Molecular Catalysis
·
2022
·
IF 5.089
Yaping Yang,Xuesong Liu,Zhiming Sui,Yanghui Wang,Ping Fang,Peng Jiang,Xiaodong Wu
The purpose of this study is to investigate the interaction of Ce and W species with TiO 2 , Al 2 O 3 and SiO 2 supports, so as to illustrate the influence of supports and distribution of Ce, W species on SCR reaction. It is found that low-temperature activity followed the order of CeW > CeWTi > CeWAl > CeWSi. The reasons for the various activity of the catalyst were investigated by a series of characterization. The low-temperature NH 3 -SCR activity is associated with the surface concentrations of Ce 3+ , oxygen vacancies and active oxygen species, which are dominated by the dispersion and interactions of Ce/W species with the supports. Arising from interactions of Ti 4+ with high-density electron cloud, finely dispersed Ce and W species facilitate the W-Ce synergism and produce more active oxygen. All these contribute toTiO 2 can make Ce and W species in an ideal distribution, so the corresponding catalyst shows excellent NO x conversion of CeWTi catalyst at 200–350 °C. The reaction process observed by in situ DRIFT indicated that the NH 3 -SCR reaction on CeO 2 -WO 3 containing catalysts mainly follow Langmuir-Hinshelwood (L-H) mechanism at low temperature. Based on the analysis of the characterization and reaction process, it is concluded that the control step of NH 3 -SCR reaction at low temperature over CeO 2 -WO 3 containing catalysts is the adsorption and activation of NO x .
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Jian Gao,Xinrui Dai,Zhenhua Gu,Guixian Deng,Jiangyong Yuan,Kongzhai Li
Catalysts loaded with metal oxides of M (M = Mn, Co, Ce) were synthesized by deposition precipitation method using cold rolled sludge (iron oxide as the main component) as a raw material for the selective catalytic reduction of NO x by ammonia (NH 3 -SCR). Among the various formulations, the co-supported catalyst containing 5 % Mn and 5 % Co on CRS-400 exhibited exceptional SCR performance, achieving over 90 % conversion of NO x from 80 °C to 200 °C. The addition of 5 % Mn and 5 % Co as active components resulted in an increase in the specific surface area for catalytic performance and an enhancement of the redox capacity, leading to a significant improvement in catalyst activity. The catalyst’s efficient denitration performance was attributed to the synergistic interaction between Mn, Co, and Fe oxides, resulting in a catalyst with a higher proportion of adsorbed oxygen, as well as an elevated composition of Mn 4+ and Fe 2+ species. The catalyst demonstrated excellent SCR activity at low-temperatures, indicating its potential for downstream applications in soot treatment equipment. This would achieve the dual benefits of purifying the atmosphere and disposing of solid waste.
