To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The ...To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.展开更多
Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a meth...Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a method to construct superior Fe-Beta catalysts based on Al-rich zeolites.This strategy successfully promotes the formation of NH3-SCR-active isolated Fe^(3+)species,thus effectively improving the low-temperature activity of the Fe-Beta catalysts.Thanks to the abundant Brønsted acid sites of the Al-rich zeolite,the Fe_(2)O_(3) particles are redispersed and anchored as isolated Fe^(3+)during hydrothermal aging.This dynamic evolution of Fe species makes up for the adverse effect of dealumination of the Al-rich zeolite framework and achieves high stability for the Al-rich Fe-Beta catalyst.This study may promote the understanding of highly efficient and stable catalyst design using Al-rich zeolites.展开更多
本研究基于自行搭建的5 k W旋流预混火焰实验台,开展了轴向空气分级方式下CH_(4)/NH_(3)旋流预混火焰的实验测试,重点考察了分级风比例、分级风高度及分级风喷口数目对CH_(4)/NH_(3)旋流预混火焰燃烧及排放特性的影响。结果表明:随着NH_...本研究基于自行搭建的5 k W旋流预混火焰实验台,开展了轴向空气分级方式下CH_(4)/NH_(3)旋流预混火焰的实验测试,重点考察了分级风比例、分级风高度及分级风喷口数目对CH_(4)/NH_(3)旋流预混火焰燃烧及排放特性的影响。结果表明:随着NH_(3)占比的增大,火焰高度变长,燃烧室出口的NO排放量呈先增大后减小的趋势且在NH_(3)占比为50%达到峰值;在50%掺氨工况下采用轴向空气分级使一级燃烧室处于富燃状态可以有效降低NO的排放,其中分级风的最佳比例范围是30%~50%(当量比1.21~1.70),且随着分级风高度的增大呈下降趋势;此外,在最佳分级风比例和高度条件下(分级风高度80 mm、占比30%),增加分级风的喷口数目可减轻分级风碰撞对上游主燃区富燃状态的影响,使NO排放进一步降低。展开更多
Understanding the influence of HCl on the NH_(3)-selective catalytic reduction reaction mechanism is crucial for designing highly efficient denitrification catalysts.The formation of chlorate species on the surface of...Understanding the influence of HCl on the NH_(3)-selective catalytic reduction reaction mechanism is crucial for designing highly efficient denitrification catalysts.The formation of chlorate species on the surface of the synthesized SbCeO_(x)catalyst,induced by HCl,significantly enhances low-temperature activity,as evidenced by a 30%increase in NO conversion at 155℃.Furthermore,it improves N_(2)selectivity at high temperatures,with a notable 17%increase observed at 405℃.Both experimental results and density functional theory calculations confirm that chlorate species form at Ce sites.This formation facilitates the creation of oxygen vacancies,boosting the oxygen exchange capacity.It also increases NH_(3)adsorption at the Ce sites,promotes the formation of Sb-OH,and reduces competitive OH adsorption on these sites.Notably,compared with the reaction mechanism without HCl,the presence of chlorate species enhances NH_(3)adsorption and activation,which is vital for subsequent catalytic reactions.展开更多
The influence of different NH 4 +/NO 3 - ratios on nitrogen metabolism of cotton was studied under controlled hydroponics.The results showed that compared with single nitrate nutrition,solutions with 25/75,50/50,75/25...The influence of different NH 4 +/NO 3 - ratios on nitrogen metabolism of cotton was studied under controlled hydroponics.The results showed that compared with single nitrate nutrition,solutions with 25/75,50/50,75/25 and 100/0 of NH 4 +/NO 3 - significantly increased the soluble protein accumulation in leaves and roots of cotton,and the maximum content of soluble protein in leaves and roots appeared respectively in the solution with 50/50 and 75/25 of NH 4 +/NO 3 -.The soluble protein content in roots was increased with the increase of NH + 4 percentage,but was slightly less in the solution of 100/0 than 75/25,which was probably related to the excess NH + 4 limiting boot metabolism.With the increase of NH + 4 percentage,the nitrate content in petiole and the nitrate reductase activity in functional blade declined,but ammoniac nitrogen content increased in every organ of cotton.These results showed that foreign nitrogen affected the nitrogen metabolism of cotton in a different way,and the nitrogen absorption by cotton was probably related to different forms of foreign nitrogen.展开更多
基金financially supported by National Natural Science Foundation of China(No.52264043).
