2 axial ligand groups,for anchoring the Co core within the CoPc.Owing to the PEI addition,the onset potential of the hydrogen peroxide oxidation reaction was shifted by 0.13 V in the negative direction(0.02 V) and the current density was improved by 1.92 times(1.297 mA cm^(-2)),compared to those for RGO/CoPc(0.15 V and 0.676 mA cm^(-2),respectively),due to the formation of donor-acceptor dyads and the prevention of CoPc from leaching out.The biocatalyst using glucose oxidase(GOx)([RGO/CoPc]/PEI/GOx) showed a better onset potential and catalytic activity(0.15 V and 318.7 μA cm^(-2)) than comparable structures,as well as significantly improved operational durability and long-term stability.This is also attributed to PEI,which created a favorable microenvironment for the enzyme.The maximum power densities(MPDs) and open-circuit voltages(OCVs) obtained for HPFCs and EBCs using the suggested catalyst were 105.2±1.3 μW cm^(-2)(0.317±0.003 V) and 25.4±0.9 μW cm^(-2)(0.283±0.007 V),respectively.This shows that the amine axial ligand effectively improves the performance of the actual driving HPFCs and EBCs.展开更多
The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,pe...The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,peptide containing —SH and amino acid containing imidazolyl en- hance the catalytic activity.The effect of imidazole amounts on the catalytic activity of CoTPP is studied.展开更多
Seven 2,2'-bipyridine-based oxazole derivatives have been synthesized through multi-step reactions using 2,2'-bipyridine-3,3'-dicarboxylic acid as raw material.The structures of compounds 1-6 were characte...Seven 2,2'-bipyridine-based oxazole derivatives have been synthesized through multi-step reactions using 2,2'-bipyridine-3,3'-dicarboxylic acid as raw material.The structures of compounds 1-6 were characterized by using 1H NMR,13C NMR,MS,and X-ray single crystal diffraction techniques.The results indicate that only axially chiral enantiomers were observed in the single crystal structures of products 1 and 3 synthesized from achiral amino alcohols;Using racemic amino alcohol((±)-2-aminopropanol)as the raw material,only axial chiral isomers were observed in the single crystal structure of product 2,and no racemic isomer was found.The crystal structure of product 4 based on chiral amino alcohol((S)-valinol)contains non axial chiral isomers and S-type isomers.However,the other two optically pure amino alcohols((S)-phenylpropanol,(R)-phenylpropanol)can only obtain optically pure axially chiral and chiral products 5 and 6,respectively,maintaining the configuration of the raw amino alcohol and no non axial chiral isomer is observed.The product using(±)-2-aminobutanol as the raw material cannot be determined for its absolute configuration as a single crystal of the product has not been obtained.展开更多
The effects of peptides, amino acids and organic bases as axial ligands on reaction activities in the electrocarboxylation of benzyl chloride with CO2 catalyzed by CoTPP are reported. Imidazole, peptide containing -SH...The effects of peptides, amino acids and organic bases as axial ligands on reaction activities in the electrocarboxylation of benzyl chloride with CO2 catalyzed by CoTPP are reported. Imidazole, peptide containing -SH and amino acid containing imi dazyl can enhance the catalytic activity. As an axial ligand, imidazole is the best one, it can make the current efficency of electrocarboxylation catalyzed by CoTPP rising about 23%. The effects of different amount of imidazole on CoTPP’s catalytic activities have been studied, and the cause of these effects have been explaind predrinarily.展开更多
基金supported by National Natural Science Foundation of China (20977115, 21272281)Natural Science Foundation of Hubei Province (2014CFB919)the Science and Technology Plan Innovation Team of Wuhan City (2015070504020220)~~
文摘The photocatalytic activity of cobalt octakis（butylthio） porphyrazine（CoPz（BuS）8） was assessed through photodegradation of the dye rhodamine B（RhB） in water under irradiation with a Xe lamp and aerated conditions.The photocatalytic activity of CoPz（BuS）8 loaded on Al2O3 or SiO2@Fe3O4nanoparticles or coordinated with an axial azide ligand was also investigated.The results demonstrated that the photocatalytic activity of CoPz（BuS）8 loaded on Al2O3 was higher than that loaded on SiO2@Fe3O4.The kinetic curves of RhB degradation in aqueous solutions at different pH indicated the pseudo first-order kinetics of the reaction.The highest degradation rate for CoPz（BuS）8 loaded Al2O3 at pH = 4 after 160 min was 84.6%.However,the advantages of easier separation and recycling as well as the ability to terminate the reaction at any time for the CoPz（BuS）8 loaded SiO2@Fe3O4 cannot be ignored.When electron-rich NaN3 was coordinated with CoPz（BuS）8 as an axial ligand and loaded on Al2O3,the resulting catalyst produced more active oxygen species such as O2^- and HO· to promote the quicker degradation of RhB than that by the other catalysts.For the N3-coordinated CoPz（BuS）8 loaded on Al2O3,the reactions at pH = 4 and 7 distinctly deviated from first-order kinetics,and the degradation rate reached 77.6%after 80 min at pH = 4.