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One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH_(3) at low temperature 被引量:1
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作者 Shuang Qiu Yonghou Xiao +3 位作者 Haoran Wu Shengnan Lu Qidong Zhao Gaohong He 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第4期193-202,共10页
NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperat... NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The Ce Cu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02%(mass) Ce constituent exhibited the best catalytic activity below 300℃ and a maximum NO_(x) conversion of 99% was attained;the NO_(x) removal rates of more than 68% and 94% were achieved at 150℃ and 200℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH_(3)-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Br?nsted acid centers and promote the synergistic effect between CuO grains and isolated Cu^(2+) to enhance the redox cycle, which benefit the NH_(3)-SCR reaction.This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature. 展开更多
关键词 CeCu-SAPO-34 selective catalytic reduction(scr) Low temperature DeNO_(x) One-pot synthesis
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Cerium-tungsten oxides supported on activated red mud for the selective catalytic reduction of NO_(x) 被引量:1
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作者 Qiuzhun Chen Dong Wang +7 位作者 Chuan Gao Bin Wang Shengli Niu Gaiju Zhao Yue Peng Junhua Li Chunmei Lu John Crittenden 《Green Energy & Environment》 SCIE EI CSCD 2023年第1期173-182,共10页
Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybde... Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species. 展开更多
关键词 Air pollution control NOx selective catalytic reduction CERIUM TUNGSTEN
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Effect of samarium on the N_(2) selectivity of Sm_(x)Mn_(0.3-x)Ti catalysts during selective catalytic reduction of NO_(x) with NH_(3)
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作者 Shengyang Zhang Bolin Zhang +2 位作者 Boyu Wu Bo Liu Shengen Zhang 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2023年第4期642-652,共11页
This work aims to study the improvement effect of Sm on Mn-based catalysts for selective catalytic reduction (SCR) of NO with NH3.A series of Sm_(x)Mn_(0.3-x)-xTi catalysts (x=0,0.1,0.15,0.2,and 0.3) were prepared by ... This work aims to study the improvement effect of Sm on Mn-based catalysts for selective catalytic reduction (SCR) of NO with NH3.A series of Sm_(x)Mn_(0.3-x)-xTi catalysts (x=0,0.1,0.15,0.2,and 0.3) were prepared by co-precipitation.Activity tests indicated that the Sm_(0.15)Mn_(0.15)Ti catalyst showed superior performances,with a NO conversion of 100%and N_(2)selectivity above 87%at 180–300℃.The characterizations showed that Sm doping suppressed the crystallization of TiO_(2)and Mn2O3phases and increased the specific surface area and acidity.In particular,the surface area increased from 152.2 m^(2)·g^(-1)for Mn0.3Ti to 241.7 m^(2)·g^(-1)for Sm_(0.15)Mn_(0.15)Ti.These effects contributed to the high catalytic activity.The X-ray photoelectron spectroscopy (XPS) results indicated that the relative atomic ratios of Sm^(3+)/Sm and Oβ/O of Sm_(0.15)Mn_(0.15)Ti were 76.77at%and 44.11at%,respectively.The presence of Sm contributed to an increase in surface-absorbed oxygen (Oβ) and a decrease in Mn^(4+)surface concentration,which improved the catalytic activity.In the results of hydrogen temperature-programmed reduction(H_(2)-TPR),the presence of Sm induced a higher reduction temperature and lower H_(2)consumption (0.3 mmol·g^(-1)) for the Sm_(0.15)Mn_(0.15)Ti catalyst compared to the Mn0.3Ti catalyst.The decrease in Mn^(4+)weakened the redox property of the catalysts and increased the N_(2)selectivity by suppressing N_(2)O formation from NH3oxidation and the nonselective catalytic reduction reaction.The in situ diffuse reflectance infrared Fourier transform spectra (DRIFTs) revealed that NH3-SCR of NO over the Sm_(0.15)Mn_(0.15)Ti catalyst mainly followed the Eley–Rideal mechanism.Sm doping increased surface-absorbed oxygen and weakened the redox property to improve the NO conversion and N_(2)selectivity of the Sm_(0.15)Mn_(0.15)Ti catalyst. 展开更多
