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In-plasma catalytic degradation of toluene over different MnO_2 polymorphs and study of reaction mechanism

Chinese Journal of Catalysis 2017年第5期38卷 793-804页

作者： Ting Wang Si Chen Haiqiang Wang Zhen Liu zhongbiao wu Key Laboratory of Environment Remediation and Ecological Health of Ministry of Education College of Environmental & Resources Sciences Zhejiang University Hangzhou 310058 Zhejiang China Zhejiang Provincial Engineering Research Center of Industrial Boiler & Furnace Flue Gas Pollution Control Hangzhou 310027 Zhejiang China Institute of Industrial Ecology and Environment College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310007 Zhejiang China

α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic *** relationship between catalytic performance and MnO2crystal structures was *** was noted that the toluene removal efficiency was32.5%at the specific input energy of160J/L when non‐thermal plasma was used ***α‐MnO2catalyst showed the best activity among the investigated catalysts,yielding a toluene conversion of78.1%at the specific input energy of160J/***β‐MnO2,γ‐MnO2andδ‐MnO2,removal efficiencies of47.4%,66.1%and50.0%,respectively,were *** powder X‐ray diffraction,Raman spectroscopy,transmission electron microscopy,scanning electron microscopy,Brunauer‐Emmett‐Teller,H2temperature‐programmed reduction and X‐ray photoelectron spectroscopy analyses,it was concluded that the tunnel structure,the stability of the crystal in plasma,the Mn-O bond strength of MnO2and the surface‐chemisorbed oxygen species played important roles in the plasma‐catalytic degradation of ***,the degradation routes of toluene in non‐thermal plasma and in the plasma‐catalytic process were also *** was concluded that the introduction of MnO2catalysts enabled O3,O2,electrons and radical species in the gas to be adsorbed on the MnO2surface via a facile interconversion among the Mn4+,Mn3+and Mn2+*** four species could then be transported to the toluene or intermediate organic by‐products,which greatly improved the toluene removal efficiency and decreased the final output of by‐products.

关键词： Toluene Catalytic oxidation Non‐thermal plasma MnO2 Crystal structure

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Structural effect and reaction mechanism of MnO_2 catalysts in the catalytic oxidation of chlorinated aromatics

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Chinese Journal of Catalysis 2019年第5期40卷 638-646页

作者： Xiaole Weng Yu Long Wanglong Wang Min Shao zhongbiao wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental and Resource SciencesZhejiangUniversityHangzhou 310058ZhejiangChina Zhejiang Provincial Engineering Research Center of Industrial Boiler & Furnace Flue Gas Pollution Control Hangzhou 310058ZhejiangChina State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Environmental and climate Research institute Jinan UniversityGuangzhou 511443GuangdongChina

Various MnO2 structures have been extensively applied in catalysis. In this study,γ-MnO2,α-MnO2, and δ-MnO2 with corresponding rod, tube, and hierarchical architecture morphologies were prepared and applied for the catalytic oxidation of chlorobenzene (CB). The redox ability, H2O activation behavior, and acidity of MnO2 were analyzed using a range of techniques, including TPR, H2O-TPD, XPS, and pyridine-IR. The catalytic activities in CB oxidation were assessed;this revealed that γ-MnO2 exhibited the highest activity and best stability, owing to its enriched surface oxygen vacancies that functioned to activate O2 and H2O, and capture labile chlorine, which reacted with dissociated H2O to form HCl. All the MnO2 phases generated toxic polychlorinated by-products, including CHCl3, CCl4, C2HCl3, and C2Cl4, indicating the occurrence of electrophilic chlorination during CB oxidation. In particular, the dichlorobenzene detected in the effluents of α-MnO2 might generate unintended dioxins via a nucleophilic substitution reaction.

