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
Catalysts
·
2016
·Vol. 6
·期 8
·112
·
IF 2.964
Xiaobo Wang,Lei Zhang,Shiguo Wu,Weixin Zou,Shuohan Yu,Ye Shao,Lin Dong
A series of Fe–Ce–Ti catalysts were prepared via co-precipitation method to investigate the effect of doping Ce into Fe–Ti catalysts for selective catalytic reduction of NO with NH3. The NO conversion over Fe–Ce–Ti catalysts was considerably improved after Ce doping compared to that of Fe–Ti catalysts. The Fe(0.2)–Ce(0.4)–Ti catalysts exhibited superior catalytic activity to that of Fe(0.2)–Ti catalysts. The obtained catalysts were characterized by N2adsorption (BET), X-ray diffraction (XRD), temperature programmed reduction (H2-TPR), temperature programmed desorption (NH3-TPD), Fourier transform infrared (FT-IR) spectrophotometry, thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS). The data showed that the introduction of Ce results in higher surface area and better dispersion of active components on the catalyst surface and enhances the amount of surface acid sites. The interactions between Fe and Ce species were found to improve the redox ability of the catalyst, which promotes catalytic performance at low temperature. The XPS results revealed that Fe3+/Fe2+and Ce4+/Ce3+coexisted on the catalyst surface and that Ti was in 4+ oxidation state on catalyst surface. Ce doping increased the atomic ratio of Fe/Ti and Ce/Ti and enhanced the surface adsorbed oxygen species. In addition, Fe(0.2)–Ce(0.4)–Ti catalyst also showed better tolerance to H2O and SO2and up to 92% NO conversion at 270 °C with 200 ppm SO2added over 25 h, which suggests that it is a promising industrial catalyst for mid-low temperature NH3–selective catalytic reduction (SCR) reaction.Keywords:SCR;denitration;catalytic activity;synergistic effect;SO2resistance
研究领域:
环境科学
·
催化化学
✓ 已验证
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
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rui Li,Xiangqiong Jiang,Jiecheng Lin,Zhiping Zhang,Qintong Huang,Guangying Fu,Yujun Zhu,Jiuxing Jiang
SSZ-16 zeolite with AFX topology was synthesized by hydrothermal method using 1,4-diazabicyclo[2.2.2]-octane-C4-diquat dibromide as organic structure directing agent. Cu x -SSZ-16 catalysts were prepared by exchanging SSZ-16 zeolite with Cu and applied for selective catalytic reduction (SCR) of NO x with ammonia. Among these catalysts, Cu 2.2 -SSZ-16 performs the best SCR denitration (deNO x ) performance that above 90% NO x conversion can be achieved at 175–600 °C. Especially, the influences of the hydrothermal aging at various temperatures (650, 750 and 850 °C) on active species and AFX framework of the Cu 2.2 -SSZ-16 catalyst are investigated in detail by various characterization methods including XRD, SEM , H 2 -TPR, NMR, UV–vis-DRS, EPR, NH 3 -TPD and in situ DRIFTS . Cu 2.2 -SSZ-16 still shows good NH 3 -SCR activity after hydrothermal aging at 650 and 750 °C due to more Cu 2+ -2Z species in the sample. Still, obvious deactivation can be observed after hydrothermal aging at 850 °C because of the collapse of AFX skeleton and the weak interaction between active Cu species and the skeleton. Nevertheless, Cu 2.2 -SSZ-16 is a competitive candidate for NH 3 -SCR deNO x reaction in practical applications.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xinyu Han,Kaijie Liu,Mengyao Bian,Zhaoxu Yuan,Yannan Li,Yunlong Zhang,Xiangguang Yang,Yibo Zhang
Despite SO 2 being recognized as a catalyst poisoning substance, a trace amount can enhance the acidity of the NH 3 -SCR (selective catalytic reduction) catalyst, which facilitates NH 3 adsorption and accelerates the reaction rate according to the Eley-Rideal mechanism. In this study, monoatomically dispersed Ce atoms were doped into the MoTiO x lattice to regulate the quantity and distribution of sulfate. This regulation was achieved by leveraging the stronger affinity of SO 2 to Ce, thus maximizing the acidifying effect of SO 2 to boost the NH 3 -SCR performance of the catalyst. The catalyst demonstrated the ability to maintain over 80 % NO x conversion for at least 144 hours in the presence of high concentration SO 2 (250 ppm). A detailed examination of the surface dynamics after SO 2 introduction revealed that NH 4 (SO 4 ) 2 , formed on the surface, converted to NH 4 HSO 4 . The decomposition of NH 4 HSO 4 extracted lattice oxygen from the catalyst, leading to an increase in oxygen vacancies on the catalyst surface as the duration of SO 2 exposure increased. The surface-adsorbed oxygen, brought about by these oxygen vacancies, was readily activated, which promoted the dehydrogenation process of NH 3 and the progression of NH 3 -SCR. Further, based on the discovery of the unique phenomenon and mechanism of NH 4 HSO 4 decomposition that generates oxygen vacancies, gases containing poisonous SO 2 were utilized for the pretreatment of the catalyst to optimize its surface and enhance its sulfur resistance (fighting poison with poison). The results demonstrated that the pretreated catalyst rapidly achieved optimal NO x conversion and maintained catalytic stability for over 240 h even in the presence of 250 ppm SO 2 without any decrease in activity. This research innovatively leveraged the poisonous SO 2 to optimize the catalyst's surface, thereby achieving higher catalytic performance and sulfur resistance, which offers valuable insights into the design of novel sulfur-resistant catalysts.