关键词 manganese oxides nitric oxide nitrous oxide SAMARIUM selective catalytic reduction nitrogen selectivity
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Dynamic model for predicting nitrogen oxide concentration at outlet of selective catalytic reduction denitrification system based on kernel extreme learning machine 被引量:1
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作者 Ma Ning Liu Lei +2 位作者 Yang Zhenyong Yan Laiqing Dong Ze 《Journal of Southeast University(English Edition)》 EI CAS 2022年第4期383-391,共9页
To solve the increasing model complexity due to several input variables and large correlations under variable load conditions,a dynamic modeling method combining a kernel extreme learning machine(KELM)and principal co... To solve the increasing model complexity due to several input variables and large correlations under variable load conditions,a dynamic modeling method combining a kernel extreme learning machine(KELM)and principal component analysis(PCA)was proposed and applied to the prediction of nitrogen oxide(NO_(x))concentration at the outlet of a selective catalytic reduction(SCR)denitrification system.First,PCA is applied to the feature information extraction of input data,and the current and previous sequence values of the extracted information are used as the inputs of the KELM model to reflect the dynamic characteristics of the NO_(x)concentration at the SCR outlet.Then,the model takes the historical data of the NO_(x)concentration at the SCR outlet as the model input to improve its accuracy.Finally,an optimization algorithm is used to determine the optimal parameters of the model.Compared with the Gaussian process regression,long short-term memory,and convolutional neural network models,the prediction errors are reduced by approximately 78.4%,67.6%,and 59.3%,respectively.The results indicate that the proposed dynamic model structure is reliable and can accurately predict NO_(x)concentrations at the outlet of the SCR system. 展开更多
关键词 selective catalytic reduction nitrogen oxides principal component analysis kernel extreme learning machine dynamic model
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Influence of coke rate on thermal treatment of waste selective catalytic reduction(SCR)catalyst during iron ore sintering
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作者 Pengnan Ma Jiankang Wang +4 位作者 Hanxiao Meng Laiquan Lv Hao Fang Kefa Cen Hao Zhou 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第2期415-423,共9页
Waste selective catalytic reduction(SCR)catalyst as a hazardous waste has a significant impact on the environment and human health.In present study,a novel technology for thermal treatment of waste SCR catalyst was pr... Waste selective catalytic reduction(SCR)catalyst as a hazardous waste has a significant impact on the environment and human health.In present study,a novel technology for thermal treatment of waste SCR catalyst was proposed by adding it to sinter mix for iron ore sintering.The influences of coke rate on the flame front propagation,sinter microstructure,and sinter quality during sintering co-processing the waste SCR catalyst process were studied.In situ tests results indicated the maximum sintering bed temperature increased at higher coke rate,indicating more liquid phase generated and higher airflow resistance.The sintering time was longer and the calculated flame front speed dropped at higher coke rate.Sinter microstructure results found the coalescence and reshaping of bubbles were more fully with increasing coke rate.The porosity dropped from 35.28%to 25.66%,the pore average diameter of large pores decreased from 383.76μm to 311.43μm.With increasing coke rate,the sinter indexes of tumbler index,productivity,and yield,increased from 33.2%,9.2 t·m^(-2)·d^(-1),28.9%to 58.0%,36.0 t·m^(-2)·d^(-1),68.9%,respectively.Finally,a comprehensive index was introduced to systematically assess the influence of coke rate on sinter quality,which rose from 100 to 200 when coke rate was increased from 3.5%(mass)to 5.5%(mass). 展开更多
