A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3（NH3-SCR） was determined.The effects of SO2 and H2O,and the...A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3（NH3-SCR） was determined.The effects of SO2 and H2O,and their combined effect,on the activity were examined at 340 ℃ for 24 h.The catalysts were characterized using N2 adsorption-desorption,X-ray diffraction,X-ray photoelectron spectroscopy,temperature-programmed reduction of H2（H2-TPR）,temperature-programmed desorption of NH3（NH3-TPD）,and in situ diffuse-reflectance infrared Fourier-transform spectroscopy（DRIFTS）.The CuSO4/TiO2 catalysts had good activities,with low production of N2O above 340 ℃.SO2 or a combination of SO2 and H2O had little effect on the activity,and H2O caused only a slight decrease in activity during the experimental period.The NH3-TPD and H2-TPR results showed that CuSO4 increased the amounts of acid sites and adsorbed oxygen on the catalyst.In situ DRIFTS showed that the NH3-SCR reaction on the CuSO4/TiO2 catalysts followed an Eley-Rideal mechanism.The reaction of gaseous NO with NH3 adsorbed on Lewis acid sites to form N2 and H2O could be the main reaction pathway,and oxygen adsorption might favor this process.展开更多
We study a model based on precursor mechanism for CO-NO catalytic reaction on square lattice with Monte Carlo simulation. The precursor mechanism clearly demonstrates its impact on the phase diagram. The steady reacti...We study a model based on precursor mechanism for CO-NO catalytic reaction on square lattice with Monte Carlo simulation. The precursor mechanism clearly demonstrates its impact on the phase diagram. The steady reactive state （SRS） gets established. The width of reactive region increases by increasing the range of precursor mobility. When the precursor mobility is increased to third-nearest neighbourhood, the second-order transition disappears.展开更多
Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by N...Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by NH3 at low temperature.Mn((2))Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH(with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction(SCR) catalytic activity,with about 96% NOx conversion at 750 C and-99%in the temperature range from 100 to 250℃.X-ray diffraction(XRD) results showed that Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH catalysts crystallized in the form of Mn2NiO4 and MnO2-Mn2NiO4 spinel,respectively.The latter gave relatively good selectivity to N2,which might be due to the presence of the MnO2 phase and high metal-O binding energy,resulting in low dehydrogenation ability.According to the results of various characterization methods,it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn2NiO4 spinel played important roles in the high-efficiency SCR activity of these catalysts.Mn(2)Ni(1)Ox catalysts presented good resistance to H2O or/and SO2 with stable activity,which benefited from the Mn2NiO4 spinel structure and Eley-Rideal mechanism,with only slight effects from SO2.展开更多
Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction （photo-SCR） with ammonia over TiO2 in this study. NO reduction efficiency and N2 selectivity were determi...Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction （photo-SCR） with ammonia over TiO2 in this study. NO reduction efficiency and N2 selectivity were determined from gases composition at the outlet stream of photoreactor. Effect of operating conditions, e.g. light intensity and inlet concentrations of ammonia and oxygen, on the NO reduction efficiency and N2 selectivity were discussed to determine the feasible operating condition for photocatalytic reduction of NO. Experimental results showed that selective catalytic reduction of NO with ammonia over TiO2 in the presence of oxygen was a spontaneous reaction in dark. The photoirradiation on the TiO2 surface caused remarkable photocatalytic reduction of NO to form N2, NO2, and N20 under 254 nm UV illuminations, while almost 90% of N2 selectivity was achieved in this study. The ammonia and oxygen molecules played the roles of reductant and oxidant for NO reduction and active sites regeneration, respectively. The reduction of NO was found to be increased with the increase of inlet ammonia and oxygen concentrations until specific concentrations because of the limited active sites on the surface of TiO2. The kinetic model proposed in this study can be used to reasonably describe the reaction mechanism of photo-SCR.展开更多
The hydration of halogens has been widely researched because of its close relation with the water desalination and biochemical reactions.In this work,by a combination of scanning tunneling microscopy and X-ray photoel...The hydration of halogens has been widely researched because of its close relation with the water desalination and biochemical reactions.In this work,by a combination of scanning tunneling microscopy and X-ray photoelectron spectroscopy,we have explored the hydration process of iodine via the Eley-Rideal process on the Au(111)surface.Moreover,the hydration process of iodine with the presence of the NiPc self-assembled network as a template has also been investigated,where the stepwise hydration of iodine at room temperature can be visualized on Au(111).展开更多
基金supported by the Bureau of Science and Technology,Fujian Province,China(2015H0043)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB05050500)the National Natural Science Foundation of China(21403210)~~
文摘A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3（NH3-SCR） was determined.The effects of SO2 and H2O,and their combined effect,on the activity were examined at 340 ℃ for 24 h.The catalysts were characterized using N2 adsorption-desorption,X-ray diffraction,X-ray photoelectron spectroscopy,temperature-programmed reduction of H2（H2-TPR）,temperature-programmed desorption of NH3（NH3-TPD）,and in situ diffuse-reflectance infrared Fourier-transform spectroscopy（DRIFTS）.The CuSO4/TiO2 catalysts had good activities,with low production of N2O above 340 ℃.SO2 or a combination of SO2 and H2O had little effect on the activity,and H2O caused only a slight decrease in activity during the experimental period.The NH3-TPD and H2-TPR results showed that CuSO4 increased the amounts of acid sites and adsorbed oxygen on the catalyst.In situ DRIFTS showed that the NH3-SCR reaction on the CuSO4/TiO2 catalysts followed an Eley-Rideal mechanism.The reaction of gaseous NO with NH3 adsorbed on Lewis acid sites to form N2 and H2O could be the main reaction pathway,and oxygen adsorption might favor this process.
