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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) 被引量:1
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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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Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products
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作者 Qi Zhao Kai Lei +2 位作者 Bao Yu Xia Rachel Crespo-Otero Devis Di Tommaso 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期166-173,I0005,共9页
Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding th... Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal centres.This investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular catalysts.The modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)products.Our findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R process.Fu rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular catalysts.Strategic placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) products.This research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products. 展开更多
关键词 Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations
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Cerium-tungsten oxides supported on activated red mud for the selective catalytic reduction of NO_(x) 被引量:2
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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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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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Utilization of nickel slag using selective reduction followed by magnetic separation 被引量:14
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作者 潘建 郑国林 +1 位作者 朱德庆 周仙霖 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2013年第11期3421-3427,共7页
In order to utilize slag discarded by nickel plants, the selective recovery of nickel and copper versus iron was investigated by selective reduction, which was achieved by controlling the reduction parameters and magn... In order to utilize slag discarded by nickel plants, the selective recovery of nickel and copper versus iron was investigated by selective reduction, which was achieved by controlling the reduction parameters and magnetic separation process on bench scale. The results show that increasing the basicity (mass ratio of CaO to SIO2) of nickel slag facilitates the enrichment of nickel and copper The process parameters for selective reduction were optimized as follows: basicity of 0.15, reducing at 1200 ~C for 20 min, 5% coal on a dried slag mass base. The grinding-magnetic separation results of reduced briquettes show that concentrate containing 3.25%Ni, 1.20%Cu and 75.26%Fe is obtained and selective enrichment is achieved with a recovery of 82.20%, 80.00% for nickel and copper respectively, while the recovery of iron is only 42.17%. The S and P contents are not reduced obviously and further research may be needed to examine the behaviors of S and P in the process. 展开更多
关键词 nickel slag selective reduction magnetic separation
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Promotional roles of ZrO_2 and WO_3 in V_2O_5-WO_3/TiO_2-ZrO_2 catalysts for NO_x reduction by NH_3:Catalytic performance,morphology,and reaction mechanism 被引量:8
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作者 张亚平 王龙飞 +4 位作者 李娟 张会岩 徐海涛 肖睿 杨林军 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第11期1918-1930,共13页
V2O5/TiO2-ZrO2 catalysts containing various amounts of WO3 were synthesized.The catalyst morphologies,catalytic performances,and reaction mechanisms in the selective catalytic reduction of NOx by NH3 were investigated... V2O5/TiO2-ZrO2 catalysts containing various amounts of WO3 were synthesized.The catalyst morphologies,catalytic performances,and reaction mechanisms in the selective catalytic reduction of NOx by NH3 were investigated using in situ diffuse-reflectance infrared Fourier-transform spectroscopy,temperature-programmed reduction(TPR),X-ray diffraction,and the Brunauer-Emmett-Teller(BET) method.The BET surface area of the triple oxides increased with increasing ZrO2 doping but gradually decreased with increasing WO3 loading.Addition of sufficient WO3 helped to stabilize the pore structure and the combination of WO3 and ZrO2 improved dispersion of all the metal oxides.The mechanisms of reactions using V2O5-9%WO3/TiO2-ZrO2 and V2O5-9%WO3/TiO2were compared by using either a single or mixed gas feed and various pretreatments.The results suggest that both reactions followed the Eley-Ridel mechanism;however,the dominant acid sites,which depended on the addition of WO3 or ZrO2,determined the pathways for NOx reduction,and involved[NH4^+-NO-Bronsted acid site]^* and[NH2-NO-Lewis acid site]^* intermediates,respectively.NH3-TPR and H2-TPR showed that the metal oxides in the catalysts were not reduced by NH3 and O2did not reoxidize the catalyst surfaces but participated in the formation of H2O and NO2. 展开更多
关键词 ZIRCONIA Tungsten oxide Selective catalytic reduction by ammonia In situ infrared diffuse-reflectance Fourier-transform spectroscopy Reaction mechanism
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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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In situ synthesized Cu-ZSM-5/cordierite for reduction of NO 被引量:5
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作者 王建成 田东 +2 位作者 韩丽娜 常丽萍 鲍卫仁 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2011年第2期353-358,共6页
ZSM-5 zeolites were directly synthesized on the surface of honeycomb cordierite substrates by hydrothermal method and certified by XRD and SEM techniques; the adhesion of ZSM-5 coatings was evaluated by ultrasonic vib... ZSM-5 zeolites were directly synthesized on the surface of honeycomb cordierite substrates by hydrothermal method and certified by XRD and SEM techniques; the adhesion of ZSM-5 coatings was evaluated by ultrasonic vibration. Cu-ZSM-5/cordierite monolithic catalyst was prepared by ion-exchange and impregnation method and applied for the selective catalytic reduction (SCR) of NO by NH3 using a simulated diesel exhaust. The results show that the cordierite surface is almost completely covered by ZSM-5 crystals and the crystallization time greatly impacts the loadings and adhesion of ZSM-5 coatings on substrate, the NOx removal rate over Cu-ZSM-5/cordierite is above 90% in a temperature range of 240-480℃. Moreover, Cu-ZSM-5/cordierite prepared by different methods shows a wide temperature window (240-540 ℃) with high NO removal activities. 展开更多