关键词 Flame front Waste selective catalytic reduction(scr) CATALYST Thermal treatment Iron ore sintering
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Performances of CuSO_4/TiO_2 catalysts in selective catalytic reduction of NO_x by NH_3 被引量:6
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作者 于艳科 陈进生 +1 位作者 王金秀 陈衍婷 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第2期281-287,共7页
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
关键词 selective catalytic reduction Copper sulfate ACTIVITY Eley-Rideal mechanism Lewis acid sites
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Fe-Mn/Al_2O_3 catalysts for low temperature selective catalytic reduction of NO with NH_3 被引量:6
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作者 王晓波 伍士国 +3 位作者 邹伟欣 虞硕涵 归柯庭 董林 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第8期1314-1323,共10页
A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactiva... A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature‐programmed reduction, NH3 temperature‐programmed desorption, X‐ray photoelectron spectroscopy (XPS), thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to character‐ize the catalysts. The 8Fe‐8Mn/Al2O3 catalyst gave 99%of NO conversion at 150?? and more than 92.6%NO conversion was obtained in a wide low temperature range of 90–210??. XPS analysis demonstrated that the Fe3+was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4+/Mn3+ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe‐8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe‐8Mn/Al2O3 cata‐lyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst. 展开更多
关键词 Nitrogen monoxide Low-temperature selective catalytic reduction Fe-Mn catalyst X-ray photoelectron spectroscopy Sulfur dioxide Fourier transform infrared spectroscopy
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Co(x)/ZRP催化剂的CH_(4)-SCR脱硝性能研究
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作者 林世静 王龙帅 +7 位作者 马宇彤 张丽芳 钟绍轩 汪澈 王轩 卢毅 卢学斌 王虹 《北京石油化工学院学报》 2024年第3期1-7,共7页
为消除氮氧化物对人类健康和生态环境的危害,以甲烷为还原剂进行选择性催化脱硝(CH_(4)-SCR)得到了普遍的关注。研发高活性的CH_(4)-SCR脱硝催化剂成为该技术的研究重点。采用浸渍法制备了Co(x)/ZRP催化剂,考察了钴负载量对Co(x)/ZRP催... 为消除氮氧化物对人类健康和生态环境的危害,以甲烷为还原剂进行选择性催化脱硝(CH_(4)-SCR)得到了普遍的关注。研发高活性的CH_(4)-SCR脱硝催化剂成为该技术的研究重点。采用浸渍法制备了Co(x)/ZRP催化剂,考察了钴负载量对Co(x)/ZRP催化剂CH_(4)-SCR脱硝性能的影响。利用X射线衍射仪(XRD)、H_(2)程序升温还原(H_(2)-TPR)、吡啶吸附红外光谱(Py-IR)、NH_(3)程序升温脱附(NH_(3)-TPD)和NO程序升温脱附(NO-TPD)等对Co(x)/ZRP催化剂的理化性质进行了表征,在常压固定床微型反应器上评价了Co(x)/ZRP催化剂的CH_(4)-SCR脱硝性能。结果表明:Co(x)/ZRP催化剂中钴物种为Co_(3)O_(4),钴负载量增加,Co_(3)O_(4)晶粒变大,催化剂的氧化还原能力和NO的吸脱附性能均得到改善。随着钴负载量的增加,Co(x)/ZRP催化剂的CH_(4)-SCR脱硝活性先增强后降低,与催化剂中的中强酸量在总酸中的变化规律基本一致。其中Co(20)/ZRP催化剂的中强酸量较多,CH_(4)-SCR脱硝性能较好,T_(m)为342℃,X_(No)^(max)为39.2%。催化剂表面的L酸位以及中强酸量对催化剂的CH_(4)-SCR催化脱硝活性具有重要作用。 展开更多
关键词 Co_(3)O_(4) NO ZRP分子筛 甲烷 选择性催化还原
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Synthesis of a chabazite-supported copper catalyst with full mesopores for selective catalytic reduction of nitrogen oxides at low temperature 被引量:9
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作者 刘计省 刘坚 +4 位作者 赵震 宋卫余 韦岳长 段爱军 姜桂元 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第5期750-759,共10页
A series of meso‐microporous copper‐supporting chabazite molecular sieve(CuSAPO‐34) catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction(NH3‐SCR)have been synthesized ... A series of meso‐microporous copper‐supporting chabazite molecular sieve(CuSAPO‐34) catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction(NH3‐SCR)have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2+ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts. 展开更多
关键词 One-pot synthesis Meso-microporous Cu-SAPO-34 Low temperature selective catalytic reduction Nitrogen oxides
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Promotional effects of Zr on K^+-poisoning resistance of CeTiO_x catalyst for selective catalytic reductionof NO_x with NH_3 被引量:5
