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In situ FT-IR investigation on the reaction mechanism of visible light photocatalytic NO oxidation with defective g-C_3N_4

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Science Bulletin 2018年第2期63卷 117-125页

作者： Hong wang Wenjie He Xing’an Dong haiqiang wang Fan Dong Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and Resources Chongqing Technology and Business University Department of Environmental Engineering Key Laboratory of Polluted Environment Remediation and Ecological Health of Ministry of Education Zhejiang University

The g-C_3N_4 with different structures was prepared by heat treatment using urea(CN-U) and thiourea(CN-T) as precursors under the same conditions. The microstructure and optical properties of the photocatalyst were analyzed with advanced tools. The results showed that the CN-U has a porous structure, a high specific surface area and a wide band gap in comparison with CN-T. The in situ FT-IR technique was used to monitor the adsorption and reaction process of visible photocatalytic NO oxidation on g-C_3N_4. The corresponding reaction mechanism was proposed based on the results of reaction intermediate observation and electron paramagnetic resonance(EPR) radical scavenging. It was revealed that(1) the presence of defective sites favored the adsorption of gas molecules and electronically compensated it leading to promoted formation of the final products;(2) the high separation efficiency of photogenerated electron-hole pairs enhanced the production of radicals during the photocatalytic reaction;(3) the hydroxyl radicals(-OH) are not selective for the decomposition of pollutants, which are favorable to the complete oxidation of the reaction intermediates. The above three aspects are the main reasons for the CN-U possessing the efficient visible light photocatalytic activity. The present work could provide new insights and methods for understanding the mechanism of photocatalysis.

关键词： g-C3N4 Visible light photocatalysis Defects In situ FT-IR Reaction mechanism

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The numerical simulation of a new double swirl static mixer for gas reactants mixing

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Chinese Journal of Chemical Engineering 2020年第9期28卷 2438-2446页

作者： Zhuokai Zhuang Jingtian Yan Chenglang Sun haiqiang wang Yuejun wang Zhongbiao Wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental&Resources ScienceZhejiang UniversityHangzhou310058China Zhejiang Provincial Engineering Research Centre of Industrial Boiler&Furnace Flue Gas Pollution Control Hangzhou 310058China College of Control Science and Engineering Zhejiang UniversityHangzhou 310027China Zhejiang Tianlan Environmental Protection Technology Co.Ltd Hangzhou 311202China

For the nitrogen oxide removal processes,high performance gas mixer is deeply needed for the injection of NH3 or *** this study,a new type of double swirl static mixer in gas mixing was investigated using computational fluid dynamics(CFD).The results obtained using Particle Image Velocimetry(PIV)correlated well with the results obtained from *** comparisons in pressure loss between the experimental results and the simulation results showed that the model was suitable and accurate for the simulation of the static *** process conditions and design were *** L/D equaled 4,coefficient of variation(COV)was<5%.The inlet velocity did not affect the distributions of turbulent kinetic *** terms of both COV and pressure loss,the inner connector is important in the design of the static *** nozzle length should be set at 4 *** both COV and pressure loss into consideration,the optimal oblique degree is *** averaged kinetic energy changed according to process conditions and *** new static mixer resulted in improved mixing performance in a more compact *** new static mixer is more energy efficient compared with other SV static ***,the double swirl static mixer is promising in gas mixing.

关键词： CFD PIV Gas mixing Double swirl static mixer Pressure loss

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Enhanced CO_2 adsorptive performance of PEI/SBA-15 adsorbent using phosphate ester based surfactants as additives

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Journal of Environmental Sciences 2015年第12期27卷 1-7页

作者： Dandan Cheng Yue Liu haiqiang wang Xiaole Weng Zhongbiao Wu Department of Environmental Engineering Zhejiang University Zhejiang Provincial Engineering Research Center of Industrial Boiler and Furnace Flue Gas Pollution Control

