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Catalytic oxidation of o-chlorophenol over Co2XAI(X=Co,Mg,Ca,Ni)hydrotalcite-derived mixed oxide catalysts

Frontiers of Environmental Science & engineering 2020年第6期14卷 159-169页

作者： Na Li Xin Xing Yonggang Sun Jie Cheng Gang Wang Zhongshen Zhang Zhengping Hao Key Laboratory of Environmental Nanotechnology and Health Effects Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation ***-transition metal oxides(Co2XA10,X=Co,Mg,Ca and Ni)were investigated for the deep catalytic oxidation of o-chlorophenol as a typical heteroatom contaminant containing chlorine *** partial substitution of Co by Mg,Ca or Ni in the mixed oxide can promote the catalytic oxidation of *** Co2MgA10 catalyst presented the best catalytic activity,and could maintain 90%o-chlorophenol conversion at 167.1℃,compared only 27%conversion for the Co3A10 *** results demonstrated that the high activity could be attributed to its increased low-temperature reducibility,rich active oxygen species and excellent oxygen *** the existence of acid and base sites,catalysts with strong basicity also showed preferred *** organic by-products generated during the o-chlorophenol catalytic oxidation over Co2MgAlO catalyst included carbon tetrachloride,trichloroethylene,2,4-dichlorophenol,and 2,6-dichloro-p-benzoquinon,et *** work provides a facile method for the preparation of Co-based composite oxide catalysts,which represent promising candidates for typical chlorinated and oxygenated volatile organic compounds.

关键词： Hydrotalcite-derived mixed oxides o-chlorophenol Catalytic oxidation Organic by-products

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Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

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Journal of Environmental Sciences 2020年第10期32卷 55-63页

作者： Xin Xing Na Li Jie Cheng Yonggang Sun Zhongshen Zhang Xin Zhang Zhengping Hao Key Laboratory of Environmental Nanotechnology and Health Effects Research Center for Eco-Enuironmental SciencesChinese Academy of SciencesBeijing 100085China National Engineering Laboratory/or VOCs Pollution Control Material&Technology Research Center/or Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

In this work, a series of Cu-ZSM-5 catalysts with different SiO2/Al2O3 ratios(25, 50, 100 and200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350 ℃ over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5(25) exhibited the highest selectivity to N2, exceeding 90% at 350 ℃. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N2 selectivity was impacted by the Bronsted acidity and the isolated Cu^2+ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.

关键词： CH3CH2CH2CH2NH2 Selective oxidation Cu-ZSM-5 Cu species Acid sites

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High temperature H_(2)S selective oxidation on a copper-substituted hexaaluminate catalyst: A facile process for treating low concentration acid gas

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Chinese Chemical Letters 2022年第3期33卷 1279-1282页

作者： Xin Xu Ganggang Li Fenglian Zhang Guoxia Jiang Zhengping Hao Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

H_(2)S selective catalytic oxidation technology is a prospective way for the treatment of low concentration acid gas with simple process operation and low investment. However, undesirable results such as large formation of SO_(2) and catalyst deactivation inevitably occur, due to the temperature rise of fixed reaction bed caused by the exothermic reaction. Catalyst with high activity in wide operating temperature window, especially in high temperature range, is urgently needed. In this paper, a series of copper-substituted hexaaluminate catalysts (LaCu_(x), x = 0, 0.5, 1, 1.5, 2, 2.5) were prepared and investigated for the H_(2)S selective oxidation reaction at high temperature conditions (300-550℃). The LaCu_(1) catalyst exhibited excellent catalytic performance and great stability, which was attributed to the best reductive properties and proper pore structure. Besides, two facile deep processing paths were proposed to eliminate the remaining H_(2)S and SO_(2) in the tail gas.

关键词： Low concentration acid gas H_(2)S selective oxidation High temperature Hexaaluminate catalyst

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Decomposition of dioxin-like components in a DBD reactor combined with Hg/Ar electrodeless ultraviolet

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Plasma Science and technology 2020年第3期22卷 34-39页

作者： Weixuan ZHAO Liping LIAN Yanpei WU Yanghaichao LIU Renxi ZHANG Gang LUO Huiqi HOU Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433People’s Republic of China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China

A new combined reactor with Hg/Ar electrodeless ultraviolet(EDUV)activated by DBD for 3,4-dichlorodiphenyl ether abatement is *** effect of specific input energy and feeding gas component on 3,4-dichlorodiphenyl ether removal efficiency has been *** with a single DBD system,this new combined process performed a significant promotion on 3,4-dichlorodiphenyl ether *** results verified that active oxygen clearly contributed to the synergistic activity of DBD-EDUV *** of emission spectra showed that UV radiation of 253.7 nm could be detected in the DBD-EDUV ***,the products of DBD-EDUV process were analyzed via gas chromatographymass spectrometer(GC-MS)to reveal involved decomposition mechanism.