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作者 徐宝强 徐海迪 +6 位作者 林涛 曹毅 兰丽 李元山 冯锡 龚茂初 陈耀强 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第8期1354-1361,共8页
CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 (NH3‐SCR). Various amounts of KNO3 were impregnated on the catalyst surface to invest... CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 (NH3‐SCR). Various amounts of KNO3 were impregnated on the catalyst surface to investigate the effects of Zr addition on the K+‐poisoning resistance of the CeTiOx catalyst. The NH3‐SCR performance of the catalysts showed that the NOx removal activity of the Zr‐modified catalyst after poisoning was better than that of the CeTiOx catalyst. Brunau‐er‐Emmett‐Teller data indicated that the Zr‐containing catalyst had a larger specific surface area and pore volume both before and after K+poisoning. X‐ray diffraction, Raman spectroscopy, and transmission electron microscopy showed that Zr doping inhibited anatase TiO2 crystal grain growth, i.e., the molten salt flux effect caused by the loaded KNO3 was inhibited. The Ce 3d X‐ray photoelectron spectra showed that the Ce3+/Ce4+ratio of CeZrTiOx decreased more slowly than that of CeTiOx with increasing K+loading, indicating that Zr addition preserved more crystal defects and oxygen vacancies; this improved the catalytic performance. The acidity was a key factor in the NH3‐SCR performance; the temperature‐programmed desorption of NH3 results showed that Zr doping inhibited the decrease in the surface acidity. The results suggest that Zr improved the K+‐poisoning resistance of the CeTiOx catalyst. 展开更多
关键词 Cerium-titanium mixed oxide ZIRCONIUM Potassium-poisoning resistance selective catalytic reduction Nitrogen oxides
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Promotional effect of H_3PO_4 on ceria catalyst for selective catalytic reduction of NO by NH_3 被引量:5
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作者 易婷 张一波 +1 位作者 李经纬 杨向光 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第2期300-307,共8页
A series of H3PO4-modified CeO2 samples were prepared by impregnation of CeO2 with H3PO4solution,and evaluated for the selective catalytic reduction of NOx by NH3.The samples were characterized by X-ray diffraction,N2... A series of H3PO4-modified CeO2 samples were prepared by impregnation of CeO2 with H3PO4solution,and evaluated for the selective catalytic reduction of NOx by NH3.The samples were characterized by X-ray diffraction,N2 adsorption-desorption,infrared spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy,temperature-programmed desorption of NH3,and temperature-programmed reduction of H2.The results showed that more than 80%NO conversion was achieved in the temperature range 250-550℃ over the H3PO4-CeO2 catalyst.The enhanced catalytic performance could be ascribed to the increase in acidic strength,especially Bronsted acidity,and reduction in redox properties of the CeO2 after H3PO4 modification. 展开更多
关键词 AMMONIA selective catalytic reduction CERIA Phosphoric acid Redox ACIDITY
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Resistance to SO_2 poisoning of V_2O_5/TiO_2-PILC catalyst for the selective catalytic reduction of NO by NH_3 被引量:4
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作者 臧思淼 张桂臻 +3 位作者 邱文革 宋丽云 张然 何洪 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第6期888-897,共10页
A titania pillared interlayered clay(Ti-PILC) supported vanadia catalyst(V2O5/TiO2-PILC) was prepared by wet impregnation for the selective catalytic reduction(SCR) of NO with ammonia. Compared to the traditiona... A titania pillared interlayered clay(Ti-PILC) supported vanadia catalyst(V2O5/TiO2-PILC) was prepared by wet impregnation for the selective catalytic reduction(SCR) of NO with ammonia. Compared to the traditional V2O5/TiO2 and V2O5-MoO3/TiO2 catalysts, the V2O5/TiO2-PILC catalyst exhibited a higher activity and better SO2 and H2O resistance in the NH3-SCR reaction. Characterization using TPD, in situ DRIFT and XPS showed that surface sulfate and/or sulfite species and ionic SO4^(2-)species were formed on the catalyst in the presence of SO2. The ionic SO4^(2-) species on the catalyst surface was one reason for deactivation of the catalyst in SCR. The formation of the ionic SO4^(2-) species was correlated with the amount of surface adsorbed oxygen species. Less adsorbed oxygen species gave less ionic SO4^(2-) species on the catalyst. 展开更多
