Materials
·
2021
·Vol. 14
·期 20
·5958
·
IF 3.623
Xusheng Ren,Zhiliang Ou,Bang Wu
The activated coke is a promising support for catalysts, and it is important to study the performance of the activated coke catalyst on the removal of NOx. In the current research, a series of the activated coke-supported Mn–Cu catalysts are prepared by the incipient wetness impregnation method. The effects of the molar ration of Mn/Cu, the content of Mn–Cu, the calcination temperature, and reaction space velocity on NO conversion are investigated, and it was found that the 8 wt.% Mn0.7Cu0.3/AC had the best catalytic activity when the calcination temperature was 200 °C. The existence of SO2caused the catalyst to deactivate, but the activity of the poisoning catalyst could be recovered by different regeneration methods. To uncover the underlying mechanism, BET, XPS, XRD, SEM and FTIR characterizations were performed. These results suggested that the specific surface area and total pore volume of the poisoning catalyst are recovered and the sulfite and sulfate on the surface of the poisoning catalysts are removed after water washing regeneration. More importantly, the water washing regeneration returns the value of Mn3+/Mn4+, Cu2+/Cu+, and Oα/Oβ, related to the activity, basically back to the level of the fresh catalyst. Thus, the effect of water washing regeneration is better than thermal regeneration. These results could provide some helpful information for the design and development of the SCR catalysts.Keywords:activated coke;low-temperature NH3-SCR;sulfur poisoning;regeneration
研究领域:
催化化学
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2021
·
IF 6.064
Bichun Huang,Hansun Fang,Huajun Huang,Meijuan Lu,Chenglong Yu
A one-pot synthetic method was used to prepare copper (Cu)-modified manganese (Mn)-rich MnSAPO-34 catalysts, which were then used for NO x removal from stationary-source flue gas. The addition of Cu to these Mn-rich MnSAPO-34 catalysts significantly enhanced their low temperature (LT) selective catalytic reduction (SCR) activity and H 2 O resistance. The Mn 0.4 Cu 0.05 SAPO-34 catalysts demonstrated excellent LT NH 3 -SCR activity, with NO x removal being >90% from 160 to 300 °C. In addition, Mn 0.4 Cu 0.05 SAPO-34 catalysts exhibited high H 2 O resistance. This excellent performance was ascribed to strong synergistic effects between Mn 4+ and isolated Cu 2+ species in Mn 0.4 Cu 0.05 SAPO-34 catalysts, leading to suitable redox ability. The results of in situ FT-IR analysis indicated that LT-SCR reactions mainly proceeded by an Eley–Rideal reaction pathway at 200 °C in Cu-modified manganese-rich MnSAPO-34 catalysts. Thus, Mn 0.4 Cu 0.05 SAPO-34 was considered as a promising candidate for NO x removal from flue gas of stationary sources at low temperatures.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 7
·3007-3018
·
IF 3.134
Liu Fengyuan,Li Junqi,Chen Chaoyi,Ning Deyang,Yang Jian,Chu Zhiyao,Mao Xisong,Lan Yuanpei
A novel tactic was employed to evaluate the low-temperature NH 3 -SCR (selective catalytic reduction) NO x removal property of manganese oxides (MnO x ) in various valence states, avoiding the influences of size, morphology and synthetic method on catalytic activity. Firstly, similar sized hollow-spherical MnO 2 , Mn 2 O 3 , Mn 3 O 4 and MnO were obtained by decomposing MnCO 3 at 440 and 500 °C in Air, 430 °C in H 2 and Ar, respectively. The orders of MnO x catalytic activity varied at different reaction temperature range, while MnO 2 showed the best NO conversion. Surface acidity has significant influences on the SCR activity, Mn 3 O 4 exhibits a better catalytic property than Mn 2 O 3 below 300 °C, and conversely, Mn 2 O 3 has a better high-temperature NO conversation than Mn 3 O 4 due to a stronger NH 3 adsorption ability above 300 °C. MnO will be oxidized in the studied atmosphere with 5% O 2 to Mn 3 O 4 , Mn 5 O 8 and finally to Mn 2 O 3 successively, and the mixed phases of MnO/Mn 3 O 4 or Mn 3 O 4 /Mn 5 O 8 exhibit a better catalytic activity than Mn 2 O 3 at 200–300 °C.
