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Design of Ca-type todorokite catalysts with highly active for the selective reduction of NO_(x) by NH_(3) at low temperatures

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Journal of Environmental Sciences 2024年第4期138卷 697-708页

作者： Chuang Chang Zidi Yan Chunlei Zhang Yanshuang Zhang Miao Jiang Luna Ruan Min Xiao yunbo yu Hong He School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Ca-type todorokite catalysts were designed and prepared by a simple redox method and applied to the selective reduction of NO_(x) by NH_(3)(NH_(3)-SCR)for the first *** with the Na-type manjiroite prepared by the same method,the todorokite catalysts with different Mn/Ca ratios showed greatly improved catalytic activity for NO_(x) *** them,Mn8Ca4 catalyst exhibited the best NH_(3)-SCR performance,achieving 90%NO_(x) conversion within temperature range of 70-275℃ and having a high sulphur *** to the Na-type manjiroite sample,Ca-type todorokite catalysts possessed an increased size of tunnel,resulting in a larger specific surface *** increased the amounts of Ca doping,the Na content in Ca-type todorokite catalysts significantly decreased,providing larger amounts of Bronsted acid sites for NH_(3) adsorption to produce NH_(4)^(+).The NH_(4)^(+)species were highly active for reaction with NO+O_(2),playing a determining role in NH_(3)-SCR process at low ***,larger amounts of surface adsorbed oxygen contained over the Ca-doping samples than that over Na-type manjiroite,promoting the oxidation of NO and fast SCR *** the Ca-type todorokite catalysts,furthermore,nitrates produced during the flow of NO+O_(2),were more active for reaction with NH_(3) than that over Na-type manjiroite,benefiting the occurrence of NH_(3)-SCR *** study provides novel insights into the design of NH_(3)-SCR catalysts with high performance.

关键词： NO_(x) NH_(3)-SCR Mn-based oxides Ca-type todorokite Bronsted acid sites

Interface sites on vanadia-based catalysts are highly active for NO_(x) removal under realistic conditions

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Journal of Environmental Sciences 2024年第2期136卷 523-536页

作者： Zhihui Lv Guangzhi He Wenshuo Zhang Jingjing Liu Zhihua Lian Yang Yang Zidi Yan Guangyan Xu Wenpo Shan yunbo yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China Ningbo Research Center for Urban Environment Chinese Academy of SciencesNingbo 315800China

TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic *** these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface *** reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working *** the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O *** wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)*** wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.

关键词： NO_(x)removal Vanadia-based catalysts V-O-Ti entities Interface sites Reaction mechanism

Shape dependence of support for NO_x storage and reduction catalysts

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Journal of Environmental Sciences 2019年第1期31卷 396-407页

作者： Wen Xie yunbo yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of Sciences University of Chinese Academy of Sciences Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences

Pt/BaO/Al_2O_3 catalysts with different BaO loadings prepared from Al_2O_3 nanorods(Pt/BaO/Al_2O_3-nr) and irregular Al_2O_3 nanoparticles(Pt/BaO/Al_2O_3-np) were investigated for NOx storage and reduction(NSR). The Pt/BaO/Al_2O_3 materials derived from Al_2O_3 nanorods always exhibited much higher NOx storage capacity(NSC) over the whole temperature range of 100–400°C than the corresponding Pt/BaO/Al_2O_3-np samples containing the same BaO loading, giving the maximum NSC value of 966.9 μmol/gcatat 400°C, 1.4 times higher than that of Pt/BaO/Al_2O_3-np. Higher catalytic performance of nanorod-supported NSR samples was also observed during lean-rich cyclic conditions(90 sec vs. 5 sec), giving more than 98% NOx conversion at 300–450°C over the Pt/BaO/Al_2O_3-nr sample with 15% BaO loading. To reveal this dependence on the shape of the support during the NSR process, a series of characterization techniques including the Brunauer–Emmett–Teller(BET) method,X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), H_2 temperature programmed reduction(H2-TPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) were also conducted. It was found that intimate contact of Ba–Al and Ba–Pt sites was achieved over the Pt/BaO/Al_2O_3 surface when using Al_2O_3-nr as a *** strong interaction among the multi-components of Pt/BaO/Al_2O_3-nr thus triggered the formation of surface nitrite and nitrate during the lean period, and also accelerated the reverse spillover of ad-NOxspecies onto the Pt surface, enhancing their reduction and leading to high NSR performance.