关键词 selective catalytic reduction TiO2-pillared clay Nitrogen oxide Vanadia catalyst In situ diffuse reflectance infrared Fourier transform spectroscopy
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应用集成极限学习机的电站SCR脱硝系统建模与分析 被引量:1
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作者 马宁 尚勇 +4 位作者 尤默 杨振勇 李展 刘磊 康静秋 《中国测试》 CAS 北大核心 2024年第1期185-192,共8页
针对火电机组普遍采用的选择性催化还原(selective catalytic reduction,SCR)脱硝反应容易受到环境因素影响,且具有非线性、大迟延、强扰动特点,难以建立准确反应模型的问题,提出一种基于集成极限学习机的SCR脱硝系统建模方法。首先,选... 针对火电机组普遍采用的选择性催化还原(selective catalytic reduction,SCR)脱硝反应容易受到环境因素影响,且具有非线性、大迟延、强扰动特点,难以建立准确反应模型的问题,提出一种基于集成极限学习机的SCR脱硝系统建模方法。首先,选择4种具有不同激活函数的极限学习机和核极限学习机作为基学习器,分别建立SCR脱硝系统模型;然后,利用偏最小二乘算法将各基学习器的结果进行集成;最后,采用某1000 MW超超临界机组实际运行数据与所提建模方法相结合建立SCR脱硝系统模型。实验结果验证模型的有效性;与其他方法所建模型对比,结果表明基于集成极限学习机的SCR脱硝系统模型具有更好的模型泛化能力。 展开更多
关键词 火电机组 选择性催化还原 极限学习机 集成
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Kinetics of selective catalytic reduction of NO by NH_3 on Fe-Mo/ZSM-5 catalyst 被引量:9
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作者 LI Zhe SHEN Lin-tao HUANG Wei XIE Ke-chang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2007年第12期1516-1519,共4页
The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH3. The kinetics of the SCR reaction in the pre... The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH3. The kinetics of the SCR reaction in the presence of O2 was studied in this work. The results showed that the observed reaction orders were 0.74-0.99, 0.01-0.13, and 0 for NO, O2 and NH3 at 350-450℃, respectively. And the apparent activation energy of the SCR was 65 kJ/mol on the Fe-Mo/ZSM-5 catalyst. The SCR mechanism was also deduced. Adsorbed NO species can react directly with adsorbed ammonia species on the active sites to form N2 and H2O. Gaseous O2 might serve as a reoxidizing agent for the active sites that have undergone reduction in the SCR process. It is also important to note that a certain amount of NO was decomposed directly over the Fe-Mo/ZSM-5 catalyst in the absence of NH3. 展开更多
关键词 selective catalytic reduction scr nitric oxide (NO) Fe-Mo/ZSM-5 KINETICS activation energy
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Influence of chromium modification on the properties of MnO_x-FeO_x catalysts for the low-temperature selective catalytic reduction of NO by NH_3 被引量:7
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作者 Kai Shen Yaping Zhang +3 位作者 Xiaolei Wang Haitao Xu Keqin Sun Changcheng Zhou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第4期617-623,共7页
Catalytic properties of MnOx-FeOx complex oxide (hereafter denoted as Mn-Fe) catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-cbemical techniques, su... Catalytic properties of MnOx-FeOx complex oxide (hereafter denoted as Mn-Fe) catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-cbemical techniques, such as N2 physisorption, X-ray diffraction (XRD), high-resolution transmission electron microscope (HRTEM), in situ Fourier transform infrared spectroscopy (in situ FT-IR) and temperature-programmed reduction (TPR) and their catalytic activities were evaluated with the selective catalytic reduction (SCR) of NOx by NH3. It was found that with the addition of Cr, more NO could be removed in the low-temperature window (below 120 ℃). Among the tested catalysts, Mn-Fe- Cr (2 : 2 : 1) catalyst exhibited the best catalytic performance at 80 ℃ with the NO conversion higher than 90%. The combination of the reaction and characterization results indicated that (1) the strong interaction among tertiary metal oxides existed in the catalysts when Cr was appropriately added, which made the active components better dispersed with less agglomeration and sintering and the largest BET specific surface area could be obtained; (2) Cr improved the low-temperature reducibility of the catalyst and promoted the formation of the active intermediate (-NH3+), which favored the low-temperature SCR reaction. 展开更多
