Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochem...Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochemical methods with only several reports.This study pioneers an electrocatalytic strategy for the efficient synthesis of THFDCA via the oxidation of tetrahydrofuran dimethanol(THFDM).By constructing NiCo bimetallic oxides micron sheets on nickel foam(NiCoMS/NF)through controlled pyrolysis of a metal-organic framework(MOF)-like precursor,we achieved a remarkable THFDM conversion of 99.0%and THFDCA yield up to 98.2%,surpassing all reports on thermocatalytic oxidation as we know.In-depth analysis revealed that the synergistic effect between NiO and Co_(3)O_(4) contributes to the high catalytic performance.In-situ Raman and rotating ring-disk electrode(RRDE)techniques were employed to discuss the reaction mechanism and the inhibitory effect on oxygen evolution reaction(OER).This study not only provides a paradigm-shifting,groundbreaking strategy for the synthesis of the flexible cyclic dicarboxylic acid derived from furanic biomass but also offers deep insights into the synergistic effects of electrocatalysts.展开更多
The electrolysis of catechol was studied in the pH values of 1 to 10. The results from the rotating ring disk electrode (RRDE) experiments show that at low pH values, the electrochemical polymerization of catechol wa...The electrolysis of catechol was studied in the pH values of 1 to 10. The results from the rotating ring disk electrode (RRDE) experiments show that at low pH values, the electrochemical polymerization of catechol was performed by one step, and at higher pH values, the electrochemical polymerization of catechol was carried out by two steps, i.e . oxidation of catechol and followed by polymerization. The intermediates generated at the disk were detected at the ring electrode in the ring potential region of -0.2 to 0 V (vs. Ag/AgCl). One of reasons for the decrease in the ratio of i r to i d with increasing the ring potential is caused by formation of positively charged intermediates at the disk electrode. This ratio increases with increasing the rotation rate of the RRDE, which indicates that the intermediates are not stable. A shielding effect during polymerization of catechol was observed when the ring potential was set at 0.1 V (vs. Ag/AgCl). The electron spin resonance (ESR) of polycatechol shows that polycatechol possesses unpaired electrons. The images of polycatechol films synthesized at different conditions are described.展开更多
The relationship between gas pressure drop and gas resistance coefficient versus operation condition and gas phase Reynolds number in three packing plate distance was theoretically analyzed and experimentally measured...The relationship between gas pressure drop and gas resistance coefficient versus operation condition and gas phase Reynolds number in three packing plate distance was theoretically analyzed and experimentally measured in the centrifugal field.The experimental results show that packing plate distance has a great influence on gas phase resistance and too small distance makes liquid clogging and causes great gas phase resistance.The fitness distance of the packing plate is large than 3.1 mm under the operation condition in this paper.展开更多
The cathodic reduction mechanism of MnO2 electrode is studied by means of the rotating ring-disk electrode. The mass transport process in the solution plays an important role in the reduction process of MnO2 electrode...The cathodic reduction mechanism of MnO2 electrode is studied by means of the rotating ring-disk electrode. The mass transport process in the solution plays an important role in the reduction process of MnO2 electrode. The relation between IR-1 and ω-1/2 is deduced as a diagnostic criterion of the reduction medianism. The dissolutionprecipitation and the electron-proton mechanism occur simultaneously but the relative contributions are qulte different in various pH value solutions.展开更多
基金supported by the National Natural Science Foundation of China(22072170,U23A20125)the President Foundation of Ningbo Institute of Materials Technology and Engineering。
文摘Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochemical methods with only several reports.This study pioneers an electrocatalytic strategy for the efficient synthesis of THFDCA via the oxidation of tetrahydrofuran dimethanol(THFDM).By constructing NiCo bimetallic oxides micron sheets on nickel foam(NiCoMS/NF)through controlled pyrolysis of a metal-organic framework(MOF)-like precursor,we achieved a remarkable THFDM conversion of 99.0%and THFDCA yield up to 98.2%,surpassing all reports on thermocatalytic oxidation as we know.In-depth analysis revealed that the synergistic effect between NiO and Co_(3)O_(4) contributes to the high catalytic performance.In-situ Raman and rotating ring-disk electrode(RRDE)techniques were employed to discuss the reaction mechanism and the inhibitory effect on oxygen evolution reaction(OER).This study not only provides a paradigm-shifting,groundbreaking strategy for the synthesis of the flexible cyclic dicarboxylic acid derived from furanic biomass but also offers deep insights into the synergistic effects of electrocatalysts.
基金ProjectsupportedbytheNationalNaturalScienceFoundationofChina (No .2 0 0 740 2 7)
文摘The electrolysis of catechol was studied in the pH values of 1 to 10. The results from the rotating ring disk electrode (RRDE) experiments show that at low pH values, the electrochemical polymerization of catechol was performed by one step, and at higher pH values, the electrochemical polymerization of catechol was carried out by two steps, i.e . oxidation of catechol and followed by polymerization. The intermediates generated at the disk were detected at the ring electrode in the ring potential region of -0.2 to 0 V (vs. Ag/AgCl). One of reasons for the decrease in the ratio of i r to i d with increasing the ring potential is caused by formation of positively charged intermediates at the disk electrode. This ratio increases with increasing the rotation rate of the RRDE, which indicates that the intermediates are not stable. A shielding effect during polymerization of catechol was observed when the ring potential was set at 0.1 V (vs. Ag/AgCl). The electron spin resonance (ESR) of polycatechol shows that polycatechol possesses unpaired electrons. The images of polycatechol films synthesized at different conditions are described.
文摘The relationship between gas pressure drop and gas resistance coefficient versus operation condition and gas phase Reynolds number in three packing plate distance was theoretically analyzed and experimentally measured in the centrifugal field.The experimental results show that packing plate distance has a great influence on gas phase resistance and too small distance makes liquid clogging and causes great gas phase resistance.The fitness distance of the packing plate is large than 3.1 mm under the operation condition in this paper.
文摘The cathodic reduction mechanism of MnO2 electrode is studied by means of the rotating ring-disk electrode. The mass transport process in the solution plays an important role in the reduction process of MnO2 electrode. The relation between IR-1 and ω-1/2 is deduced as a diagnostic criterion of the reduction medianism. The dissolutionprecipitation and the electron-proton mechanism occur simultaneously but the relative contributions are qulte different in various pH value solutions.