关键词： NOx storage and reduction Pt/BaO/Al2O3 Nanorod Morphology effect Strong interaction

Oxygen adatoms and vacancies on the (110) surface of CeO2

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Science China(Technological Sciences) 2018年第1期61卷 135-139页

作者： HUANG JingLu yu yunbo ZHU Jing yu Rong National Center for Electron Microscopy in Beijing Key Laboratory of Advanced Materials of Ministry of Education of China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China University of Chinese Academy of Sciences Beijing 100049 China

The behavior of oxygen on ceria surfaces is closely related with the applications of ceria as a catalyst and oxygen conductor in solid-oxide fuel cells. Here, the atomic configurations of oxygen adatoms and vacancies on the(110) surface of CeO_2 have been studied combining aberration-corrected transmission electron microscopy and first-principles calculations. The oxygen adatoms were estimated to be located on top of Ce atoms with 50% coverage, forming a c(2×2) reconstruction. The oxygen vacancies can form stable configuration, with the Ce atoms partly reduced.

关键词： surface structure ceria oxygen adatoms oxygen vacancies aberration-corrected TEM first-principles calculations

Low CO content hydrogen production from oxidative steam reforming of ethanol over CuO-CeO_2 catalysts at low-temperature

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Journal of Energy Chemistry 2013年第6期22卷 861-868页

作者： Xue Han yunbo yu Hong He Jiaojiao Zhao Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

CuO-CeO2 catalysts were prepared by a urea precipitation method for the oxidative steam reforming of ethanol at *** catalytic performance was evaluated and the catalysts were characterized by inductively coupled plasma atomic emission spectroscopy,X-ray diffraction,temperature-programmed reduction,field emission scanning electron microscopy and thermo-gravimetric *** CuOCeO2 catalysts,H2 with low CO content was produced in the whole tested temperature range of 250–450 *** non-noble metal catalyst 20CuCe showed higher H2production rate than 1%Rh/CeO2 catalyst at 300–400 C and the advantage was more obvious after 20 h testing at400 *** results further confirmed that CuO-CeO2 catalysts may be suitable candidates for low temperature hydrogen production from ethanol.

关键词： CuO-CeO2 catalyst hydrogen production oxidative steam reforming low-temperature

Alkali resistance promotion of Ce-doped vanadium-titanic- based NH3-SCR catalysts

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Journal of Environmental Sciences 2018年第11期30卷 155-161页

作者： Zidi Yan Xiaoyan Shi yunbo yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China University of Chinese Academy of Sciences Beijing 100049 China Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China

The effect of K deactivation on V2OJWO3-TiO2 and Ce-doped V2O5/WO3-TiO2 catalysts in the selective catalytic reduction （SCR） of NOx by NH3 was studied. Ce-doped V2O5/WO3-TiO2 showed significantly higher resistance to K deactivation than V2O5/WO3-TiO2. Ce-doped V2O5/WO3-TiO2 with K/V = 4 （molar ratio） showed 90% NOx conversion at 350℃, whereas in this case V2O5/WO3-TiO2 showed no activity. The fresh and K-poisoned V2O5/WO3-TiO2 and Ce-doped V2O5/WO3-TiO2 catalysts were investigated by means of in situ diffuse reflectance infrared Fourier transform spectroscopy （DRIFTS）, NH3-temperature progress decomposition （NH3-TPD）, X-ray photoelectron spectroscopy （XPS） and H2-temperature program reduction （H2-TPR）. The effect of Ce doping on the improving resistance to K of V2O5/WO3- TiO2were discussed.