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
JOURNAL OF MATERIALS RESEARCH
·
2018
·Vol. 33
·期 16
·2414-2422
·
IF 1.495
Youchun Pan,Yuesong Shen,Qijie Jin,Shemin Zhu
A series of Ba-modified MnCeOx/TiO2 catalysts were prepared by a wet impregnation method and tested for selective catalytic reduction (SCR) of NO with NH3 at low temperature. The results showed that Ba additives obviously improved the catalytic performance of the MnCeOx/TiO2 catalyst for NH3-SCR, and the BaMnCeOx/TiO2 catalyst with 3 wt% BaO exhibited the optimal catalytic performance. Moreover, the introduction of Ba also improved the resistances toward water vapor and SO2 of catalysts. The N2 adsorption, H2-TPR, and X-ray photoelectron spectroscopy results showed that the addition of Ba increased the specific surface area, redox properties, and concentrations of surface Mn4+ and chemisorbed oxygen of catalysts. Furthermore, NH3-TPD and NO-TPD were used to investigate the absorption of NH3 and NO on the catalyst. The results revealed that although the introduction of Ba significantly promoted the adsorption of NO, it also inhibited the adsorption of NH3. Consequently, the catalytic performance of MnCeOx/TiO2 was greatly improved with the Ba additives.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Songjin Ko,Xiaolong Tang,Fengyu Gao,Honghong Yi,Hengheng Liu,Ning Luo
In this work, the phosphomolybdate (HPMo) modification strategy was applied to improve the N 2 selectivity of MnCo-BTC@SiO 2 catalyst for the selective catalytic reduction of NO x , and further, the mechanism of HPMo modification on enhanced catalytic performance was explored. Among MnCo-BTC@SiO 2 -x catalysts with different HPMo concentrations, MnCo-BTC@SiO 2 -0.75 catalyst exhibited not only the highest NH 3 -SCR performance (∼95% at 200-300°C) but also the best N 2 selectivity (exceed 80% at 100-300°C) due to the appropriate redox capacity, greater surface acidity. X-ray photoelectron spectrometer (XPS) and temperature programmed reduction of H 2 (H 2 -TPR) results showed that the modification with HPMo reduced the oxidation-reduction performance of the catalyst due to electron transfer from Mo 5+ to Mn 4+ /Mn 3+ and prevent the excessive oxidation of ammonia adsorption species. NH 3 temperature-programmed desorption of (NH 3 -TPD) results showed that the modification with HPMo could significantly improve the surface acidity and NH 3 adsorption, which enhance the catalytic activity and N 2 selectivity. In-situ diffused reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) revealed that modification with HPMo increased significantly the amount of adsorbed NH 3 species on the Bronsted acid site and C B / C L , it suppressed the production of N 2 O by inhibiting the production of NH species, the deep dehydrogenation of ammonia adsorption species. This study provided a simple design strategy for the catalyst to improve the low-temperature catalytic performance and N 2 selectivity.
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 RARE EARTHS
·
2022
·
IF 4.632
Yandi Cai,Peng Yang,Qinglong Liu,Kaili Ma,Wenxin Ma,Wang Song,Qiuhui Qian,Fei Gao,Wei Tan,Lin Dong
Sulfation treatment has been widely used to promote the catalytic performance of ceria (CeO 2 ) based catalysts for the selective catalytic reduction of NO by NH 3 (NH 3 -SCR of NO). Praseodymium oxide (PrO x ), another commonly used rare earth material with similar structural properties as CeO 2 , also shows satisfactory redox properties due to the facile redox cycle of Pr 3+ ↔ Pr 4+ . In this work, gas phase sulfation treatment with varied duration was performed on PrO x at 200 °C, and the NH 3 -SCR activity of sulfated PrO x was evaluated. Based on the results of systematic characterizations (e.g., N 2 -physisorption, NH 3 oxidation , NO oxidation, in situ diffuse Fourier transform infrared spectroscopy), it is revealed that the catalytic performance of sulfated PrO x is highly dependent on the sulfation time (or the amount of sulfate species deposited on PrO x ), which has a significant impact on the competitive reaction between NH 3 oxidation and NH 3 -SCR of NO, thus determining the NH 3 -SCR activity of PrO x . This work provides new insight into tuning the interaction between PrO x surface and reactants (NO, NH 3 ) via sulfation treatment, which cam guide the design and application of PrO x based catalysts for NH 3 -SCR of NO in the future.