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(Nos.2017R1D1A1B03032033 and 2020R1C1C1010386)“Leaders in INdustry-university Cooperation+”project supported by the Ministry of Education and National Research Foundation of Korea。
文摘In this study,an amine-coordinated cobalt phthalocyanine(CoPc)-based anodic catalyst was fabricated by a facile process,to enhance the performance of hydrogen peroxide fuel cells(HPFCs) and enzymatic biofuel cells(EBCs).For this purpose,polyethyleneimine(PEI) was added onto the reduced graphene oxide and CoPc composite(RGO/CoPc) to create abundant NH2 axial ligand groups,for anchoring the Co core within the CoPc.Owing to the PEI addition,the onset potential of the hydrogen peroxide oxidation reaction was shifted by 0.13 V in the negative direction(0.02 V) and the current density was improved by 1.92 times(1.297 mA cm^(-2)),compared to those for RGO/CoPc(0.15 V and 0.676 mA cm^(-2),respectively),due to the formation of donor-acceptor dyads and the prevention of CoPc from leaching out.The biocatalyst using glucose oxidase(GOx)([RGO/CoPc]/PEI/GOx) showed a better onset potential and catalytic activity(0.15 V and 318.7 μA cm^(-2)) than comparable structures,as well as significantly improved operational durability and long-term stability.This is also attributed to PEI,which created a favorable microenvironment for the enzyme.The maximum power densities(MPDs) and open-circuit voltages(OCVs) obtained for HPFCs and EBCs using the suggested catalyst were 105.2±1.3 μW cm^(-2)(0.317±0.003 V) and 25.4±0.9 μW cm^(-2)(0.283±0.007 V),respectively.This shows that the amine axial ligand effectively improves the performance of the actual driving HPFCs and EBCs.
文摘The effects of peptides,amino acids and organic bases as an axial ligand on reaction ac- tivities in the electrocarboxylation of benzyl chloride with CO_2 catalyzed by CoTPP are reported. The imidazole organic base,peptide containing —SH and amino acid containing imidazolyl en- hance the catalytic activity.The effect of imidazole amounts on the catalytic activity of CoTPP is studied.
基金supported by Guizhou Province College Students Innovation Project(S202310666114)the Student Program of Minzu Normal University of Xingyi(23XYXS28)Guizhou Province Qianxinan Prefecture Science and Technology Bureau project(2022-1-24).
文摘Seven 2,2'-bipyridine-based oxazole derivatives have been synthesized through multi-step reactions using 2,2'-bipyridine-3,3'-dicarboxylic acid as raw material.The structures of compounds 1-6 were characterized by using 1H NMR,13C NMR,MS,and X-ray single crystal diffraction techniques.The results indicate that only axially chiral enantiomers were observed in the single crystal structures of products 1 and 3 synthesized from achiral amino alcohols;Using racemic amino alcohol((±)-2-aminopropanol)as the raw material,only axial chiral isomers were observed in the single crystal structure of product 2,and no racemic isomer was found.The crystal structure of product 4 based on chiral amino alcohol((S)-valinol)contains non axial chiral isomers and S-type isomers.However,the other two optically pure amino alcohols((S)-phenylpropanol,(R)-phenylpropanol)can only obtain optically pure axially chiral and chiral products 5 and 6,respectively,maintaining the configuration of the raw amino alcohol and no non axial chiral isomer is observed.The product using(±)-2-aminobutanol as the raw material cannot be determined for its absolute configuration as a single crystal of the product has not been obtained.
文摘The effects of peptides, amino acids and organic bases as axial ligands on reaction activities in the electrocarboxylation of benzyl chloride with CO2 catalyzed by CoTPP are reported. Imidazole, peptide containing -SH and amino acid containing imi dazyl can enhance the catalytic activity. As an axial ligand, imidazole is the best one, it can make the current efficency of electrocarboxylation catalyzed by CoTPP rising about 23%. The effects of different amount of imidazole on CoTPP’s catalytic activities have been studied, and the cause of these effects have been explaind predrinarily.