In this study,a series of polyetherimide/SBA-15： 2-D hexagonal P6 mm,Santa Barbara USA（PEI/SBA-15） adsorbents modified by phosphoric ester based surfactants（including tri（2-ethylhexyl）phosphate（TEP）,bis（2-ethylhexyl） phosphate（BEP） and trimethyl phosphonoacetate（TMPA））were prepared for CO2 *** results indicated that the addition of TEP and BEP had positive effects on CO2 adsorption capacity over PEI/*** particular,the CO2 adsorption amount could be improved by around 20% for 45PEI-5TEP/SBA-15 compared to the additive-free *** could be attributed to the decrease of CO2 diffusion resistance in the PEI bulk network due to the interactions between TEP and loaded PEI molecules,which was further confirmed by adsorption kinetics *** addition,it was also found that the cyclic performance of the TEP-modified adsorbent was better than the surfactant-free *** could be due to two main reasons,based on the results of in situ DRIFT and TG-DSC *** and more importantly,adsorbed CO2 species could be desorbed more rapidly over TEP-modified adsorbent during the thermal desorption ***,the enhanced thermal stability after TEP addition ensured lower degradation of amine groups during adsorption/desorption cycles.

关键词： CO2 adsorption Tri(2-ethylhexyl) phosphate PEI/SBA-15 adsorbent Dispersion Surfactant

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Influences of pH value in deposition-precipitation synthesis process on Pt-doped TiO_2 catalysts for photocatalytic oxidation of NO

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Journal of Environmental Sciences 2012年第8期24卷 1519-1524页

作者： Shuzhen Song Zhongyi Sheng Yue Liu haiqiang wang Zhongbiao Wu Department of Environmental Engineering Zhejiang UniversityHangzhou 310058China Guodian Science and Technology Research Institute Nanjing 210031China

This work has been undertaken to study the influences of pH value on the characteristics and activity of photocatalyst by deposition- precipitation method during its preparation process. A series of Pt-modified TiO2 were prepared by deposition-precipitation method at different pH values as well as wet impregnation method, and characterized by XRD, XPS, TEM, UV-Vis and photoluminescence （PL）. It was found that the catalysts had the highest photocatalytic activity for NO conversion when pH value was kept at around 7. And the sample prepared by deposition-precipitation method showed higher activity than that by impregnation method. This was mainly due to their high value in highly-dispersed platinum oxides （PtOx） content on the surface of the catalysts. The results from UV-Vis absorption showed that highest absorbance was obtained for Pt/TiO2 prepared at pH values of around 7. And PL spectra results indicated that the recombination rate of photogenerated electrons and holes of the samples prepared by deposition-precipitation method was lower than that prepared by impregnation method. And in the zeta potential study, the pH values for the isoelectric point of the preparing slurry of 0.05 wt.%Pt/TiO2 and 0.5 wt.%Pt/TiO2 were determined to be 6.5-8.5, which further confirmed the enrichment of PtOx dopants for the catalysts repapered when pH value was around 7.

关键词： pH value ZiO2 PtOx NO photocatalysis zeta potential

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Simultaneous removal of NO and dichloromethane(CH_(2)Cl_(2)) over Nb-loaded cerium nanotubes catalyst

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Journal of Environmental Sciences 2022年第1期34卷 175-184页

作者： Weilong Ouyang Yi Zhou Xiaoqi Fei Yarong Bai haiqiang wang Zhongbiao Wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental and Resources ScienceZhejiang UniversityHangzhou 310058China Zhejiang Provincial Engineering Research Center of Industrial Boiler and Furnace Flue Gas Pollution Control Hangzhou 310058China

Herein,a series of niobium oxide supported cerium nanotubes(Ce NTs)catalysts with different loading amount of Nb_(2)O_(5)(0–10 wt.%)were prepared and used for selective catalytic reduction of NOxwith NH_(3)(NH_(3)-SCR)in the presence of CH_(2)Cl_(2).Commercial V_(2)O_(5)-WO_(3)-TiO_(2) catalyst was also prepared for *** physcial properties and chemical properties of the Nb_(2)O_(5) loaded cerium nanotubes catalysts were investigated by X-ray diffractometer,Transmission electron microscope,Brunauer-Emmett-Teller specific surface area,H_(2)-temperature programmed reduction,NH_(3)-temperature programmed desorption and Xray photoelectron *** experiment results showed that the loading amount of Nb_(2)O_(5) had a significant effect on the catalytic performance of the catalysts.10 wt.%Nb-Ce NTs catalyst presented the best NH_(3)-SCR performance and degradation efficiency of CH_(2)Cl_(2) among the prepared catalysts,due to its superior redox capability,abundant surface oxygen species and acid sites,the interaction between Nb and Ce,higher ratio of Nb^(4+)/(Nb^(5+)+Nb^(4+))and Ce^(3+)/(Ce^(3+)+Ce^(4+)),as well as the special tubular structure of cerium *** study may provide a practical approach for the design and synthesis of SCR catalysts for the simultaneously removal NOxand chlorinated volatile organic compounds(CVOCs)emitted from the stationary industrial sources.

