Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst...Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst(T-202) were studied in a continuous flow fixed bed reactor under pressures of 1.6-2.8 MPa, space time of 1.32-3.55 s and temperatures of 240-360 °C. Though the COG contains about 0.6 mol/mol H2, hydrogenation of CO and CO2 is not significant on this catalyst. The conversions of unsaturated hydrocarbons depend on their molecular structures. Diolefins and alkynes can be completely hydrogenated even at relatively low temperature and pressure. Olefins, in contrast, can only be progressively hydrogenated with increasing temperature and pressure. The hydrodesulfurization(HDS) of CS2 on this catalyst is easy. Complete conversion of CS2 was observed in the whole range of the conditions used in this work. The original COS in the COG can also be easily converted to a low level. However, its complete HDS is difficult due to the relatively high concentration of CO in the COG and due to the limitation of thermodynamics. H2 S can react with unsaturated hydrocarbons to form ethyl mercaptan and thiophene, which are then progressively hydrodesulfurized with increasing temperature and pressure. Based on the experimental observations, reaction kinetic models for the conversion of ethylene and sulfur-containing compounds were proposed; the values of the parameters in the models were obtained by regression of the experimental data.展开更多
A new technology was developed to recover multiple valuable elements from the spent Al2O3-based catalyst by X-ray phase analysis and exploratory experiments. The experimental results show that in the condition of roas...A new technology was developed to recover multiple valuable elements from the spent Al2O3-based catalyst by X-ray phase analysis and exploratory experiments. The experimental results show that in the condition of roasting temperature of 750℃ and roasting time of 30 min, molar ratio of Na2O to Al2O3 of 1.2, the leaching rates of alumina, vanadium and molybdenum in the spent catalyst are 97.2%, 95.8% and 98.9%, respectively. Vanadium and molybdenum in sodium aluminate solution can be recovered by precipitators A and B, and the precipitation rates of vanadium and molybdenum are 94.8% and 92.6%. Al（OH）3 was prepared from sodium aluminate solution in the carbonation decomposition process, and the purity of Al2O3 is 99.9% after calcination, the recovery of alumina reaches 90.6% in the whole process; the Ni-Co concentrate was leached by sulfuric acid, a nickel recovery of 98.2% and cobalt recovery over 98.5% can be obtained under the experimental condition of 30% H2SO4, 80℃, reaction time 4 h, mass ratio of liquid to solid 8, stirring rate 800r/min.展开更多
The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influen...The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influenced by the morphology of the support.Hydrothermal synthesis was employed to produce different morphologies ofγ-Al_(2)O_(3):flower-likeγ-Al_(2)O_(3)(f)exposing(110)crystal faces,sheet-likeγ-Al_(2)O_(3)(s)revealing(100)crystal faces,and rod-likeγ-Al_(2)O_(3)(r)displaying(111)crystal faces,followed by loading PtCo nanoparticles.The exposed crystal faces of the support impact the alloying degree of the PtCo nanoparticles,and an increase in the alloying degree correlates with enhanced catalyst reactivity.Pt_(3)Co intermetallic compounds were identified onγ-Al_(2)O_(3)(f)exposing(110)crystal faces,and PtCo/γ-Al_(2)O_(3)(f)showed high catalytic activity in the CO-PROX reaction,achieving 100%CO conversion across a broad temperature range of 50−225°C.In contrast,only partial alloying of PtCo was observed onγ-Al_(2)O_(3)(s).Furthermore,no alloying between Pt and Co occurred in PtCo/γ-Al_(2)O_(3)(r),resulting in a reaction rate at 50°C that was merely 11%of that of PtCo/γ-Al_(2)O_(3)(f).The formation of Pt3Co intermetallic compounds led to a more oxidized state of Pt,which significantly diminished the adsorption of CO on Pt and augmented the active oxygen species,thereby facilitating the selective oxidation of CO.展开更多
A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evo...A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evolution rates of 112.2 and 5.5µmol·g^(-1)·h^(-1),respectively,representing 6.3-fold and 3.9-fold enhancements over pristine BiOBr.The heterojunction demonstrated broadened light absorption,enhanced photoelectrochemical activity,reduced charge-transfer resistance,and improved separation efficiency of photogenerated carriers(e^(-)/h^(+)).These synergistic effects were attributed to the formation of a Z-scheme heterostructure,which facilitated solar energy utilization and electron reduction capacity while suppressing carrier recombination.展开更多
Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge....Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge. The experimental results were assessed in terms of total organic carbon（TOC） reduction. The operational and reaction conditions affecting the efficiencies of TOC removal such as initial pH value, H2O2 concentration, catalyst loading and UV power were studied. The results show that TOC is reduced from 347.6 mg/L to 10.8 mg/L, color is changed from 500 units to 0 under the conditions as follows： initial pH value 6. 0, H2O2 concentration of 1. 000 g/L, catalyst loading of 5 g/L, reaction duration of 120 rain and reaction temperature of 30 ℃. The irradiated Ce-Fe/Al2O3 catalyst was complexed with 1,10-phenanthroline and then it was subjected to Fourier transform infrared spectroscopy and diffuse reflectance spectroscopy to confirm the formation of Fe（Ⅱ） in the solid state. Heterogeneous photo-Fenton reaction proves to be effective for the treatment of yeast wastewater.展开更多
High-temperature Ni-based alloys are widely used in the aerospace field due to their excellent properties,but the shortcomings of brittle fracture at the grain boundaries and poor plasticity at room temperature also l...High-temperature Ni-based alloys are widely used in the aerospace field due to their excellent properties,but the shortcomings of brittle fracture at the grain boundaries and poor plasticity at room temperature also limit their development to a certain extent.Researchers found that there areγ′precipitation phases similar to Ni_(3)Al in Pt-Al based alloys.In this paper,the CASTEP code of Materials Studio software package is used to simulate the thermal and mechanical properties ofγ′-Pt_(3)Al phase andγ′-Ni_(3)Al phase.By comparing the performance characteristics of the electronic structure,mechanical properties and point defect structure of the two,it is found that the stability,elastic deformation resistance and high temperature creep resistance of theγ′-Pt_(3)Al phase are better than those of theγ′-Ni_(3)Al phase.This will provide theoretical guidance for promoting the development of Pt-Al-based high-temperature materials.展开更多
文摘Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst(T-202) were studied in a continuous flow fixed bed reactor under pressures of 1.6-2.8 MPa, space time of 1.32-3.55 s and temperatures of 240-360 °C. Though the COG contains about 0.6 mol/mol H2, hydrogenation of CO and CO2 is not significant on this catalyst. The conversions of unsaturated hydrocarbons depend on their molecular structures. Diolefins and alkynes can be completely hydrogenated even at relatively low temperature and pressure. Olefins, in contrast, can only be progressively hydrogenated with increasing temperature and pressure. The hydrodesulfurization(HDS) of CS2 on this catalyst is easy. Complete conversion of CS2 was observed in the whole range of the conditions used in this work. The original COS in the COG can also be easily converted to a low level. However, its complete HDS is difficult due to the relatively high concentration of CO in the COG and due to the limitation of thermodynamics. H2 S can react with unsaturated hydrocarbons to form ethyl mercaptan and thiophene, which are then progressively hydrodesulfurized with increasing temperature and pressure. Based on the experimental observations, reaction kinetic models for the conversion of ethylene and sulfur-containing compounds were proposed; the values of the parameters in the models were obtained by regression of the experimental data.
基金Project(2003 UDBEA00C020) supported by the Collaborative Project of School and Province of Yunnan Province
文摘A new technology was developed to recover multiple valuable elements from the spent Al2O3-based catalyst by X-ray phase analysis and exploratory experiments. The experimental results show that in the condition of roasting temperature of 750℃ and roasting time of 30 min, molar ratio of Na2O to Al2O3 of 1.2, the leaching rates of alumina, vanadium and molybdenum in the spent catalyst are 97.2%, 95.8% and 98.9%, respectively. Vanadium and molybdenum in sodium aluminate solution can be recovered by precipitators A and B, and the precipitation rates of vanadium and molybdenum are 94.8% and 92.6%. Al（OH）3 was prepared from sodium aluminate solution in the carbonation decomposition process, and the purity of Al2O3 is 99.9% after calcination, the recovery of alumina reaches 90.6% in the whole process; the Ni-Co concentrate was leached by sulfuric acid, a nickel recovery of 98.2% and cobalt recovery over 98.5% can be obtained under the experimental condition of 30% H2SO4, 80℃, reaction time 4 h, mass ratio of liquid to solid 8, stirring rate 800r/min.