关键词： Selective catalytic reduction Ammonia Nitrogen oxides V2O5/WO3-TiO2 Alkali deactivation

Modeling of microstructure evolution and mechanical properties during hot-strip rolling of Nb steels

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Journal of University of Science and Technology Beijing 2008年第4期15卷 396-401页

作者： yunbo Xu Yongmei yu Xianghua Liu Cruodong Wang State Key Laboratory of Rolling and Automation Northeastem University Shenyang 110004 China

An integrated metallurgical model was developed for Nb steels to predict the microstructure evolution and mechanical properties during the hot-strip rolling and cooling process. On the basis of the industrial data, the transformation kinetics, strength, and elongation rate were evaluated for different chemical compositions and processing parameters. The yield strength and tensile strength increase with increasing Nb content or decreasing finishing temperature. The bainite distributed in finer ferrite matrix, which is produced at relatively low coiling temperatures, can greatly increase the strength of steel, especially tensile strength, thereby decreasing the yield ratio. A reasonable agreement was found between the predicted and measured results. It indicates that the present models can be used to simulate the actual production process.

关键词： hot-strip rolling transformation microstructure mechanical properties grain size

Complete catalytic oxidation of o-xylene over CeO_2 nanocubes

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Journal of Environmental Sciences 2011年第1期23卷 160-165页

作者： Lian He yunbo yu Changbin Zhang Hong He State Key. Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China

The activities of CeO2 nanocubes calcined at different temperatures were tested for catalytic oxidation of o-xylene. Using CeO2 nanocubes as catalysts, complete catalytic oxidation of o-xylene was achieved below 210℃. The CeO2 nanomaterials were characterized by means of BET, X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and high-resolution transmission electron microscopy （HRTEM）. From the TEM images, all CeO2 nanocubes displayed cubic morphology irrespective of calcination temperature. The HRTEM images revealed that these nanocubes were enclosed by reactive {001} planes, which may contribute to the intrinsically catalytic property of o-xylene oxidation. The higher activity of CeO2 nanocubes calcined at 550℃ than those calcined at above 550℃ was attributed to their smaller crystallite size and larger surface area. The influences of reaction conditions were also studied, which found that a higher reaction temperature was necessary for complete catalytic oxidation of o-xylene at higher weight hourly space velocity （WHSV） and o-xylene concentration.

关键词： CeO2 nanocubes o-xylene catalytic oxidation calcination temperature

Influence of NO_(x) on the activity of Pd/θ-Al_(2)O_(3) catalyst for methane oxidation: Alleviation of transient deactivation

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Journal of Environmental Sciences 2022年第2期34卷 38-47页

作者： Chang Cui Yan Zhang Wenpo Shan yunbo yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Ningbo Research Center for Urban Environment Chinese Academy of SciencesNingbo 315800China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China

Alumina supported Pd catalyst(Pd/Al_(2)O_(3)) is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900 ℃ and isothermal experiments at 650 ℃ were conducted to investigate the influence of NO_(x) on transient deactivation of Pd/θ-Al_(2)O_(3) catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient deactivation in the cooling ramp from 800 to 500 ℃, which was resulted from the in situ formation of NO_(2) during the process of methane oxidation. Over the Pd/θ-Al_(2)O_(3), thermogravimetric analysis and O_(2) temperature programmed oxidation measurements confirmed that transient deactivation was due to the decomposition of Pd O particles and the hysteresis of Pd reoxidation, while the metal Pd entities were less active for methane oxidation than the Pd O ones. CO pulse chemisorption and scanning transmission electron microscopy characterizations rule out the NO_(2) effect on Pd size change. Powder X-ray diffraction and X-ray photoelectron spectroscopy characterizations were used to obtain palladium status of Pd/θ-Al_(2)O_(3) before and after reactions, indicating that in lean conditions at 650 ℃, the presence of NO_(2) increases the content of active Pd O on the catalyst surface, thus benefits methane oxidation. Homogeneous reaction between CH 4, O_(2), and NO_(x) may be partially responsible for the alleviation above 650 ℃. The interesting research of alleviation in transient deactivation by NO_(x), the components co-existing in exhausts, are of great significance for the application.

关键词： Methane Catalytic oxidation Palladium NO_(x)influence