研究领域:
化学工程
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环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Peipei Zhao,Mingyu Guo,Qingling Liu,Lijun Fan,Jinfeng Han,Caixia Liu,Na Ji,Chunfeng Song,Degang Ma,Zhenguo Li
A series of Mn a Zr b Cr c O x catalysts with different Cr/Mn molar ratios were synthesized via co-precipitation for the selective catalytic reduction of NO x with NH 3 (NH 3 -SCR). It was found that a Mn 5 Zr 2 Cr 2.5 O x catalyst with a Mn:Zr:Cr ratio of 5:2:2.5 exhibited excellent low-temperature activity and the best levels of H 2 O resistance at a high weight hourly space velocity (WHSV) of 54,000 ml/(h·g). NO conversion levels were measured as greater than 87% within a temperature range of 150–250 °C, and catalytic performance levels reached 90% even 50 h after reactions occurred in the presence of 15% H 2 O at 230 °C. The characterization results show that strong interactions occurring between Mn, Zr and Cr oxides and higher quantities of Mn 4+ and Lewis acid sites improved the redox properties and facilitated H 2 O resistance. In situ diffuse reflectance infrared Fourier transform spectra ( in situ DRIFTS) show that coordinated NH 3 on Lewis acid sites and bidentate nitrates play important roles in SCR reactions and that such reactions follow both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. The competitive adsorption of H 2 O and NO may be the main cause of the adverse effects of H 2 O on catalytic performance.
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
ENERGY & FUELS
·
2025
·
IF 5.3
Fang Wang,Xueyan Wu,Yuxuan Han,Yan Lv,Jixi Guo,Xiaoman Li,Yaping Zhang
In cement kiln flue gas emissions, high concentrations of alkali and alkaline earth metals cause the deactivation of the NbCe/Ti catalysts, significantly reducing their operational lifespan under industrial conditions. Here, the NbCe-loaded titanium nanotubes (NbCe/TiNTs) catalyst has been synthesized via hydrothermal and impregnation methods. The NbCe/TiNTs catalyst exhibits superior resistance to potassium (K) and calcium (Ca) poisoning. Notably, NbCe/TiNTs catalyst maintains high NOx conversion across a wide temperature range (192–350 °C). The 5Ca-NbCe/TiNTs and 3K-NbCe/TiNTs catalysts achieve a 90% NOx conversion at 235 and 242 °C, respectively, demonstrating remarkable resistance to K and Ca poisoning. The results indicate that TiNTs supports enhance both the specific surface area and surface acid sites of the catalyst, synergistically improving its resistance to K and Ca poisoning. Furthermore, an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study elucidates selective catalytic reduction with the NH3 (NH3-SCR) reaction mechanism, revealing dual contributions from both the Eley–Rideal (E–R) and Langmuir–Hinshelwood (L–H) mechanisms on the catalyst. This work provides a research direction for enhancing the alkali poisoning resistance of NOx removal catalysts.
研究领域:
环境催化
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材料科学
·
化学工程
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Guoquan Liu,He Zhang,Pengfei Wang,Yi Li,Xueyue Mi,Sihui Zhan
Reducing the poisoning effect of alkaline earth metals over catalysts in industrial fields presents a great challenge to selective catalytic reduction (SCR) of NO x with ammonia. Herein, we successfully introduce sulfates to the surface of supported manganese-based oxides (Nb/MnO 2 -S) for trapping calcium species, and Nb/MnO 2 -S catalyst with superior low-temperature performance and calcium-resistant property still exhibits excellent de-NO x activity in a wide operating temperature window (175–350 °C, over 80 % NO x conversion with a gas hourly space velocity of 60,000 h −1 ) after calcium poisoning. In this case, the addition of sulfates increased the quantity of chemisorbed oxygen on Nb/MnO 2 -S, thus accelerating the redox cycle in NH 3 -SCR reaction. Significantly, compared with calcium-poisoned Nb/MnO 2 , relevant spectroscopy analysis and theoretical calculations further reveal that sulfates species prefer to interact with calcium and release the Nb active sites, which maintains the efficient NH 3 adsorption and preserves a large amount of Brønsted acid sites over calcium-poisoned Nb/MnO 2 -S, thus promoting calcium-resistant performance. This work will provide a general strategy to develop calcium-resistant SCR catalysts with low-temperature activity for industrial applications.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 10