关键词： MnO2 Chlorobenzene Catalytic oxidation Polychlorinated byproducts Environmental risk

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One-step synthesized SO_4^(2-)-TiO_2 with exposed(001) facets and its application in selective catalytic reduction of NO by NH_3

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Chinese Journal of Catalysis 2018年第4期39卷 771-778页

作者： Yexuan Wen Shuang Cao Xiaoqi Fei Haiqiang Wang zhongbiao wu Key Laboratory of Environment Remediation and Ecological Health of Ministry of Education College of Environmental&Resources SciencesZhejiang UniversityHangzhou 310058ZhejiangChina Zhejiang Provincial Engineering Research Center of Industrial Boiler&Furnace Flue Gas Pollution Control Hangzhou 310027ZhejiangChina

A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling *** doping ceria,Ce/TiO2‐001 was used as the catalyst for selective catalytic reduction(SCR)of NO with *** with Ce/P25(Degussa P25 TiO2)and Ce/P25‐S(sulfated P25)catalysts,Ce/TiO2‐001 was more suitable for medium‐and high‐temperature SCR of NO due to the high surface area,sulfation,and the excellent properties of the active‐energy(001)*** of these facilitated the generation of abundant acidity,chemisorbed oxygen,and activated NOx‐adsorption species,which were the important factors for the SCR reaction.

关键词： Anatase TiO2 Sulfation (001)facets Ceria Selective catalytic reduction

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Synergetic effect between non-thermal plasma and photocatalytic oxidation on the degradation of gas-phase toluene: Role of ozone

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Chinese Journal of Catalysis 2019年第5期40卷 681-690页

作者： Haoling Ye Yiqiu Liu Si Chen Haiqiang Wang Zhen Liu zhongbiao wu Key Laboratory of Environment Remediation and Ecological Health of Ministry of Education College of Environmental & Resources Sciences ZhejiangUniversity Hangzhou 310058 Zhejiang China Zhejiang Provincial Engineering Research Center of Industrial Boiler & Furnace Flue Gas Pollution Control Hangzhou 310027 Zhejiang China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310007 Zhejiang China

In this study, a hybrid process using non‐thermal plasma (NTP) and photocatalytic oxidation (PCO) was adopted for the degradation of gas‐phase toluene using TiO2 as the photocatalyst. To discover the synergetic effect between NTP and PCO, the performances of both sole (O3, UV, NTP, and PCO) and combined (O3 + TiO2, O3 + UV, NTP + UV, O3 + PCO, and NTP + PCO) processes were investigated from different perspectives, such as the toluene removal efficiency, selectivity of COx, mineralization rate, ozone utilization, and the generation of by‐products. The toluene removal efficiency of the combined NTP + PCO process was 80.2%, which was much higher than that of a sole degradation process such as NTP (18.8%) and PCO (13.4%). The selectivity of CO2 and the ozone utilization efficiency also significantly improved. The amount of by‐products in the gas phase and the carbon‐ based intermediates adsorbed on the catalyst surface dramatically reduced. The improvement in the overall performances of the combined NTP + PCO process was mainly ascribed to the efficient utilization of ozone in the photocatalytic oxidation, and the ozone further acting as an electron acceptor and scavenger, generating more hydroxyl radicals and reducing the recombination of electron‐ hole pairs.

关键词： Non‐thermal plasma Photocatalytic oxidation Synergetic effect Ozone Toluene

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Simulation and Analysis on the Two-Phase Flow Fields in a Rotating-Stream-Tray Absorber by Using Computational Fluid Dynamics

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Chinese Journal of Chemical Engineering 2004年第2期12卷 169-173页

作者：邵雄飞吴忠标 Department of Environmental Engineering Zhejiang University Hangzhou 310027 China

The flow field of gas and liquid in a φ150mm rotating-stream-tray (RST) scrubber is simulated by using computational fluid dynamic (CFD) method. The sismulation is based on the two-equation RNG κ-ε turbulence model, Eulerian multiphase model, and a real-shape 3D model with a huge number of meshes. The simulation results include detailed information about velocity, pressure, volume fraction and so on. Some features of the flow field are obtained: liquid is atomized in a thin annular zone; a high velocity air zone prevents water drops at the bottom from flying towards the wall; the pressure varies sharply at the end of blades and so on. The results will be helpful for structure optimization and engineering design.