研究领域:
环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·
IF 0
You Mengyun,Wu Shufeng,Feng Xiaotong,Zhao Yong,Wang Yubin,Zhang Zhang
The enhancement effect of Ce modification on V 2 O 5 -WO 3 /TiO 2 catalysts at low temperatures was investigated for the selective catalytic reduction (SCR) of NO x with NH 3 (NH 3 -SCR). By adding 9% CeO 2 to 0.5%V 2 O 5 -3%WO 3 /TiO 2 catalyst, the low-temperature denitrification performance of Ce 9 V 0.5 W 3 Ti catalyst after Ce modification was significantly improved, achieving a NO conversion above 90% within a broad temperature range of 200–350℃, with catalytic activity comparable to that of 3% V 2 O 5 -3% WO 3 /TiO 2 . The catalysts were characterized by XPS, H 2 -TPR, NH 3 , and NO-TPD. The results indicated that the Ce additive could enhance the adsorption of NO x on Ce 9 V 0.5 W 3 Ti catalyst due to the synergetic interaction among the Ce and V, W species. The interaction between V and Ce also promoted the formation of V 5+ and Ce 3+ on the surface of the catalyst, which was conducive to enhancing the adsorption and oxidation capacity of the catalyst for NO. Additionally, the introduction of Ce led to a substantial deposition of nitrate species on the surface of the catalyst, especially the increase of nitrite species, which was beneficial to the NH 3 -SCR reaction process, resulting in a significant enhancement of the catalyst’s low-temperature catalytic activity.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
Materials
·
2019
·Vol. 12
·期 22
·3654
·
IF 2.972
Mingxuan Ma,Xiaoyu Ma,Suping Cui,Tingting Liu,Yingliang Tian,Yali Wang
A series of MCM-41 molecular sieves with different molar ratio of template to silicon were synthesized through hydrothermal synthesis method by using cetyltrimethylammonium bromide (CTAB) as the template, diatomite as the silicon source. By using impregnation method, the Mn-Ce/MCM-41 SCR molecular sieve-based catalysts were prepared. The results observed that when the molar ratio of template to silicon was 0.2:1, the MCM-41 as catalyst carrier has the highest surface area and largest pore volume, it also presented typically ordered hexagonal arrays of uniform channels. The denitration catalytic material based on this carrier has a high number of Lewis acidic sites, and the denitration efficiency can reach more than 93%.
研究领域:
环境催化
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材料科学
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化学工程
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大气污染控制
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无机多孔材料
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 10
·3147-3157
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IF 5
Hange Wang,Wen Chen,Wei Jin,Yueli Liu
SCR technology is considered to be the most effective method for denitrification. However, the low NOx conversion rate of the current catalysts at low temperatures limits their further application. Herein, Sn-doped modified CoAl-LDH carriers are synthesized by a hydrothermal method, and the typical hexagonal sheet structure of the MnOx(0.25)/CoSn3Al-LDO catalyst achieves 100% NO conversion at a wide range of 120–330 °C with a GHSV of 30 000 h−1, and the 100% NO conversion may be maintained at 200 °C for 30 h. After the introduction of 150 ppm SO2 at 200 °C, the NO conversion of the MnOx(0.25)/CoSn3Al-LDO catalyst is maintained at 73.4%, which is greatly improved compared with those of CoAl-LDO and MnOx(0.25)/CoAL-LDO catalysts (64.8% and 38.6%, respectively). The active components such as MnOx and Co3O4 are highly dispersed in the MnOx(0.25)/CoSn3Al-LDO catalyst. Sn doping increases the ratios of Mn4+/Mn3+ and Co3+/Co2+ as well as the adsorbed oxygen amount on the catalyst surface, and improves the redox capacity of the catalyst and increases the number of acid sites, resulting in the excellent low-temperature NH3-SCR performance of MnOx(0.25)/CoSn3Al-LDO.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2025
·
IF 3.7
Dingding Liu,Yating Huang,Zhenguo Li,Guohua Jing,Yongdan Li,Huawang Zhao
The advancements in engine technology have led to a decrease in exhaust temperatures, hence enhancing the activity of Cu-SSZ-13 at low temperatures becomes crucial and challenging. This enhancement can be achieved using dual-phase metal oxide/Cu-SSZ-13 composite catalysts. In this work, we evaluated the comparative efficacy of Mn 3 O 4 and Mn 2 O 3 and discovered that Mn 3 O 4 exhibited a significantly superior enhancement in deNO x activity of Cu-SSZ-13 at low temperatures, achieving 95% NO x conversion at 200 °C. This is substantially higher than the conversions recorded by Mn 2 O 3 /Cu-SSZ-13 (78%) and Cu-SSZ-13 (40%). Kinetic and IR results demonstrate that Mn 3 O 4 /Cu-SSZ-13 and Mn 2 O 3 /Cu-SSZ-13 composite samples share a same low-temperature pathway, where bridged nitrates formed on the MnO x react with adsorbed on Brønsted acid sites in Cu-SSZ-13. In this reaction pathway, bridged nitrate formation is identified as the rate-determining step. The distinctive structure of Mn 3 O 4 triggers an increase in oxygen vacancies, creating a higher content of chemically adsorbed oxygen, compared to Mn 2 O 3 . Those adsorbed oxygen facilitates bridged nitrate formation. Consequently, due to the larger amount of bridged nitrate formed on Mn 3 O 4 compared to Mn 2 O 3 , the Mn 3 O 4 /Cu-SSZ-13 sample exhibits higher activity.