文摘To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.
基金supported by the National Key R&D Program of China(No.2023YFC3707200)the National Natural Science Foundation of China(Nos.22306191 and 52270112).
文摘Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a method to construct superior Fe-Beta catalysts based on Al-rich zeolites.This strategy successfully promotes the formation of NH3-SCR-active isolated Fe^(3+)species,thus effectively improving the low-temperature activity of the Fe-Beta catalysts.Thanks to the abundant Brønsted acid sites of the Al-rich zeolite,the Fe_(2)O_(3) particles are redispersed and anchored as isolated Fe^(3+)during hydrothermal aging.This dynamic evolution of Fe species makes up for the adverse effect of dealumination of the Al-rich zeolite framework and achieves high stability for the Al-rich Fe-Beta catalyst.This study may promote the understanding of highly efficient and stable catalyst design using Al-rich zeolites.
文摘本研究基于自行搭建的5 k W旋流预混火焰实验台,开展了轴向空气分级方式下CH_(4)/NH_(3)旋流预混火焰的实验测试,重点考察了分级风比例、分级风高度及分级风喷口数目对CH_(4)/NH_(3)旋流预混火焰燃烧及排放特性的影响。结果表明:随着NH_(3)占比的增大,火焰高度变长,燃烧室出口的NO排放量呈先增大后减小的趋势且在NH_(3)占比为50%达到峰值;在50%掺氨工况下采用轴向空气分级使一级燃烧室处于富燃状态可以有效降低NO的排放,其中分级风的最佳比例范围是30%~50%(当量比1.21~1.70),且随着分级风高度的增大呈下降趋势;此外,在最佳分级风比例和高度条件下(分级风高度80 mm、占比30%),增加分级风的喷口数目可减轻分级风碰撞对上游主燃区富燃状态的影响,使NO排放进一步降低。
文摘Understanding the influence of HCl on the NH_(3)-selective catalytic reduction reaction mechanism is crucial for designing highly efficient denitrification catalysts.The formation of chlorate species on the surface of the synthesized SbCeO_(x)catalyst,induced by HCl,significantly enhances low-temperature activity,as evidenced by a 30%increase in NO conversion at 155℃.Furthermore,it improves N_(2)selectivity at high temperatures,with a notable 17%increase observed at 405℃.Both experimental results and density functional theory calculations confirm that chlorate species form at Ce sites.This formation facilitates the creation of oxygen vacancies,boosting the oxygen exchange capacity.It also increases NH_(3)adsorption at the Ce sites,promotes the formation of Sb-OH,and reduces competitive OH adsorption on these sites.Notably,compared with the reaction mechanism without HCl,the presence of chlorate species enhances NH_(3)adsorption and activation,which is vital for subsequent catalytic reactions.
文摘The influence of different NH 4 +/NO 3 - ratios on nitrogen metabolism of cotton was studied under controlled hydroponics.The results showed that compared with single nitrate nutrition,solutions with 25/75,50/50,75/25 and 100/0 of NH 4 +/NO 3 - significantly increased the soluble protein accumulation in leaves and roots of cotton,and the maximum content of soluble protein in leaves and roots appeared respectively in the solution with 50/50 and 75/25 of NH 4 +/NO 3 -.The soluble protein content in roots was increased with the increase of NH + 4 percentage,but was slightly less in the solution of 100/0 than 75/25,which was probably related to the excess NH + 4 limiting boot metabolism.With the increase of NH + 4 percentage,the nitrate content in petiole and the nitrate reductase activity in functional blade declined,but ammoniac nitrogen content increased in every organ of cotton.These results showed that foreign nitrogen affected the nitrogen metabolism of cotton in a different way,and the nitrogen absorption by cotton was probably related to different forms of foreign nitrogen.