关键词 in situ synthesis Cu-ZSM-5/cordierite selective catalytic reduction NH3
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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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Fe-Mn/Al_2O_3 catalysts for low temperature selective catalytic reduction of NO with NH_3 被引量:7
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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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Highly dispersed V_2O_5/TiO_2 modified with transition metals(Cu,Fe,Mn,Co) as efficient catalysts for the selective reduction of NO with NH_3 被引量:31
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作者 赵欣 黄垒 +4 位作者 李红蕊 扈航 韩瑾 施利毅 张登松 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2015年第11期1886-1899,共14页
Different transition metals were used to modify V2O5-based catalysts (M-V, M = Cu, Fe, Mn, Co) on TiO2 via impregnation, for the selective reduction of NO with NH3. The introduced metals induced high dispersion in t... Different transition metals were used to modify V2O5-based catalysts (M-V, M = Cu, Fe, Mn, Co) on TiO2 via impregnation, for the selective reduction of NO with NH3. The introduced metals induced high dispersion in the vanadium species and the formation of vanadates on the TiO2 support, and increased the amount of surface acid sites and the strength of these acids. The strong acid sites might be responsible for the high N2 selectivity at higher temperatures. Among these catalysts, Cu-V/TiO2 showed the highest activity and N2 selectivity at 225-375 ~C. The results of X-ray photo- electron spectroscopy, NH3-temperature-programmed desorption, and in-situ diffuse reflectance infrared Fourier transform spectroscopy suggested that the improved performance was probably due to more active surface oxygen species and increased strong surface acid sites. The outstanding activity, stability, and SO2/H2O durability of Cu-V/TiO2 make it a candidate to be a NOx removal catalyst for stationary flue gas. 展开更多
关键词 deNOx Selective catalytic reduction Vanadate Transition metal
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Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust
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作者 Runnong Yang Wuyuan Liu +6 位作者 Zhaoying Wang Ming Sun Guangying Fu Zihan Gao Wenjian Jiao Rui Li Lin Yu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第7期172-182,共11页
The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH_(3)(NH_(3)-SCR).In order to further improve the catalytic pr... The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH_(3)(NH_(3)-SCR).In order to further improve the catalytic property,a series of Mn ion-assisted Cu/SSZ-13 powder catalysts were prepared by co-exchange method and stepwise exchange method.It is found that the NH_(3)-SCR activity,N_(2) selectivity,hydrothermal stability and sulfur resistance of Cu/SSZ-13 are promoted by introducing a minority of Mn(0.15%to 0.23%(mass))through co-exchange method.Characterization results reveal that the Cu,Mn co-exchange enables the higher amounts of Cu^(2+)active sites,the abundant medium strong and strong acid,the optimized ratio of Lewis acid to Brønsted acid etc.,which are required for a good NH_(3)-SCR catalytic property over broad temperature range and under harsh working environment.Moreover,a monolithic catalyst was prepared by impregnating a cordierite ceramic support into the coating slurry containing the optimized CuMn/SSZ-13 powder.The diesel engine bench tests show that Cu,Mn co-exchange gives the monolith catalyst a better catalytic property than commercial catalysts.This work provides an important guidance for the rational design of secondary-ion-assisted zeolites applied in NH_(3)-SCR. 展开更多
关键词 MnCu/SSZ-13 Co-exchange ZEOLITE CATALYSIS Selective catalytic reduction
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Hydrothermally stable metal oxide-zeolite composite catalysts for low-temperature NO_(x) reduction with improved N_(2) selectivity
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作者 Lijun Yan Shiqi Chen +5 位作者 Penglu Wang Xiangyu Liu Lupeng Han Tingting Yan Yuejin Li Dengsong Zhang 《Chinese Chemical Letters》 SCIE CAS CSCD 2024年第6期515-523,共9页
Development of hydrothermally stable,low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge.We have prepared a metal oxide-zeolite composite catalyst by dep... Development of hydrothermally stable,low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge.We have prepared a metal oxide-zeolite composite catalyst by depositing Mn active species on a mixture support of CeO_(2)/Al_(2)O_(3) and ZSM-5.This composite catalyst is hydrothermally stable and shows improved low-temperature SCR activity and significantly reduced N_(2)O formation than the corresponding metal oxide catalyst.Comparing with a Cu-CHA catalyst,the composite catalyst has a faster response to NH_(3) injection and less NH_(3) slip.Our characterization results reveal that such an oxide-zeolite composite catalyst contains more acidic sites and Mn^(3+)species as a result of oxide-zeolite interaction,and this interaction leads to the generation of more NH_(4)^(+)species bound to the Br?nsted acid sites and more reactive NOxspecies absorbed on the Mn sites.Herein,we report our mechanistic understanding of the oxide-zeolite composite catalyst and its molecular pathway for improving the low-temperature activity and N_(2) selectivity for NH_(3)-SCR reaction.Practically,this work may provide an alternative methodology for low-temperature NO_(x) control from diesel vehicles. 展开更多
