The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorp...The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.展开更多
The replacement of energy-intensive Haber-Bosch technique for ammonia production to mitigate global warming is increasingly emphasized.In this paper,we report the preparation of Z-scheme heterojunction nanocomposites ...The replacement of energy-intensive Haber-Bosch technique for ammonia production to mitigate global warming is increasingly emphasized.In this paper,we report the preparation of Z-scheme heterojunction nanocomposites for photocatalytic nitrogen fixation by coupling ultrathin two-dimensional g-C_(3)N_(4) nanosheets with MIL-101(Fe)using a solvothermal method.Methanol was used as a hole sacrificing reagent to strengthen the catalytic performance.The highest NH3 yield of the composites under full spectrum irradiation was 472.8μmol·g^(−1)·h^(−1),which is about 3.5 times that of MIL-101(Fe).From BET results,photocatalyst with high specific surface area has superior nitrogen fixation performance.The results of PL,EIS,UPS,and ESR show that the presence of Z-scheme heterojunction is largely able to facilitate the separation of electrons and holes.It is one reason for improving performance of nitrogen fixation.The study has provided a viable approach to construct heterojunction photocatalysts with outstanding nitrogen fixation performance.展开更多
To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe_(3)O_(4)@SiO_(2)@Fe-MIL...To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe_(3)O_(4)@SiO_(2)@Fe-MIL-101 magnetic composite material was successfully synthesized via the one-pot method.Preparation conditions were optimized and structural characterization of this material conducted using FTIR,SEM,EDS,XRD and Hysteresis analysis.The results show that this composite exhibits a more rapid fluoride adsorption dynamics and a higher fluoride adsorption capacity(18.34 mg/g)and its adsorption behavior fitted for the first order dynamic model and the Freundlich isotherm model.The adsorption of fluorine by this composite is mainly physical adsorption according to the mean adsorption energy(1.216 kJ/mol).The interfering ions co-existed in fluoride-containing solutions,like HCO_(3)^(-),NO^(-)and Cl^(-),have a significant effect on fluorine adsorption.This composite has also been proved with magnetism,higher adsorption selectivity and satisfactory reusability.When this composite is employed as an adsorbent for adsorption removing fluoride in zinc sulfate electrolyte,it exhibits higher pH-dependent behavior as well as high fluoride removal efficiency at pH 6.5.展开更多
基金Supported by Basic Scientific Research Project of the Liaoning Provincial Department of Education Has Been Unveiled to Facilitate Local Project Funding (JYTMS20230835)Enhanced Scientific Research Project Funded by the Departmentof Higher Education in Liaoning Province (General program)(JYTMS20230852)。
文摘The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.
基金financially supported by the Natural Science Foundation of China(22071018)the Natural Science Foundation of Jilin Province(20220101069JC)
文摘The replacement of energy-intensive Haber-Bosch technique for ammonia production to mitigate global warming is increasingly emphasized.In this paper,we report the preparation of Z-scheme heterojunction nanocomposites for photocatalytic nitrogen fixation by coupling ultrathin two-dimensional g-C_(3)N_(4) nanosheets with MIL-101(Fe)using a solvothermal method.Methanol was used as a hole sacrificing reagent to strengthen the catalytic performance.The highest NH3 yield of the composites under full spectrum irradiation was 472.8μmol·g^(−1)·h^(−1),which is about 3.5 times that of MIL-101(Fe).From BET results,photocatalyst with high specific surface area has superior nitrogen fixation performance.The results of PL,EIS,UPS,and ESR show that the presence of Z-scheme heterojunction is largely able to facilitate the separation of electrons and holes.It is one reason for improving performance of nitrogen fixation.The study has provided a viable approach to construct heterojunction photocatalysts with outstanding nitrogen fixation performance.
基金National Natural Science Foundation of China(21865011)2024 Innovation and Entrepreneurship Project of College Student in Jishou University(JDCX20241122)。
文摘To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe_(3)O_(4)@SiO_(2)@Fe-MIL-101 magnetic composite material was successfully synthesized via the one-pot method.Preparation conditions were optimized and structural characterization of this material conducted using FTIR,SEM,EDS,XRD and Hysteresis analysis.The results show that this composite exhibits a more rapid fluoride adsorption dynamics and a higher fluoride adsorption capacity(18.34 mg/g)and its adsorption behavior fitted for the first order dynamic model and the Freundlich isotherm model.The adsorption of fluorine by this composite is mainly physical adsorption according to the mean adsorption energy(1.216 kJ/mol).The interfering ions co-existed in fluoride-containing solutions,like HCO_(3)^(-),NO^(-)and Cl^(-),have a significant effect on fluorine adsorption.This composite has also been proved with magnetism,higher adsorption selectivity and satisfactory reusability.When this composite is employed as an adsorbent for adsorption removing fluoride in zinc sulfate electrolyte,it exhibits higher pH-dependent behavior as well as high fluoride removal efficiency at pH 6.5.