·4335-4345
·
IF 2.7
Jiali Zhang,Zhen Yan,Yanke Yu,Yanpeng Li
CuO/TiO2 catalysts with varying Sb doping ratios were synthesized and applied in the NH3-SCR process. The results of activity tests revealed that the addition of Sb effectively enhanced the performance of low-temperature SCR. Particularly, the CuSbTiOx-0.2 catalyst exhibited the highest activity, achieving over 91% conversion at 250 °C, along with the highest N2 selectivity and exceptional resistance to SO2. Comprehensive characterization analyses demonstrated that CuSbTiOx-0.2 possessed a significantly large specific surface area, the strongest surface acidity, and superior redox performance among the catalysts studied. In situ DRIFTS experiments provided further insights, indicating that Sb modification generated more active species, thereby enhancing the reactivity of ad-NH3 and ad-NOx species. The SCR reaction mechanism for CuSbTiOx-0.2 predominantly followed the Langmuir–Hinshelwood (L–H) and Eley–Rideal (E–R) mechanisms. These findings have the potential to advance the development of novel and effective non-vanadium SCR catalysts.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2016
·
IF 4.012
Peng Sun,Rui-tang Guo,Shu-ming Liu,Shu-xian Wang,Wei-guo Pan,Ming-yuan Li
A series of MnEuOx catalysts were prepared by the co-precipitation method and used for selective catalytic reduction of NOx with NH 3 . It was found that the modification of MnOx catalyst by Eu with a Eu/Mn molar ratio of 0.1 could greatly enhance its SCR activity and broaden its operating temperature window, accompanied by good resistance to SO 2 and H 2 O. From the characterization results of N 2 adsorption, XRD, XPS, H 2 -TPR, it could be concluded that the larger surface area resulted from the inhibited crystallization of MnOx, the enrichment of surface Mn 4+ and chemisorbed oxygen, and the higher reducibility all made a contribution to the high SCR activity of MnEuOx-0.1 catalyst. Furthermore, the results of in situ DRIFTS study revealed the NH 3 -SCR reactions over MnOx and MnEuOx-0.1 were mainly controlled by L-H mechanism (<150 °C) and E-R mechanism (>150 °C) respectively, and the contribution of E–R mechanism became more important with increasing reaction temperature. The enhanced NO oxidation and NH 3 adsorption should be mainly contribute to the distinguished SCR performance of MnEuOx catalyst in the lower temperature range (<150 °C) and higher temperature range (>150 °C) respectively.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Chaoqun Bian,Xiaohui Luo,Xiao Chen,Rongrong Liu,Jingqiu Li,Gaoyuan Zhu,Hao Xu,Shichao Han,Jie Zhu,Longfeng Zhu
Cu-SSZ-39 zeolite with 8-membered rings is regarded as a very promising catalyst in the NH3-SCR reaction, but its hydrothermal stability still remains to be improved. One of the solutions to promote hydrothermal stability is the insertion of rare earth elements in the product. Nevertheless, normal ion exchange of rare earth elements limits their contents in the zeolite product due to their large hydrated ionic radius and alkaline environment under hydrothermal conditions. Herein, we for the first time present a new method for the one-pot synthesis of Ce-SSZ-39 zeolite under solvent-free conditions. The key to success is the use of Ce-FAU zeolite as a precursor. The obtained product shows good crystallinity, sheet-like morphology, large BET surface area, and 4-coordinated Al species. Detailed investigations illustrate that Ce species in the Cu/Ce-SSZ-39 zeolite micropore can prevent the dealumination and thus formation of CuAlOx species during hydrothermal aging at 850 °C for 16 h, giving the excellent hydrothermal stability and thus showing the excellent catalytic performance in the NH3-SCR reaction. One-pot synthesis of Ce-SSZ-39 zeolite with excellent catalytic performance might open a new door for developing very efficient selective catalytic reduction (SCR) catalysts in near future.
研究领域:
催化材料
·
环境化学
✓ 已验证
产品关联
DOI
PubMed
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
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
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