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
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Lei Chen,Ding Weng,Jiadao Wang,Duan Weng,Li Cao
The CeO 2 -TiO 2 (CeTi) and CeO 2 /WO 3 -TiO 2 (CeWTi) catalysts were prepared by a sol-gel precipitation method and their NH 3 -NO/NO 2 selective catalytic reduction (SCR) performance was studied. N 2 O formation and effect of oxygen concentration on SCR performance over CeWTi catalyst were also investigated while varying the NO 2 /NO x ratio. Results indicate that fast SCR behavior of CeWTi catalyst has the best NH 3 -NO/NO 2 SCR performance due to the catalyst reoxidation rate by NO 2 higher than by O 2 . Compared with CeTi catalyst, CeWTi catalyst exhibits higher de-NO x performance under NH 3 -NO/NO 2 SCR conditions. As the CeTi and CeWTi catalysts exhibit similar redox property, addition of WO 3 provides more acid sites which accelerate the reaction between NH 4 NO 3 and NO to get a superior low-temperature activity. Amount of N 2 O formation shows a peak at 250 °C mainly derived from NH 4 NO 3 decomposition.
研究领域:
催化劑科學
·
環境工程
✓ 已验证
产品关联
DOI
高影响因子
Materials
·
2023
·Vol. 16
·期 7
·2903
·
IF 3.4
Youye Ma,Kanghui Cai,Guojie Xu,Yueling Xie,Peng Huang,Jun Zeng,Ziming Zhu,Jie Luo,Huawen Hu,Kai Zhao,Min Chen,Kun Zheng
Ultrafine Polyvinyl alcohol (PVA) fibers have an outstanding potential in various applications, especially in absorbing fields. In this manuscript, an electrostatic-field-assisted centrifugal spinning system was designed to improve the production efficiency of ultrafine PVA fibers from PVA aqueous solution for NH3adsorption. It was established that the fiber production efficiency using this self-designed system could be about 1000 times higher over traditional electrospinning system. The produced PVA fibers establish high morphology homogeneity. The impact of processing variables of the constructed spinning system including rotation speed, needle size, liquid feeding rate, and voltage on fiber morphology and diameter was systematically investigated by SEM studies. To acquire homogeneous ultrafine PVA fiber membranes, the orthogonal experiment was also conducted to optimize the spinning process parameters. The impact weight of different studied parameters on the spinning performance was thus provided. The experimental results showed that the morphology of micro/nano-fibers can be well controlled by adjusting the spinning process parameters. Ultrafine PVA fibers with the diameter of 2.55 μm were successfully obtained applying the parameters, including rotation speed (6500 rpm), needle size (0.51 mm), feeding rate (3000 mL h−1), and voltage (20 kV). Furthermore, the obtained ultrafine PVA fiber mat was demonstrated to be capable of selectively adsorbing NH3gas relative to CO2, thus making it promising for NH3storage and other environmental purification applications.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Jiancheng Wang,Zhaoliang Peng,Ying Chen,Weiren Bao,Liping Chang,Gang Feng
Cu-SSZ-13/cordierite monolithic catalyst was prepared by in situ hydrothermal synthesis method. The physicochemical properties of the as-prepared Cu-SSZ-13/cordierite were investigated by X-ray diffraction analysis, scanning electron microscopy, transmission electron microscopy, N 2 -adsorption, inductively coupled plasma, X-ray photoelectron spectroscopy, and solid-state NMR techniques. The removal of nitrogen oxides (NO x ) from simulated diesel vehicle exhaust gas was performed using fixed-bed reactor. The effects of crystallization time and addition of HF during hydrothermal synthesis, reaction space velocity, and aging treatment of catalyst on the catalytic performances of NO x reduction reactions were investigated. The results indicate that the optimum crystallization time was 72 h. Highly crystalline structure of zeolite Cu-SSZ-13 was formed, in a close combination with a carrier, via one step hydrothermal process. Cu-SSZ-13/cordierite showed excellent DeNO x performance for selective catalytic reduction (SCR) and anti-aging properties in a simulated diesel exhaust gas under a high space velocity. At a high space velocity of 72,000 h −1 , the highest conversion and N 2 selectivity of 94% and 90%, respectively, were achieved. After the aging for 50 h at 720 °C, NO x reduction rate was still >80% in the temperature range of 350–550 °C. The larger height to diameter ratio of the same catalysts enhanced the NH 3 -SCR catalytic activity and broadened the active temperature window. The addition of HF increased the catalytic activity and anti-aging performance of the sample.
