The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation ...The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.展开更多
A series of Ag,Cu and Co-doped manganese oxide octahedral molecular sieves(OMS-2) were synthesized and evaluated to remove nitrogen oxides(NOx) from cigarette mainstream smoke.The three kinds of catalysts were added t...A series of Ag,Cu and Co-doped manganese oxide octahedral molecular sieves(OMS-2) were synthesized and evaluated to remove nitrogen oxides(NOx) from cigarette mainstream smoke.The three kinds of catalysts were added to cigarettes for studying the capabilities of reducing NOx from cigarette mainstream smoke.The catalysis and reduction of NO in laboratory were studied.A mechanism for NOx catalytic reduction from burning cigarettes with the catalysts adding to cigarettes was described.The catalysts show excellent catalytic activity for NOx removal,especially the Ag-doped OMS-2 catalyst.0.5%(mass fraction) Ag-doped OMS-2 catalyst has the best ability to remove NOx from cigarette mainstream smoke.The use of Ag-doped OMS-2 as catalyst for removing carcinogenic compounds from cigarette smoke will be an effective strategy to protect the environment and public health.展开更多
The effects of NOx(in a ratio of NO∶NO2=9∶1) and SO2in cathode streamonthe performance of a single proton ex-change membrane fuel cell(PEMFC) were investigated.NOxwith concentrations of 1×10-3%(in volume,the sa...The effects of NOx(in a ratio of NO∶NO2=9∶1) and SO2in cathode streamonthe performance of a single proton ex-change membrane fuel cell(PEMFC) were investigated.NOxwith concentrations of 1×10-3%(in volume,the same as fol-lows),1.4×10-2%and 1×10-3%could cause significant detri mental effects on the cell performance.However,nearly com-plete recovery of the cell performance could be observed after NOxwas shut off and purged with clean air.The electrochemicalmeasurements suggested that thei mpacts of NOxresulted mainlyfromthe superposition of the oxygen reduction reaction(ORR),NOand HNO2oxidation reactions,and the increased cathodic i mpedance.Trace SO2with concentrations of 5×10-6%,5×10-3%,2×10-4%and 3.2×10-4%influenced the cell muchseverer,which could be attributed toits strong adsorption onthesurface of Pt atoms.The cell performance could not be completely recovered after purged with clean air and cyclic voltammetry(CV) tests,due to the changes of electrochemical i mpedance spectroscopy(EIS) and electrochemical active surface(EAS) causedby surface state change after SO2exposure.展开更多
A solution of 0.1 mol/L to 1.0 mol/L H2SO4 can dissolve alkali metals and alkaline earth metals which weaken an active site of SCR catalyst. The waste catalyst washed with 0.5 mol/L H2SO4 regained the best catalytic a...A solution of 0.1 mol/L to 1.0 mol/L H2SO4 can dissolve alkali metals and alkaline earth metals which weaken an active site of SCR catalyst. The waste catalyst washed with 0.5 mol/L H2SO4 regained the best catalytic activity. When a concentration of the sulfuric acid is less than 0.5 mol/L, sufficient cleaning effects cannot be obtained. In contrast, when the concentration is greater than 1.0 tool/L, the active components, vanadium and tungsten are undesirably eluted. The total BET surface of the catalyst regenerated by air lift loop reactor showed almost the same as that of fresh catalyst due to the removal of insoluble compounds which may be penetrated into pores of catalyst. The addition of a solution of 0.075 mol/L ammonium vanadate （NHnVO3） and 0.075 mol/L ammonium paratungstate （5（NH4）20· 12WO3-5H20） to 0.1 mol/L H2SO4 significantly increases the activity of the waste catalyst.展开更多
Process control is an effective approach to reduce the NO_(x) emission from sintering flue gas.The effects of different materials adhered on coke breeze on NO_(x) emission characteristics and sintering performance wer...Process control is an effective approach to reduce the NO_(x) emission from sintering flue gas.The effects of different materials adhered on coke breeze on NO_(x) emission characteristics and sintering performance were studied.Results showed that the coke breeze adhered with the mixture of CaO and Fe_(2)O_(3) or calcium ferrite significantly lowers the NO_(x) emission concentration and conversion ratio of fuel-N to NO_(x).Pretreating the coke with the mixture of lime slurry and iron ore fines helped to improve the granulation effect,and optimize the carbon distribution in granules.When the mass ratio of coke breeze,quick lime,water and iron ore fines was 2:1:1:1,the average NO_(x) emission concentration was decreased from 220 mg/m^(3) to 166 mg/m^(3),and the conversion ratio of fuel-N was reduced from 54.2%to 40.9%.展开更多
The unburned carbon concentration in fly ash and the influence of main factors on the reduction of nitrogen oxides during gaseous fuel reburning process were experimentally studied in a 36 kW down-fired furnace when f...The unburned carbon concentration in fly ash and the influence of main factors on the reduction of nitrogen oxides during gaseous fuel reburning process were experimentally studied in a 36 kW down-fired furnace when five typical coals with different qualities were served as the primary fuel. It is found that the higher nitrogen oxide reduction efficiency can be obtained by reburning process when the coal used as the primary fuel contains more volatile matter. But under the optimizational operating conditions, both above 50% nitrogen oxide reduction and low carbon loss can be achieved by reburning process even though the primary fuel is the low-volatile coal. The experimental results show that the reasonable residence time in reburn zone is 0.6-0.9 s, the appropriate gaseous reburn fuel percentage is 10%-15% and the optimal average excess air coefficient in reburn zone is 0.8-0.9. These results extend the ranges of the key parameter values for reburning process with respect to that the low-volatile coals are used as the primary fuel.展开更多
基金supported by Natural Science Foundation of Shandong Province(ZR2021MB075)Fundamental Research Funds for the Central Universities,Ocean University of China(202461021).