文摘We study a model based on precursor mechanism for CO-NO catalytic reaction on square lattice with Monte Carlo simulation. The precursor mechanism clearly demonstrates its impact on the phase diagram. The steady reactive state （SRS） gets established. The width of reactive region increases by increasing the range of precursor mobility. When the precursor mobility is increased to third-nearest neighbourhood, the second-order transition disappears.
基金financially supported by the National Key R&D Program of China (No.2017YFC0210303)National Natural Science Foundation of China (Nos.21806009 and 21677010)+1 种基金China Postdoctoral Science Foundation (Nos.2019T120049 and 2018M631344)Fundamental Research Funds for the Central Universities (No.FRF-TP-18-019A1).
文摘Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NOx) by NH3 at low temperature.Mn((2))Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH(with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction(SCR) catalytic activity,with about 96% NOx conversion at 750 C and-99%in the temperature range from 100 to 250℃.X-ray diffraction(XRD) results showed that Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH catalysts crystallized in the form of Mn2NiO4 and MnO2-Mn2NiO4 spinel,respectively.The latter gave relatively good selectivity to N2,which might be due to the presence of the MnO2 phase and high metal-O binding energy,resulting in low dehydrogenation ability.According to the results of various characterization methods,it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn2NiO4 spinel played important roles in the high-efficiency SCR activity of these catalysts.Mn(2)Ni(1)Ox catalysts presented good resistance to H2O or/and SO2 with stable activity,which benefited from the Mn2NiO4 spinel structure and Eley-Rideal mechanism,with only slight effects from SO2.
文摘Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction （photo-SCR） with ammonia over TiO2 in this study. NO reduction efficiency and N2 selectivity were determined from gases composition at the outlet stream of photoreactor. Effect of operating conditions, e.g. light intensity and inlet concentrations of ammonia and oxygen, on the NO reduction efficiency and N2 selectivity were discussed to determine the feasible operating condition for photocatalytic reduction of NO. Experimental results showed that selective catalytic reduction of NO with ammonia over TiO2 in the presence of oxygen was a spontaneous reaction in dark. The photoirradiation on the TiO2 surface caused remarkable photocatalytic reduction of NO to form N2, NO2, and N20 under 254 nm UV illuminations, while almost 90% of N2 selectivity was achieved in this study. The ammonia and oxygen molecules played the roles of reductant and oxidant for NO reduction and active sites regeneration, respectively. The reduction of NO was found to be increased with the increase of inlet ammonia and oxygen concentrations until specific concentrations because of the limited active sites on the surface of TiO2. The kinetic model proposed in this study can be used to reasonably describe the reaction mechanism of photo-SCR.
基金support from the National Natural Science Foundation of China(Grants No.22125203,21790351,22102117,and 22002183)the Fundamental Research Funds for the Central Universities(Grant No.22120210365).
文摘The hydration of halogens has been widely researched because of its close relation with the water desalination and biochemical reactions.In this work,by a combination of scanning tunneling microscopy and X-ray photoelectron spectroscopy,we have explored the hydration process of iodine via the Eley-Rideal process on the Au(111)surface.Moreover,the hydration process of iodine with the presence of the NiPc self-assembled network as a template has also been investigated,where the stepwise hydration of iodine at room temperature can be visualized on Au(111).