关键词 Selective catalytic reduction Mn-based catalysts Hydrothermal stability N_(2) selectivity
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Understanding the roles of Brønsted/Lewis acid sites on manganese oxide-zeolite hybrid catalysts for low-temperature NH_(3)-SCR
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作者 Hyun Sub Kim Hwangho Lee +2 位作者 Hongbeom Park Inhak Song Do Heui Kim 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期79-88,共10页
Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s... Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents. 展开更多
关键词 Hybrid metal oxide-zeolite The role of acid sites Manganese oxides Physical mixing Selective catalytic reduction of NOx with NH3
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Improvement of High-efficiency Green Catalysts for Flue Gas Denitrification
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作者 Liyan JIN Qingyi YU +3 位作者 Naixin ZHANG Yu WEI Xinlu YANG Yu GAO 《Meteorological and Environmental Research》 2024年第4期49-51,共3页
Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechani... Based on the basic principle and mechanism of flue gas denitrification,the commonly used catalysts for flue gas denitrification were introduced firstly,and then the catalytic performance,stability and reaction mechanism of catalysts in the market were analyzed.Different types of catalysts were studied to look for green catalysts with high activity,sulfur resistance,water vapor resistance and other advantages.The mechanism of denitration reaction of green catalysts was discussed,and the laws of formation,propagation and consumption of active species in the reaction process were revealed to provide theoretical basis for optimizing catalyst design and improving reaction conditions.Then the research status and problems of new catalysts for flue gas denitrification were described.Finally,the future development direction of green catalysts for flue gas denitration was discussed to improve the performance and stability of catalysts and meet the performance requirements of denitration catalysts in different industries. 展开更多
关键词 Flue gas denitration Green catalyst Denitration catalyst ACTIVITY Selective catalytic reduction Catalyst activation
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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 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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Thermodynamic of selective reduction of laterite ore by reducing gases 被引量:1
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作者 陈松 郭曙强 +2 位作者 姜兰 徐玉棱 丁伟中 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2015年第9期3133-3138,共6页
As the sulfide ore deposits become less economical and environmental viable as a source of nickel,increasing attention is being paid to the laterite ores.But in the pyrometallurgical process of laterite,more efforts s... As the sulfide ore deposits become less economical and environmental viable as a source of nickel,increasing attention is being paid to the laterite ores.But in the pyrometallurgical process of laterite,more efforts should be paid to control the reduction of iron oxide in order to get high nickel-content nickeliferous product.For these reasons,equilibrium condition of iron oxide when laterite ore was selectively reduced by CO2/CO,H2O/H2 and CO2/H2 was studied from the perspective of iron activity with an assumption that the activities of Fe O and Fe3O4 equal 1 in this work,and it well accounts for the inescapability of Fe metallization.Activity coefficient of iron in Ni-Fe binary solid alloy was calculated by Miedema model based on the known thermodynamics datum filed.According to Raoult's law,the relationship among the Fe/Ni ratio,reduction temperature and reduction gas composition was calculated when laterite ore was selectively reduced by the three different reduction systems.The calculation result was discussed and also compared with the experimental result.The trend of metal iron content in the reduction product of laterite ore varying with temperature and gas composition was well predicted by the calculation result. 展开更多
关键词 selective reduction laterite ore activity coefficient Miedema model
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Kinetic Model and Simulation of Promoted Selective Non-catalytic Reduction by Sodium Carbonate 被引量:32
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作者 韩奎华 路春美 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2007年第4期512-519,共8页
Abstract The detailed kinetic model of selective non-catalytic reduction (SNCR) of nitric oxide, including so-dium species reactions, was deyeloped on the basis of recent studies on thermal DeNOx mechanism, NOxOUTme... Abstract The detailed kinetic model of selective non-catalytic reduction (SNCR) of nitric oxide, including so-dium species reactions, was deyeloped on the basis of recent studies on thermal DeNOx mechanism, NOxOUTmechanism and promotion mechanism of Na2CO3. The model was validated by comparison with several experi-mental findings, thus providing an effective tool for the primary and promoted SNCR process simulation. Experimental and simulated results show part-per-million level of sodium carbonate enhances NO removal efficiency andextend the effective SNCR temperature range in comparison with use of a nitrogen agent alone. The kinetic modeling, sensitivity and rate-of-production analysis suggest that the performance improvement can be explained as ho-mogeneous sodium species reactions producing more reactive OH radicals. The net result of sodium species reac-tions is conversion of H2O and inactive HO2 radicals into reactive OH radicals, i.e. H2O+HO2=3OH, which enhances the SNCR performance of nitrogen agents by mainly increasing the production rate of NH2 radicals. More-over, N2O and CO are eliminated diversely via the reactions Na+N20=NaO+N2, NaO+CO=Na+CO2 andNaO2+CO =NaO+CO2, in.the pro.moted SNCR process, especially in the NOxOUT process. 展开更多
关键词 kinetic naodel SIMULATION selective non-catalytic reduction nitfic oxide sodium carbonate MECHANISM
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