研究领域:
催化材料
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 22
·27663-27673
·
IF 3.056
Liu Yuan-zhen,Xu Qi-yan,Guo Rui-tang,Duan Chao-peng,Wu Gui-lin,Miao Yu-fang,Gu Jing-wen
The Cu/TiO 2 catalysts with the addition of Eu were developed by the sol-gel way for the selective catalytic reduction (SCR) of NO x by NH 3 . Activity tests revealed that CuEu/TiO 2 -0.15 catalyst showed the optimal de-NO x performance in a wide temperature range (150–300 °C), along with an admirable SO 2 tolerance. According to characterization analysis, the relationship between the NH 3 -SCR performance and physicochemical characters of samples was explored. The adjunction of Eu on Cu/TiO 2 catalyst can contribute to the formation of a large amount of Cu 2+ , adsorbed oxygen, and acid sites on the catalyst surface. Moreover, the Eu addition on Cu/TiO 2 is favorable to the generation of activated NO x and NH 3 substances adsorbed on the catalyst surface, which would conduce to the NH 3 -SCR process by Langmuir-Hinshelwood (L-H) mechanism effectively.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Hanzi Liu,Yi Zhang,Haiming Wang,Changfu You
Selective non-catalytic reduction of NOx (SNCR) with NH 3 is commonly used in industrial facilities like circulating fluidized bed (CFB) furnaces. However, the strongly temperature-dependent de-NOx feature confines its applications in a specific temperature range (900–1050 °C). Here, we report a new strategy on using Fe-Ni-W exchanged zeolite (0.5FNW-H) as a catalyst to extend the SNCR temperature window. In the CFB reactor, a significant NOx conversion improvement ranging from 14.1% to 80.9% was achieved at 700 to 850 °C by applying the developed catalyst. Catalyst dosage of 4500 h −1 (GHSV), a particle diameter of 0.1–0.3 mm, and NH 3 injection position at the dense-phase zone were found preferred for NOx reduction with the highest efficiency of ~85% at 700 °C. The physicochemical properties of the catalysts remained stable after the circulating reactions in the CFB reactor. The developed catalyst is particularly applicable for improving the SNCR performance when the thermal power plants are operated at low loads.
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
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 8
·2270-2279
·
IF 3.186
Bie Xuan,Jiao Kunling,Gong Chunqin,Qu Baozhong,Liu Daokuan,Ma Shuangchen
To develop highly efficient NH 3 -SCR catalysts with a wide temperature range, catalysts based on MnAlO x and Cerium elements loading with various mixing ratios were prepared for selective catalytic reduction of NO by NH 3 . The special role of cerium was demonstrated by the surface structure characteristics and unique catalytic performance, involving the surface-active sites and compositions analysis. Interestingly, the strengthening of Mn 1.2 Al 0.8 Ce a O x on both acid sites, especially medium acids and strong acids, were clearly manifested. Meanwhile, the strong interaction between MnAlOx and CeO 2 enabled favorable electron transfers from MnOx to CeO 2 while generating more oxygen vacancies and active oxygen species, consequently accelerating the redox cycle. The results illustrate that the NOx conversion and the selectivity of N 2 can be improved with more medium acids tuned by appropriate Ce adding. However, an opposite effect will appear by excessive addition. In addition, the reaction mechanisms at different acid sites are revealed. Our findings, therefore, provide a strategy for the rational design of moderate-temperature NH 3 -SCR catalysts through adding-induced component engineering of composite materials. Graphic Abstract Mn 1.2 Al 0.8 Ce a O x Catalysts with different surface features were fabricated by an environment-friendly method. The strong interaction between MnAlOx and CeO 2 was systematically illustrated. Meanwhile, the importance of medium acids was convincingly revealed. And the reaction mechanisms at different acid sites were demonstrated. These provide a strategy for the rational design of moderate-temperature NH 3 -SCR catalysts through adding-induced component engineering of composite materials.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yarong Bai,Houlin Wang,Chao Jin,Chuan Gao,Shangchao Xiong,Zhengjun Gong,Yue Peng,Junhua Li
Precision modulation of metal-support interactions is essential for optimizing catalytic activity and selectivity in automotive exhaust treatment. In this study, we systematically regulate the strength of Pt-CeO 2 interaction by altering Pt anchoring strategies on Al 2 O 3 , thereby achieving a controlled balance between NO x reduction efficiency and by-product formation. Comprehensive structural and spectroscopic analyses reveal that increasing the interaction strength (PtCeAl-mix
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）