关键词： Cerium nanotubes Niobium oxide Selective catalytic reduction Nitrogen oxides CH_(2)Cl_(2) Simultaneous removal

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Enhanced CH4 selectivity in CO2 photocatalytic reduction over carbon quantum dots decorated and oxygen doping g-C3N4

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Nano Research 2019年第11期12卷 2749-2759页

作者： Qian Li Songcan wang Zhuxing Sun Qijun Tang Yiqiu Liu Lianzhou wang haiqiang wang Zhongbiao Wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental and Resources ScienceZhejiang UniversityHangzhou 310058China Zhejiang Provincial Engineering Research Center of Industrial Boiler and Furnace Flue Gas Pollutin Control Hangzhou 311202China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandBrisbaneQLD 4072Australia Schoo of Envionmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Graphitic carbon nitride(g-C3N4,CN)exhibits inefficient charge separation,deficient CO2 adsorption and activation sites,and sluggish surface reaction kinetics,which have been recognized as the main barriers to its application in CO2 photocatalytic *** this work,carbon quantum dot(CQD)decoration and oxygen atom doping were applied to CN by a facile one-step hydrothermal *** incorporated CQDs not only facilitate charge transfer and separation,but also provide alternative CO2 adsorption and activation ***,the oxygen-atom-doped CN(OCN),in which oxygen doping is accompanied by the formation of nitrogen defects,proves to be a sustainable H^+ provider by facilitating the water dissociation and oxidation *** of the synergistic effect of the hybridized binary CQDs/OCN addressing the three challenging issues of the CN based materials,the performance of CO2 photocatalytic conversion to CH4 over CQDs/OCN-x(x represents the volume ratio of laboratory-used H2O2(30 wt.%)in the mixed solution)is dramatically improved by 11 times at *** hybrid photocatalyst design and mechanism proposed in this work could inspire more rational design and fabrication of effective photocatalysts for CO2 photocatalytic conversion with a high CH4 selectivity.

关键词： photocalytic CO2 reduction graphitic carbon nitride(g-C3N4) carbon quantum dot oxygen doping

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Photocatalytic oxidation of gaseous benzene over nanosized TiO_2 prepared by solvothermal method

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Chinese Science Bulletin 2007年第22期52卷 3061-3067页

作者： WU ZhongBiao GU ZhuoLiang ZHAO WeiRongt wang haiqiang Department of Environmental Engineering Zhejiang University Hangzhou 310027 China

Nanosized TiO2 particles were prepared by solvothermal method using tetrabutyl titanate as precursor,ethanol and water as solvents,and a facile immobilization method of nanosized TiO2 particles on woven glass fabric was developed. The samples obtained under various preparation conditions were charac-terized by means of thermo gravimetric analysis(TG) and differential scanning calorimetry(DSC) ,X-ray diffraction(XRD) ,transmission electron microscopy(TEM) ,high resolution-transmission electron mi-croscopy(HR-TEM) ,and Brunauer-Emmett-Teller(BET) . The results show that the cube-shape of TiO2 prepared by solvothermal method has good crystallinity of(101) surface,higher thermal stability and large specific surface area. Scanning electron microscopy(SEM) images confirmed that the immobi-lized TiO2 film was uniformly distributed and clung to the substrate firmly. The photocatalytic activity of the catalysts was tested using photocatalytic oxidation of gaseous benzene. The results show that the TiO2 calcined after solvothermal treatment suffers from lower specific surface area,and hence de-creases its photocatalytic activity. The photocatalytic activities of the TiO2 by solvothermal treatment with or without calcination in degradation 400 mg/m3 benzene are 3.7 and 4.1 times as high as catalyst without solvothermal treatment,respectively.