关键词 MnOx-FeOx Cr MODIFICATION low-temperature selective catalytic reduction CATALYSTS
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Study on methane selective catalytic reduction of NO on Pt/Ce_(0.67)Zr_(0.33)O_2 and its application 被引量:9
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作者 Zhimin Liu Kangcai Wang Xiaoyu Zhang Jianli Wang Hongyan Cao Maochu Gong Yaoqiang Chen 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2009年第1期66-70,共5页
Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction (SCR) of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO a... Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction (SCR) of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO and CH4 can be converted completely at 450℃. Meanwhile, NO and CH4 can be converted completely when there exists excess oxygen. The Pt/Ce0.67Zr0.33O2 catalyst were further investigated by using methane as reducing agent to SCR NO in a novel equipment which combined the CH4 selective catalytic reduction of NO with methane combustion. The result shows that the catalyst is high active and the novel equipment is very effective. The conversion of NO is above 92% under the conditions used in this work. The prepared burner and catalysts have great potential for application. 展开更多
关键词 Pt/Ce0.67Zr0.33O2 selective catalytic reduction NO catalytic burner APPLICATION
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Plasma-catalytic Selective Reduction of NO with C_(2)H_(4)in the Presence of Excess Oxygen 被引量:7
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作者 QiSUN AiMinZHU +4 位作者 XueFengYANG JinHaiNIU YongXU ZhiMinSONG JingLIU 《Chinese Chemical Letters》 SCIE CAS CSCD 2005年第6期839-842,共4页
This paper reports observations of significant synergistic effects between dielectric barrier discharge (DBD) plasmas and Cu-ZSM-5 catalysts for C2H4 selective reduction of NOx at 250 °C in the presence of excess... This paper reports observations of significant synergistic effects between dielectric barrier discharge (DBD) plasmas and Cu-ZSM-5 catalysts for C2H4 selective reduction of NOx at 250 °C in the presence of excess oxygen by using a one-stage plasma-over-catalyst (POC) reactor. With the reactant gas mixture of 530 ppm NO, 650 ppm C2H4, 5.8% O2 in N2 and GHSV = 12000 h-1, the pure catalytic, pure plasma-induced (discharges over fused silica pellets) and plasma- catalytic (in the POC reactor) NOx conversion are 39%, 1.5% and 79%, respectively. The in-situ optical emission spectra of the reactive systems imply some short-lived active species formed from plasma-induced and plasma-catalytic processes may be responsible to the observed synergistic effects in this one-stage POC system. 展开更多
关键词 NOx removal selective catalytic reduction non-thermal plasma CuZSM-5 ETHENE optical emission spectroscopy.
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Cu改性MIL-100(Fe)催化剂的SCR-C_(3)H_(6)脱硝特性
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作者 付维 宁淑英 +3 位作者 蔡晨 陈佳音 周皞 苏亚欣 《化工进展》 EI CAS CSCD 北大核心 2024年第9期4951-4960,共10页
烃类化合物选择性催化还原氮氧化物(SCR-HC)是一种很有发展前景的脱硝技术。催化剂有效的氧化-还原能力是影响其活性的关键因素。利用水热法制备了新型有机金属骨架MIL-100(Fe),通过超声浸渍法合成不同Cu含量的m Cu-MIL-100(Fe)催化剂,... 烃类化合物选择性催化还原氮氧化物(SCR-HC)是一种很有发展前景的脱硝技术。催化剂有效的氧化-还原能力是影响其活性的关键因素。利用水热法制备了新型有机金属骨架MIL-100(Fe),通过超声浸渍法合成不同Cu含量的m Cu-MIL-100(Fe)催化剂,在固定床微反应器中对其催化C_(3)H_(6)选择性还原NO的特性进行了实验研究。结果表明Cu的引入使MIL-100(Fe)催化活性得到改善。2.3Cu-MIL-100(Fe)的NO转化率在275℃下可达到100%,275~400℃范围内可维持85%以上NO转化率及90%以上N_(2)选择性,且具有较好抗SO_(2)的能力。通过各种技术手段对催化剂的微观结构及物化性质进行了表征,并对反应机理作了进一步讨论。N_(2)吸附-脱附结果表明,加入适量Cu可以增大催化剂的比表面积,并增强催化剂表面对反应气体的吸附能力;XPS研究结果表明,Cu可以提高催化剂表面的氧空位数目。Cu与Fe之间具有协同作用,二者之间存在电子转移现象。H_(2)-TPR曲线表明Cu使催化剂的还原特征峰向低温方向移动,增强了其还原性能。 展开更多
关键词 氮氧化物 选择催化还原 碳氢化合物 催化剂 Cu改性 抗SO_(2)性能
