It is generally recognized that internal-loop reactors are well-developed mass and heat-transfer multiphase flow reactors. However, the internal flow field in the internal-loop reactor is influenced by the structure p...It is generally recognized that internal-loop reactors are well-developed mass and heat-transfer multiphase flow reactors. However, the internal flow field in the internal-loop reactor is influenced by the structure parameter of the reactor, which has a great effect on the reaction efficiency. In this study, the computational fluid dynamics simulation method was used to determine the influence of reactor structure on flow field, and a volume-offluid model was employed to simulate the gas–liquid, two-phase flow of the internal-loop micro-electrolysis reactor. Hydrodynamic factors were optimized when the height-to-diameter ratio was 4:1, diameter ratio was9:1, draft-tube axial height was 90 mm. Three-dimensional simulations for the water distributor were carried out, and the results suggested that the optimal conditions are as follows: the number of water distribution pipes was four, and an inhomogeneous water distribution was used. According to the results of the simulation,the suitable structure can be used to achieve good fluid mechanical properties, such as the good liquid circulation velocity and gas holdup, which provides a good theoretical foundation for the application of the reactor.展开更多
The nitrate nitrogen removal efficiency of iron-carbon micro-electrolysis system was discussed in treating pharmaceutical wastewater with high nitrogen and refractory organic concentration. The results show that the g...The nitrate nitrogen removal efficiency of iron-carbon micro-electrolysis system was discussed in treating pharmaceutical wastewater with high nitrogen and refractory organic concentration. The results show that the granularity of fillings,pH,volume ratios of iron-carbon and gas-water,and HRT. have significant effects on the nitrogen removal efficiency of iron-carbon micro-electrolysis system. The iron-carbon micro-electrolysis system has a good removal efficiency of pharmaceutical wastewater with high nitrogen and refractory organic concentration when the influent TN,NH4+-N,NO3--N and BOD5/CODCr are 823 mg/L,30 mg/L,793 mg/L and 0.1,respectively,at the granularity of iron and carbon 0.425 mm,pH 3,iron-carbon ratio 3,gas-water ratio 5,HRT 1.5 h,and the removal rates of TN,NH4+-N and NO3--N achieve 51.5%,70% and 50.94%,respectively.展开更多
The zero valent iron/granular active carbon(ZVI/GAC) micro-electrolysis enhanced by ultrasound(US) coupled with hydrogen peroxide(H_2O_2) was investigated for the deep degradation of nitrobenzene-containing wastewater...The zero valent iron/granular active carbon(ZVI/GAC) micro-electrolysis enhanced by ultrasound(US) coupled with hydrogen peroxide(H_2O_2) was investigated for the deep degradation of nitrobenzene-containing wastewater. The results of scanning electron microscopy-energy dispersive X-rays analysis(SEM-EDS) demonstrated that continuously accelerated regeneration of ZVI and GAC in situ by US could improve the process for converting nitrobenzene(NB) to aniline(AN). H_2O_2 was decomposed catalytically by the byproduct Fe^(2+) ions generated in the micro-electrolysis process to hydroxyl radicals and the organic pollutants in the wastewater were finally mineralized to CO2 and H2O. Effects of the ZVI dosage, the ZVI/GAC mass ratio, the initial pH value and the H_2O_2 dosage on the efficiency for degradation of NB were studied in these experiments. The optimal operating conditions covered a ZVI dosage of 15 g/L, a ZVI/GAC mass ratio of 1:2,an initial pH value of 3 and a H_2O_2 dosage of 4 mL. In this case, the NB removal efficiency reached 97.72% and the total organic carbon(TOC) removal efficiency reached 73.42% at a NB concentration of 300 mg/L. The reduction of NB by USZVI/GAC followed the pseudo-first-order kinetics model, and the pseudo-first-order rate constants were given at different initial pH values. The reaction intermediates such as AN, benzoquinonimine, p-benzoquinone, p-nitrophenol and other organic acids were detected and a probable pathway for NB degradation has been proposed.展开更多
A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost ...A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.展开更多
Rational regulation on pore structure and active site density plays critical roles in enhancing the performance of Fe-N-C catalysts. As the microporous structure of the carbon substrate is generally regarded as the ac...Rational regulation on pore structure and active site density plays critical roles in enhancing the performance of Fe-N-C catalysts. As the microporous structure of the carbon substrate is generally regarded as the active site hosts, its hostility to electron/mass transfer could lead to the incomplete fulfillment of the catalytic activity. Besides, the formation of inactive metallic Fe particles during the conventional catalyst synthesis could also decrease the active site density and complicate the identification of real active site. Herein, we developed a facial hydrogen etching methodology to yield single site Fe-N-C catalysts featured with micro/mesoporous hierarchical structure. The hydrogen concentration in pyrolysis process was designated to effectively regulate the pore structure and active site density of the resulted catalysts.The optimized sample achieves excellent ORR catalytic performance with an ultralow H2O2 yield(1%)and superb stability over 10,000 cycles. Our finding provides new thoughts for the rational design of hierarchically porous carbon-based materials and highly promising non-precious metal ORR catalysts.展开更多
基金Supported by the National Natural Science Foundation of China(21677018)Jointly Projects of Beijing Natural Science Foundation and Beijing Municipal Education Commission(KZ201810017024)
文摘It is generally recognized that internal-loop reactors are well-developed mass and heat-transfer multiphase flow reactors. However, the internal flow field in the internal-loop reactor is influenced by the structure parameter of the reactor, which has a great effect on the reaction efficiency. In this study, the computational fluid dynamics simulation method was used to determine the influence of reactor structure on flow field, and a volume-offluid model was employed to simulate the gas–liquid, two-phase flow of the internal-loop micro-electrolysis reactor. Hydrodynamic factors were optimized when the height-to-diameter ratio was 4:1, diameter ratio was9:1, draft-tube axial height was 90 mm. Three-dimensional simulations for the water distributor were carried out, and the results suggested that the optimal conditions are as follows: the number of water distribution pipes was four, and an inhomogeneous water distribution was used. According to the results of the simulation,the suitable structure can be used to achieve good fluid mechanical properties, such as the good liquid circulation velocity and gas holdup, which provides a good theoretical foundation for the application of the reactor.