研究领域:
环境催化
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材料化学
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大气污染控制
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化学工程
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表面科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Zhicheng Xu,Jin Xiong,Yuran Li,Junxiang Guo,Bin Wang,Tingyu Zhu
For industrial flue gas purification at medium and low temperatures, it is highly necessary to promote the denitrification activity of V-based catalysts in a SO2 atmosphere. Transition metals (Ce, Co, Fe, and Mn) are used to modify V/Ti catalysts to improve SO2 resistance with ammonium bisulfate deposition on the catalysts. Sulfation on Ce with less ammonium bisulfate deposition considerably improves the SO2 resistance of V1Ce5/Ti, and stable sulfation on TiO2 promoted by Co provides additional Brønsted acid sites for V1Co5/Ti to reduce the deactivation. Serious sulfation on V1Mn5/Ti with large ammonium bisulfate deposition on V1Fe5/Ti causes deeper deactivation. The formation mechanism of ammonium bisulfate on active metal sites and TiO2 carriers has been clarified. SO2 is adsorbed on V sites and transition metal sites followed by oxidation and ammoniation or adsorbed on TiO2 carriers followed by ammoniation and oxidation. The first pathway is more dominant than the second pathway in the presence of O2 with the co-oxidation of SO2 by O2 and lattice oxygen. The initial formation temperature and stable temperature of dominant intermediates were determined by in situ DRIFTS. SO2 adsorbed on TiO2 carriers is oxidized by V sites above 170 °C to form a tridentate sulfate, while SO2 adsorbed on transition metal sites is initially oxidized by transition metal sites above 50 °C to form monodentate and bidentate sulfates, as well as competitively oxidized by V sites above 170 °C to form tridentate sulfates. The selective adsorption of SO2 on transition metal sites or TiO2 carriers and the competitive oxidation of SO2 by transition metal sites and V sites provide a synergistic effect between V sites and transition metal sites to reduce ammonium sulfate deposition and release more active sites. These findings provide theoretical guidance to design and prepare V-based catalysts with high denitrification activity in the presence of SO2.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qin Wu,Chi Fan,Ya Wang,Xiaoping Chen,Guimin Wang,Zhengxing Qin,Svetlana Mintova,Junhua Li,Jianjun Chen
The reduction of NO x emission during the cold start period of diesel vehicles requires special attention in accordance with the emission regulations. In this work, the direct incorporation of cerium and copper in SAPO-18 catalyst with AEI type framework structure (CuCe-SAPO-18) resulting in a substantial enhancement of the performance in the low-temperature NH 3 -SCR reaction (<200 ℃). A small amount of cerium (0.13–0.31 wt%) broadened the reaction temperature range of use and increased the hydrothermal stability of the catalyst considerably. The cerium species was introduced in the ion-exchange sites of Cu-SAPO-18 in the form of Ce 3+ ions even with high loading (3.15 wt%). The Ce 3+ ions were found to affect the distribution of silicon and aluminum atom coordination ( 29 Si NMR, 27 Al MAS NMR) in the AEI-type skeleton structure leading to an increase of both the amount of active Cu 2+ species and the acidity of the CuCe-SAPO-18 catalysts that are beneficial for the NH 3 -SCR reaction.