基金supported by the National Natural Science Foundation of China(22376063,21976057)the Fund of the National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2020A05)Fundamental Research Funds for the Central Universities.
文摘The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influenced by the morphology of the support.Hydrothermal synthesis was employed to produce different morphologies ofγ-Al_(2)O_(3):flower-likeγ-Al_(2)O_(3)(f)exposing(110)crystal faces,sheet-likeγ-Al_(2)O_(3)(s)revealing(100)crystal faces,and rod-likeγ-Al_(2)O_(3)(r)displaying(111)crystal faces,followed by loading PtCo nanoparticles.The exposed crystal faces of the support impact the alloying degree of the PtCo nanoparticles,and an increase in the alloying degree correlates with enhanced catalyst reactivity.Pt_(3)Co intermetallic compounds were identified onγ-Al_(2)O_(3)(f)exposing(110)crystal faces,and PtCo/γ-Al_(2)O_(3)(f)showed high catalytic activity in the CO-PROX reaction,achieving 100%CO conversion across a broad temperature range of 50−225°C.In contrast,only partial alloying of PtCo was observed onγ-Al_(2)O_(3)(s).Furthermore,no alloying between Pt and Co occurred in PtCo/γ-Al_(2)O_(3)(r),resulting in a reaction rate at 50°C that was merely 11%of that of PtCo/γ-Al_(2)O_(3)(f).The formation of Pt3Co intermetallic compounds led to a more oxidized state of Pt,which significantly diminished the adsorption of CO on Pt and augmented the active oxygen species,thereby facilitating the selective oxidation of CO.
文摘A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evolution rates of 112.2 and 5.5µmol·g^(-1)·h^(-1),respectively,representing 6.3-fold and 3.9-fold enhancements over pristine BiOBr.The heterojunction demonstrated broadened light absorption,enhanced photoelectrochemical activity,reduced charge-transfer resistance,and improved separation efficiency of photogenerated carriers(e^(-)/h^(+)).These synergistic effects were attributed to the formation of a Z-scheme heterostructure,which facilitated solar energy utilization and electron reduction capacity while suppressing carrier recombination.
基金Project(20277010) supported by the National Natural Science Foundation of China
文摘Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge. The experimental results were assessed in terms of total organic carbon（TOC） reduction. The operational and reaction conditions affecting the efficiencies of TOC removal such as initial pH value, H2O2 concentration, catalyst loading and UV power were studied. The results show that TOC is reduced from 347.6 mg/L to 10.8 mg/L, color is changed from 500 units to 0 under the conditions as follows： initial pH value 6. 0, H2O2 concentration of 1. 000 g/L, catalyst loading of 5 g/L, reaction duration of 120 rain and reaction temperature of 30 ℃. The irradiated Ce-Fe/Al2O3 catalyst was complexed with 1,10-phenanthroline and then it was subjected to Fourier transform infrared spectroscopy and diffuse reflectance spectroscopy to confirm the formation of Fe（Ⅱ） in the solid state. Heterogeneous photo-Fenton reaction proves to be effective for the treatment of yeast wastewater.
文摘High-temperature Ni-based alloys are widely used in the aerospace field due to their excellent properties,but the shortcomings of brittle fracture at the grain boundaries and poor plasticity at room temperature also limit their development to a certain extent.Researchers found that there areγ′precipitation phases similar to Ni_(3)Al in Pt-Al based alloys.In this paper,the CASTEP code of Materials Studio software package is used to simulate the thermal and mechanical properties ofγ′-Pt_(3)Al phase andγ′-Ni_(3)Al phase.By comparing the performance characteristics of the electronic structure,mechanical properties and point defect structure of the two,it is found that the stability,elastic deformation resistance and high temperature creep resistance of theγ′-Pt_(3)Al phase are better than those of theγ′-Ni_(3)Al phase.This will provide theoretical guidance for promoting the development of Pt-Al-based high-temperature materials.