关键词： dielectric barrier discharge(DBD) dioxin-like 3,4-dichlorodiphenyl ether EDUV photolysis

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DBD coupled with MnOx/γ-Al2O3 catalysts for the degradation of chlorobenzene

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Plasma Science and technology 2020年第3期22卷 115-122页

作者： Yanghaichao LIU Liping LIAN Weixuan ZHAO Renxi ZHANG Huiqi HOU Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433People’s Republic of China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China

This paper investigates the degradation of chlorobenzene by dielectric barrier discharge(DBD)coupled with MnOx/γ-Al2O3 ***/γ-Al2O3 catalysts were prepared using the impregnation method and were characterized in detail by N2 adsorption/desorption,x-ray diffraction and x-ray photoelectron *** with the single DBD reactor,the coupled reactor has a better performance on the removal rate of chlorobenzene,the selectivity of COx,and the inhibition of ozone production,especially at low discharge *** degradation rate of chlorobenzene and selectivity of COx can reach 96.3%and 53.0%,respectively,at the specific energy density of 1350 J ***,the ozone concentration produced by the discharge is significantly reduced because the MnOx/Al2O3 catalysts contribute to the decomposition of ozone to form oxygen atoms for the oxidation of *** addition,based on analysis of the byproducts,the decomposition mechanism of chlorobenzene in the coupled reactor is also discussed.

关键词： plasma catalytsis system chlorinated vocs MnOx/Al2O3 catalysts

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Fabricating PdCe/OMS-2 catalysts with boosted low-temperature activity for toluene deep degradation

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Journal of Rare Earths 2023年第6期41卷 839-849,I0002页

作者： Lin Yue Zhihua Xu Minghua Hu Mingjiao Tian Mudi Ma Bijie Huang Chi He State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi'an Jiaotong UniversityXi'an 710049China State Key Laboratory of Precision Blasting and Hubei Key Laboratory of Industrial Fume and Dust Pollution Control Jianghan UniversityWuhan 430056China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China

Porous cryptomelane-type octahedral molecular sieve(OMS-2)with mixed Mn valence and abundant lattice oxygen species has attracted much attention in volatile organic compounds(VOC)catalytic ***,complete conversion of arene over OMS-2 catalysts at relatively low temperature is still a challenge due to its limited crystal structure and inferior ***,a series of PdCe/OMS-2 catalysts with different Pd/Ce molar ratios was fabricated by a facile impregnation method and the physicochemical properties of which were extensively characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),high-resolution transmission electron microscopy(HR-TEM),B runauer-Emmett-Teller(BET)method,X-ray fluorescence(XRF),X-ray photoelectron spectroscopy(XPS),temperature programmed reduction of H2(H2-TPR),Raman,In situ diffused reflectance infrared Fourier transform spectra(DRIFTS),and density functional theory(DFT)*** show that the total conversion of toluene can be achieved at 207℃ over PdCe2 with apparent activation energy as low as 62.6 kJ/*** strong synergistic effect between Pd and Ce remarkably boosts the catalytic activity of OMS-2,attributed to the abundant Mn^(3+)-O bands and active surface oxygen *** results reveal that oxygen vacancy can be formed over PdCe2 much easily than that of Pd/OMS-2 and Ce/OMS-2 with the oxygen vacancy formation energy of2.42,2.83 and 2.68 eV,*** increasing the Pd content cannot promote the catalytic activity although PdO is a critical active center in toluene *** vacancy attributed to the integrative effect of Pd,Ce and Mn species plays a promine nt role over prepared catalysts in toluene activation *** findings reported in this work showed new insights into the designing of highly efficient OMS-2catalysts for VOC deep oxidation by tuning oxygen vacancy concentration.