关键词： rotating-stream-tray two-phase flow field simulation computational fluid dynamics

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Supercritical water syntheses of transition metal-doped CeO_2 nano-catalysts for selective catalytic reduction of NO by CO:An in situ diffuse reflectance Fourier transform infrared spectroscopy study

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Chinese Journal of Catalysis 2018年第4期39卷 728-735页

作者： Xiaoxia Dai Weiyu Jiang Wanglong Wang Xiaole Weng Yuan Shang Yehui Xue zhongbiao wu Ministry of Education Key Laboratory of Environment Remediation and Ecological Health College of Environmental and Resource and SciencesZhejiang UniversityHangzhou 310058ZhejiangChina Zhejiang Provincial Engineering Research Centre of Industrial Boiler&Furnace Flue Gas Pollution Control Hangzhou 310058ZhejiangChina

In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice,forming solid *** catalysts were then used for the selective catalytic reduction(SCR)of NO by *** Cu‐doped catalyst exhibited the highest SCR activity;it had a T50(i.e.,50%NO conversion)of only 83°C and a T90(i.e.,90%NO conversion)of 126°*** an activity was also higher than in many state‐of‐the‐art *** situ diffuse reflectance Fourier transform infrared spectroscopy suggested that the MOx‐CeO2 catalysts(M=Co and Fe)mainly followed an Eley‐Rideal reaction mechanism for CO‐*** contrast,a Langmuir‐Hinshelwood SCR reaction mechanism occurred in CuO‐CeO2 owing to the presence of Cu+species,which ensured effective adsorption of *** explains why CuO‐CeO2 exhibited the highest activity with regard to the SCR of NO by CO.

关键词： Supercritical water Nitrogen oxides CO Selective catalytic reduction Diffuse reflectance Fourier transform infrared spectroscopy CeO2

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Atmosphere Environment Science and Technology Development

Atmosphere Environment Science and Technology Development

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作者： Yu Xuezeng Zhang Yuanhang Zhu Tong Fan Shaojia wu zhongbiao

Atmosphere environment science and technology discipline is a new branch of science of multidisciplinary crossed. According to the discipline classification standard of our country at present, the report mainly discus...

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Transformation of Flue-Gas-Desulfurization Gypsum to α-Hemihydrated Gypsum in Salt Solution at Atmospheric Pressure

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Chinese Journal of Chemical Engineering 2011年第2期19卷 349-355页

作者：吴晓琴童仕唐官宝红吴忠标 Department of Chemical Engineering Wuhan University of Science and Technology Wuhan 430081 China Department of Environmental Engineering Zhejiang University Hangzhou 310027 China

Direct phase transformation of flue gas desulfurization gypsum in hot salt solution at atmospheric pres-sure was *** effects of temperature,salt species,salt concentration,solids content,pH and modifier were *** crystals obtained under different conditions and solubility of calcium sulfate in contact with solid gypsum were also determined.α-Calcium sulfate hemihydrate crystals of stubby columnar shape and regular pentahedral sides were obtained under the following conditions：salt concentration 20%-30%,operation tempera-ture 95-100 °C,solids mass content in the slurry 10%-30% and neutral *** analysis revealed that phase transformation of calcium sulfate dihydrate to α-calcium sulfate hemihydrate occurs because of the difference in solubilities between the two solid gypsum phases in this system.