文摘The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.
文摘A series of Ag,Cu and Co-doped manganese oxide octahedral molecular sieves(OMS-2) were synthesized and evaluated to remove nitrogen oxides(NOx) from cigarette mainstream smoke.The three kinds of catalysts were added to cigarettes for studying the capabilities of reducing NOx from cigarette mainstream smoke.The catalysis and reduction of NO in laboratory were studied.A mechanism for NOx catalytic reduction from burning cigarettes with the catalysts adding to cigarettes was described.The catalysts show excellent catalytic activity for NOx removal,especially the Ag-doped OMS-2 catalyst.0.5%(mass fraction) Ag-doped OMS-2 catalyst has the best ability to remove NOx from cigarette mainstream smoke.The use of Ag-doped OMS-2 as catalyst for removing carcinogenic compounds from cigarette smoke will be an effective strategy to protect the environment and public health.
文摘The effects of NOx(in a ratio of NO∶NO2=9∶1) and SO2in cathode streamonthe performance of a single proton ex-change membrane fuel cell(PEMFC) were investigated.NOxwith concentrations of 1×10-3%(in volume,the same as fol-lows),1.4×10-2%and 1×10-3%could cause significant detri mental effects on the cell performance.However,nearly com-plete recovery of the cell performance could be observed after NOxwas shut off and purged with clean air.The electrochemicalmeasurements suggested that thei mpacts of NOxresulted mainlyfromthe superposition of the oxygen reduction reaction(ORR),NOand HNO2oxidation reactions,and the increased cathodic i mpedance.Trace SO2with concentrations of 5×10-6%,5×10-3%,2×10-4%and 3.2×10-4%influenced the cell muchseverer,which could be attributed toits strong adsorption onthesurface of Pt atoms.The cell performance could not be completely recovered after purged with clean air and cyclic voltammetry(CV) tests,due to the changes of electrochemical i mpedance spectroscopy(EIS) and electrochemical active surface(EAS) causedby surface state change after SO2exposure.
基金Project(2009T100100602) supported by the Korea Institute of Energy Technology Evaluation and Planning,Korea
文摘A solution of 0.1 mol/L to 1.0 mol/L H2SO4 can dissolve alkali metals and alkaline earth metals which weaken an active site of SCR catalyst. The waste catalyst washed with 0.5 mol/L H2SO4 regained the best catalytic activity. When a concentration of the sulfuric acid is less than 0.5 mol/L, sufficient cleaning effects cannot be obtained. In contrast, when the concentration is greater than 1.0 tool/L, the active components, vanadium and tungsten are undesirably eluted. The total BET surface of the catalyst regenerated by air lift loop reactor showed almost the same as that of fresh catalyst due to the removal of insoluble compounds which may be penetrated into pores of catalyst. The addition of a solution of 0.075 mol/L ammonium vanadate （NHnVO3） and 0.075 mol/L ammonium paratungstate （5（NH4）20· 12WO3-5H20） to 0.1 mol/L H2SO4 significantly increases the activity of the waste catalyst.
基金Project(2017YFC0210302)supported by the National Key R&D Program of ChinaProjects(U1660206,U1760107)supported by the National Natural Science Foundation of China
文摘Process control is an effective approach to reduce the NO_(x) emission from sintering flue gas.The effects of different materials adhered on coke breeze on NO_(x) emission characteristics and sintering performance were studied.Results showed that the coke breeze adhered with the mixture of CaO and Fe_(2)O_(3) or calcium ferrite significantly lowers the NO_(x) emission concentration and conversion ratio of fuel-N to NO_(x).Pretreating the coke with the mixture of lime slurry and iron ore fines helped to improve the granulation effect,and optimize the carbon distribution in granules.When the mass ratio of coke breeze,quick lime,water and iron ore fines was 2:1:1:1,the average NO_(x) emission concentration was decreased from 220 mg/m^(3) to 166 mg/m^(3),and the conversion ratio of fuel-N was reduced from 54.2%to 40.9%.
基金Projects(50806025 50721005) supported by the National Natural Science Foundation of China
文摘The unburned carbon concentration in fly ash and the influence of main factors on the reduction of nitrogen oxides during gaseous fuel reburning process were experimentally studied in a 36 kW down-fired furnace when five typical coals with different qualities were served as the primary fuel. It is found that the higher nitrogen oxide reduction efficiency can be obtained by reburning process when the coal used as the primary fuel contains more volatile matter. But under the optimizational operating conditions, both above 50% nitrogen oxide reduction and low carbon loss can be achieved by reburning process even though the primary fuel is the low-volatile coal. The experimental results show that the reasonable residence time in reburn zone is 0.6-0.9 s, the appropriate gaseous reburn fuel percentage is 10%-15% and the optimal average excess air coefficient in reburn zone is 0.8-0.9. These results extend the ranges of the key parameter values for reburning process with respect to that the low-volatile coals are used as the primary fuel.