关键词： PdCe/OMS-2 Toluene Catalytic oxidation Oxygen vacancy Rare earths

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In situ electron-induced reduction of NOx via CNTs activated by DBD at low temperature

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Frontiers of Environmental Science & engineering 2020年第2期14卷 87-96页

作者： Weixuan Zhao Liping Lian Xingpeng Jin Renxi Zhang Gang Luo Huiqi Hou Shanping Chen Ruina Zhang Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049China Shanghai Institute for Design&Research on Environmental Engineering Shanghai 200232China

In this study,a new in situ electron-induced process is presented with carbon nanotubes(CNTs)as a reduction agent activated by dielectric barrier discharge(DBD)for nitrogen oxide(NOx)abatement at low temperature(<407 K).Compared with a single DBD system and a DBD system with activated carbon(DBD-AC),a DBD system with carbon nanotubes(DBD-CNT)showed a significant promotion of NOx removal efficiency and N2 *** the 02 content was 10%,the NOv conversion and N2 selectivity in the DBD-CNT system still reached 64.9%and 81.9%at a specific input energy(SIE)of 1424 J^L,and these values decreased to 16.8%,31.9%and 43.2%,62.3%in the single DBD system and the DBD-AC system,respectively.X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM)were utilized to investigate surface changes in the CNTs after activation by DBD to explore the NO.t reduction abatement mechanism of this new ***,the outlet gas components were also observed via Fourier transform infrared spectroscopy(FTIR)to help reveal the NOr reduction *** results verified that carbon atoms excited by DBD and the structure of CNTs contributed to the synergistic activity of the DBD-CNT *** new deNOx process was accomplished through in situ heterogenetic reduction reactions between the NOx and carbon atoms activated by the plasma on the *** addition,further results indicated that the new deNOv process exhibited acceptable S02 tolerance and water resistance.

关键词： Dielectric barrier discharge NOx abatement In situ electron-induced reduction Carbon nanotubes

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Synergistic effect of oxygen vacancies and edging/corner-connected MnOs structural motifs in multi-dimensional manganese oxides to enhance Ovocs catalytic oxidation

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Chinese Chemical Letters 2023年第12期34卷 291-299页

作者： Yonggang Sun Ganggang Li Jie Cheng Na Li Xin Xing Xin Zhang Zhongshen Zhang State Key Laboratory of High-eficiency Coal Utilization and Green Chemical Engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China National Engineering Laboratory for VOCs pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China College of Resources and Environment University of Chinese Academy of SciencesBejing 101408China

The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese *** work elaborates,at the atomic level,through in-situ experimental and theoretical methods,the synergistic effects of two types of structural defect sites of Vo-e(edge-sharing oxygen)and Vo-c(corner-sharing oxygen)and MnO6 structural motifs of manganese ***-dimensional manganese oxides,namely those with corner-connected MnOs structural motifs and Vo-c structural oxygen defect sites,significantly improved the activation of vinyl *** of enol structure formation,acetate and formate intermediate species,and tautomerism between enol structure and acetaldehyde were detected when oxygen vacancies of manganese oxides were present in combination with corner/edge-connected ***,the activation of chemical bonds and deep catalytic oxidation of vinyl acetate depend on the presence of a redox couple,surface oxygen species,and weakened Mn-O *** provides a valuable notion for investigating and designing catalytic systems and reaction processes for the purpose of emission reduction and the management of environmental contaminants.

关键词： Oxygen vacancies Synergistic effects MnO_(6)structural motifs In-situ technologies Catalytic oxidation

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Experimental observation of fine secular frequency resonance oscillation with a rectilinear ion trap mass spectrometer

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Chinese Journal of Chemical Physics 2024年第6期37卷 792-796,I0042页

作者： Lixin Shan Zuojian Zhang Zhiyang Wei Yongze Gao Zhiyuan Luo Shiyu Cheng Jinian Shu Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of SciencesBeijing 101408China National Engineering Laboratory for VOCs Pollution Control Material&Technology Beijing 101408China

The mass resolution of the ordinary ion trap mass spectrometer derived from the quadrupole mass spectrometer usually ranges from hundreds to *** this study,the fine secular frequency resonance oscillation was observed with a rectilinear ion trap mass *** FWHM of the responding resonance secular frequency of benzene was 0.012 *** corresponding mass resolution was 8600 m/Δm for benzene(m/z=78).The mass spectrometer with secular frequency scanning has a linear response to benzene in the concentration range from 200 ppbv to 10000 *** study shows a new feature of the secular frequency scanning for ion trap mass spectrometers.

关键词： Fine secular frequency Resonance oscillation Mass resolution Rectilinear ion trap mass spectrometer

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High performance lithium oxygen batteries based on a phosphorous-doped holey graphene cathode

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Rare Metals 2022年第12期41卷 4027-4033页

作者： Ying Meng Jia-Kui Zhang Hai-Ying Lu Xiang-Hong Chen Jian-Tie Xu National Engineering Laboratory for VOCs Pollution Control Technology and Equipment Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution ControlSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510640China

The sluggish electrochemical kinetics of cathode is one of the critical issues for the development of high performance lithium oxygen batteries(LOBs).Graphene-based materials have attracted great attentions as advance... 详细信息

关键词： lithium performance kinetics

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