关键词： flue gas desulfurization gypsum crystal growth thermogravimetric analysis phase transformation

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吸收协同高级氧化工艺处理低浓度含氰废气实验研究

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环境科学学报 2021年第7期41卷 2617-2623页

作者：张天昱刘越吴忠标浙江大学环境与资源学院杭州310058 浙江省工业锅炉炉窑烟气污染控制工程技术研究中心杭州310058

以乙腈作为含氰废气的典型组分,考察吸收协同不同高级氧化体系下低浓度乙腈的去除效率以及产物分配情况.研究结果表明:UV/PS和VUV/PS体系均能有效吸收并降解乙腈,在60 min内其脱除效率近100%,且矿化率近80%或以上.主要原因是吸收液中的... 详细信息

以乙腈作为含氰废气的典型组分,考察吸收协同不同高级氧化体系下低浓度乙腈的去除效率以及产物分配情况.研究结果表明:UV/PS和VUV/PS体系均能有效吸收并降解乙腈,在60 min内其脱除效率近100%,且矿化率近80%或以上.主要原因是吸收液中的过硫酸盐(PS)可以在紫外光的激发下产生大量的HO^(·)和SO_(4)^(·-),这些自由基可以促进乙腈和中间产物的氧化.同时实验还观察到乙腈中的氮元素主要被转化为NO^(-)_(3)和NH^(+)_(4),这说明乙腈的直接氧化和水解反应同时进行.NO^(-)_(3)的累积会竞争消耗反应体系中的自由基,这是其稳定性实验中乙腈矿化率下降的主要原因.此外,干扰离子Cl^(-)也会由于自由基的捕获作用抑制乙腈的降解.最后,根据产物的分析结果,提出了包含氧化与水解路径的乙腈总体降解反应途径.

关键词：乙腈液相吸收高级氧化过硫酸盐反应路径

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La掺杂BiOI微球可见光下光催化氧化NO性能研究

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物理化学学报 2021年第8期37卷 91-100页

作者：李钱胡静周易王海强吴忠标浙江大学环境技术研究所杭州310058

光催化氧化技术被广泛认为是一种经济有效的治理低浓度NO的技术。三维BiOI微球是一种典型的可见光光催化剂,其光催化氧化NO的性能常受限于快速的光生载流子复合以及较差的导电性。然而,由于BiOI微球的尺寸较大,其与其它半导体或者助催... 详细信息

光催化氧化技术被广泛认为是一种经济有效的治理低浓度NO的技术。三维BiOI微球是一种典型的可见光光催化剂,其光催化氧化NO的性能常受限于快速的光生载流子复合以及较差的导电性。然而,由于BiOI微球的尺寸较大,其与其它半导体或者助催化剂的复合通常不匹配,缺乏足够的接触界面。本文通过简易的一步水热法,首次采用稀土金属La掺杂策略改性BiOI微球,并系统研究了其可见光光催化氧化NO的性能。实验优化调整了La的前驱体以及掺杂量。研究结果发现,同LaCl3和La(AC)_(3)相比,La(NO3)_(3)的效果最佳。0.3%La/BiOI光催化氧化NO的转化率最优(74%),远高于单纯的BiOI微球(44%),且其在连续5次循环实验中也表现出优异的稳定性。理化性质分析发现,La掺杂可促进BiOI结晶,但对其形貌和结构几乎不产生影响。La^(3+)可能会通过取代Bi^(3+)进入BiOI的晶格中,或形成La_(2)O_(3)纳米簇均匀的分散在BIOI微球的介孔中。机理分析进一步发现,La掺杂不仅减小了BiOI的带隙,促进了对太阳光的吸收,而且可引入更多的氧空位,有利于水分子解离,生成更丰富的·OH。这些因素共同提升了BiOI光催化氧化NO的性能。此外,La/BiOI主要将NO氧化成NO_(2),且形成的NO_(2)倾向于从催化剂表面脱附,这不仅保全了催化剂表面的活性位点,NO光催化氧化反应得以持续进行,而且可避免催化剂频繁洗涤再生,因此La/BiOI具有优异的稳定性,且使用寿命长。此外,生成的NO_(2)可轻易彻底地被尾部碱性液体吸收,有效避免了二次污染。本研究表明掺杂是一种有效改善三维BiOI微球光催化性能的改性方法,期待其可为各种应用于光催化反应的三维半导体材料的改性和合理设计提供新颖的思路。

关键词： La BiOI微球 NO转化光催化氧化

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