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TiO_2-Supported Binary Metal Oxide Catalysts for Low-temperature Selective Catalytic Reduction of NO_x with NH_3 被引量:5
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作者 WU Bi-jun LIU Xiao-qin +1 位作者 XIAO Ping WANG Shu-gang 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 2008年第5期615-619,共5页
Binary metal oxide(MnOx-A/TiO2)catalysts were prepared by adding the second metal to manganese oxides supported on titanium dioxide(TiO2),where,A indicates Fe2O3,WO3,MoO3,and Cr2O3.Their catalytic activity,N2 sele... Binary metal oxide(MnOx-A/TiO2)catalysts were prepared by adding the second metal to manganese oxides supported on titanium dioxide(TiO2),where,A indicates Fe2O3,WO3,MoO3,and Cr2O3.Their catalytic activity,N2 selectivity,and SO2 poisonous tolerance were investigated.The catalytic performance at low temperatures decreased in the following order:Mn-W/TiO2〉Mn-Fe/TiO2〉Mn-Cr/TiO2〉Mn-Mo/TiO2,whereas the N2 selectivity decreased in the order:Mn-Fe/TiO2〉Mn-W/TiO2〉Mn-Mo/TiO2〉Mn-Cr/TiO2.In the presence of 0.01%SO2 and 6%H2O,the NOx conversions in the presence of Mn-W/TiO2,Mn-Fe/TiO2,or Mn-Mo/TiO2 maintain 98.5%,95.8%and 94.2%, respectively,after 8 h at 120°C at GHSV 12600 h? 1 .As effective promoters,WO3 and Fe2O3 can increase N2 selectivity and the resistance to SO2 of MnOx/TiO2 significantly.The Fourier transform infrared(FTIR)spectra of NH3 over WO3 show the presence of Lewis acid sites.The results suggest that WO3 is the best promoter of MnOx/TiO2,and Mn-W/TiO2 is one of the most active catalysts for the low temperature selective catalytic reduction of NO with NH3. 展开更多
关键词 selective catalytic reduction of NO with NH3 Low-temperature selective catalytic reduction Binary metal oxide catalyst FTIR NH3-TPD
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Mn/beta and Mn/ZSM-5 for the low-temperature selective catalytic reduction of NO with ammonia: Effect of manganese precursors 被引量:12
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作者 Wenjin Xu Guangxu Zhang +4 位作者 Hanwei Chen Guomeng Zhang Yang Han Yichuan Chang Peng Gong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第1期118-127,共10页
Two series of Mn/beta and Mn/ZSM‐5catalysts were prepared to study the influence of how different Mn precursors,introduced to the respective parent zeolites by wet impregnation,affected the selective catalytic reduct... Two series of Mn/beta and Mn/ZSM‐5catalysts were prepared to study the influence of how different Mn precursors,introduced to the respective parent zeolites by wet impregnation,affected the selective catalytic reduction(SCR)of NO by NH3across a low reaction temperature window of50–350°C.In this study,the catalysts were characterized using N2adsorption/desorption,X‐ray diffraction,X‐ray fluorescence,H2temperature‐programmed reduction,NH3temperature‐programmed desorption and X‐ray photoelectron spectroscopy.As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl2in addition to the presence of low levels of crystalline Mn3O4,which resulted in poor catalytic performance.However,the manganese nitrate precursor formed crystalline MnO2as the major phase in addition to a minor presence of unconverted Mn‐nitrate.Furthermore,manganese acetate resulted principally in a mixture of amorphous Mn2O3and MnO2,and crystalline Mn3O4.From all the catalysts screened,the test performance data showed Mn/beta‐Ac to exhibit the highest NO conversion(97.5%)at240°C,which remained>90%across a temperature window of220–350°C.The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnOx(Mn2O3and MnO2)species that act as the active phase in the NH3‐SCR process.Furthermore,together with a suitable amount of weakly acidic centers,higher concentration of surface manganese and a greater presence of surface labile oxygen groups,SCR performance was collectively enhanced at low temperature.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved. 展开更多
关键词 Mn/beta Mn/ZSM‐5 Low‐temperature catalytic performance selective catalytic reduction Manganese precursors
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