研究领域:
催化化学
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环境科学
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材料化学
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大气污染控制
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无机固体化学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Shuohan Yu,Yiyang Lu,Yuan Cao,Jiaming Wang,Bowen Sun,Fei Gao,Changjin Tang,Lin Dong
Mn-based catalysts were believed to be promoting low temperature NH 3 -SCR catalysts for their satisfactory catalytic activity, whereas their poor SO 2 and H 2 O tolerance inhibited their applications. In this work, utilizing poor SO 2 tolerance of Mn oxides, composite catalytic systems containing Mn oxides as deSO x catalyst was designed and synthesized, which exhibited excellent low temperature NH 3 -SCR performance in the presence of SO 2 and H 2 O. The deSO x mechanism of Mn oxides was systematically investigated. In results, SO 2 was catalytic oxidized on the surface of Mn oxides. Oxidized sulfur species could flow away from Mn oxides surface through feed gas flow or form MnSO 4 . When NH 3 and H 2 O were introduced into the feed gas, the oxidized sulfur species were completely deposited as NH 4 HSO 4 instead of forming MnSO 4 . Thus, SO 2 was removed from feed gas entirely resulting in the superb low temperature NH 3 -SCR performances. This work provided a general strategy to enhance SO 2 and H 2 O tolerance of NH 3 -SCR catalysts at low temperature by removing SO 2 using NH 3 and H 2 O who existed in the exhaust gas from stationary sources.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Jinfeng Chen,Qingze Zhang,Yuanhong Zhong,Zhaoying Wang,Yakun Guo,Ming Sun,Lin Yu
To address the limitations of molecular sieves and metal oxides in the NH3-SCR of NOx, we synthesized a novel hybrid catalyst by integrating FeNbCe metal oxides with Cu-SSZ-13. The FeNbCe comodification significantly enhanced the low-temperature performance and sulfur resistance of Cu-SSZ-13 while maintaining 100% N2 selectivity across a broad activity window. The incorporation of Fe, Nb, and Ce reduced weak-acid and Lewis-acid sites while increasing strong Brønsted-acid sites, crucial for catalytic activity. The FeNbCe/Cu-SSZ-13 catalyst exhibited an enhanced surface oxygen content and redox capacity, promoting the “fast SCR” pathway and improving N2 selectivity at low temperatures. The FeNbCe oxides synergistically reacted with SO2, protecting Cu2+ active sites from sulfur poisoning and maintaining 100% NOx conversion for 4 h after SO2 introduction, maintaining 85% within 24 h. In situ DRIFTS characterization confirmed the dominance of the Langmuir-Hinshelwood (L-H) mechanism. The FeNbCe modification represents a significant advancement in the field of NH3–SCR catalysis, offering a practical and effective solution to enhance the performance of Cu-SSZ-13 while addressing key challenges such as sulfur resistance and low-temperature activity.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2014
·
IF 5.9
Lei Chen,Zhichun Si,Xiaodong Wu,Duan Weng
A CuO–CeO2–TiO2 catalyst for selective catalytic reduction of NOx with NH3 (NH3-SCR) at low temperatures was prepared by a sol–gel method and characterized by X-ray diffraction, Brunner–Emmett–Teller surface area, ultraviolet–visible spectroscopy, H2 temperature-programmed reduction, scanning electron microscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). The CuO–CeO2–TiO2 ternary oxide catalyst shows excellent NH3-SCR activity in a low-temperature range of 150–250 °C. Lewis acid sites generated from Cu2+ are the main active sites for ammonia activation at low temperature, which is crucial for low temperature NH3-SCR activity. The introduction of ceria results in increased reducibility of CuO species and strong interactions between CuO particles with the matrix. The interactions between copper, cerium and titanium oxides lead to high dispersion of metal oxides with increased active oxygen and enhanced catalyst acidity. Homogeneously mixed metal oxides facilitate the “fast SCR” reaction among Cu2+–NO, nitrate (coordinated on cerium sites) and ammonia (on titanium sites) on the CuO–CeO2–TiO2 catalyst at low temperatures.
研究领域:
环境催化
·
材料化学
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表面科学
·
化学工程
·
大气污染控制
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）