基金Project(2009ZX07315-005) supported by the National Water Pollution Controlled and Treatment Great Special of China
文摘The nitrate nitrogen removal efficiency of iron-carbon micro-electrolysis system was discussed in treating pharmaceutical wastewater with high nitrogen and refractory organic concentration. The results show that the granularity of fillings,pH,volume ratios of iron-carbon and gas-water,and HRT. have significant effects on the nitrogen removal efficiency of iron-carbon micro-electrolysis system. The iron-carbon micro-electrolysis system has a good removal efficiency of pharmaceutical wastewater with high nitrogen and refractory organic concentration when the influent TN,NH4+-N,NO3--N and BOD5/CODCr are 823 mg/L,30 mg/L,793 mg/L and 0.1,respectively,at the granularity of iron and carbon 0.425 mm,pH 3,iron-carbon ratio 3,gas-water ratio 5,HRT 1.5 h,and the removal rates of TN,NH4+-N and NO3--N achieve 51.5%,70% and 50.94%,respectively.
基金supported by the Natural Science Foundation of China (U1610106)the Excellent Youth Science and Technology Foundation of Province Shanxi of China (2014021007)+1 种基金the Specialized Research Fund for Sanjin Scholars Pragram of Shanxi Prouince (201707)the North University of China Fund for Distinguished Young Scholars (201701)
文摘The zero valent iron/granular active carbon(ZVI/GAC) micro-electrolysis enhanced by ultrasound(US) coupled with hydrogen peroxide(H_2O_2) was investigated for the deep degradation of nitrobenzene-containing wastewater. The results of scanning electron microscopy-energy dispersive X-rays analysis(SEM-EDS) demonstrated that continuously accelerated regeneration of ZVI and GAC in situ by US could improve the process for converting nitrobenzene(NB) to aniline(AN). H_2O_2 was decomposed catalytically by the byproduct Fe^(2+) ions generated in the micro-electrolysis process to hydroxyl radicals and the organic pollutants in the wastewater were finally mineralized to CO2 and H2O. Effects of the ZVI dosage, the ZVI/GAC mass ratio, the initial pH value and the H_2O_2 dosage on the efficiency for degradation of NB were studied in these experiments. The optimal operating conditions covered a ZVI dosage of 15 g/L, a ZVI/GAC mass ratio of 1:2,an initial pH value of 3 and a H_2O_2 dosage of 4 mL. In this case, the NB removal efficiency reached 97.72% and the total organic carbon(TOC) removal efficiency reached 73.42% at a NB concentration of 300 mg/L. The reduction of NB by USZVI/GAC followed the pseudo-first-order kinetics model, and the pseudo-first-order rate constants were given at different initial pH values. The reaction intermediates such as AN, benzoquinonimine, p-benzoquinone, p-nitrophenol and other organic acids were detected and a probable pathway for NB degradation has been proposed.
基金financially supported by the National Natural Science Foundation of China (Nos. 21601098 and 51602167)Shandong Provincial Science Foundation (ZR2016EMB07 and ZR2017JL021)+1 种基金Key Research and Development Program (2018GGX102033)Qingdao Applied Fundamental Research Project (16-5-1-92-jch and 17-1-1-81-jch)
文摘A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.
基金supported by the National Natural Science Foundation of China(21633008,21433003,U1601211,21733004)National Science and Technology Major Project(2016YFB0101202)+1 种基金Jilin Province Science and Technology Development Program(20150101066JC,20160622037JC,20170203003SF,20170520150JH)Hundred Talents Program of Chinese Academy of Sciences and the Recruitment Program of Foreign Experts(WQ20122200077)
文摘Rational regulation on pore structure and active site density plays critical roles in enhancing the performance of Fe-N-C catalysts. As the microporous structure of the carbon substrate is generally regarded as the active site hosts, its hostility to electron/mass transfer could lead to the incomplete fulfillment of the catalytic activity. Besides, the formation of inactive metallic Fe particles during the conventional catalyst synthesis could also decrease the active site density and complicate the identification of real active site. Herein, we developed a facial hydrogen etching methodology to yield single site Fe-N-C catalysts featured with micro/mesoporous hierarchical structure. The hydrogen concentration in pyrolysis process was designated to effectively regulate the pore structure and active site density of the resulted catalysts.The optimized sample achieves excellent ORR catalytic performance with an ultralow H2O2 yield(1%)and superb stability over 10,000 cycles. Our finding provides new thoughts for the rational design of hierarchically porous carbon-based materials and highly promising non-precious metal ORR catalysts.