关键词：光催化剂气体苯二氧化钛检验方法

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Revisiting miR-155 in intervertebral disc degeneration:Blood cell signature and local cell-free profiles

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BIOCELL 2022年第2期46卷 511-517页

作者： ZHIHENG LIU ZHEN SUN ZHONGYUAN WAN haiqiang wang Department of Cardiac Surgery Xijing HospitalAir Force Medical UniversityXi’an710032China Institute of Integrative Medicine Shaanxi University of Chinese MedicineXi’an712046China Department of Orthopedics Xijing HospitalAir Force Medical UniversityXi’an710032China Department of Orthopedics Seventh Medical Center of General Hospital of PLABeijing100700China

We unraveled the expression profiles of coding-noncoding RNAs in intervertebral disc degeneration(IDD).However,it remains elusive regarding miR-155 expression in peripheral blood mononuclear cells(PBMCs)and local extracellular space in *** study aimed for investigating the miR-155 expression of PBMCs,extracellular miRNAs(ex-miRNAs)of human nucleus pulposus(NP)tissues,and morphological changes of cell death in the IDD ***,we harvested peripheral blood and NP samples from scoliosis and IDD patients as control and degenerative groups,*** standard Ficoll density-gradient centrifugation was used to isolate *** two subpopulations of PBMCs were divided based on the cellular difference in adherence,i.e.,monocytes/macrophages and *** real-time PCR was used to evaluate miR-155 relative expression in ***-miRNAs were screened by comparison between GSE19943,GSE63492,and extracellular RNA(exRNA)*** morphological changes of cell death subtypes in IDD were observed in transmission electron microscopy(TEM).Results indicate that the lower expression of miR-155 in PBMCs from IDD patients ascribed to alterations in monocytes/***,we identified 594 shared hsa-miRNAs as the intracellular miRNA expression profile and 258 miRNAs as the ex-miRNA expression profile in human NP ***-155 was amongst intracellular miRNAs in *** observation presented multiple endocytic secretory vesicles within human NP cells,implicating exosome transporting *** necroptosis and pyroptosis were noted in human ***,this study reveals miR-155 expression in PBMCs from IDD ***,we propose ex-miRNA expression profile and necroptosis/pyroptosis in human NP tissue,shedding novel light on the etiology of IDD.

关键词： miR-155 PBMCs Lumbar disc disease Auto-immunity Cell death Exosome

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Numerical evaluation of the effectiveness of NO_2 and N_2O_5 generation during the NO ozonation process

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Journal of Environmental Sciences 2016年第3期28卷 51-58页

作者： haiqiang wang Zhuokai Zhuang Chenglang Sun Nan Zhao Yue Liu Zhongbiao Wu Department of Environment Engineering Zhejiang University Zhejiang Provincial Engineering Research Center of Industrial Boiler Furnace Flue Gas Pollution Control

Wet scrubbing combined with ozone oxidation has become a promising technology for simultaneous removal of SO_2 and NO_x in exhaust *** this paper,a new 20-species,76-step detailed kinetic mechanism was proposed between O_3 and NO_*** concentration of N_2O_5 was measured using an in-situ IR *** numerical evaluation results kept good pace with both the public experiment results and our experiment *** reaction parameters for the generation of NO_2 and N_2O_5 during the NO ozonation process were investigated by a numerical simulation *** effect of temperature on producing NO_2 was found to be *** produce NO_2,the optimal residence time was1.25 sec and the molar ratio of O_3/NO about *** the generation of N_2O_5,the residence time should be about 8 sec while the temperature of the exhaust gas should be strictly controlled and the molar ratio of O_3/NO about *** study provided detailed investigations on the reaction parameters of ozonation of NO_x by a numerical simulation method,and the results obtained should be helpful for the design and optimization of ozone oxidation combined with the wet flue gas desulfurization methods（WFGD） method for the removal of NO_x.

关键词： Numerical simulation O_3 NO N_2O_5 In-situ IR spectra

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Comparative study of Co_(3)O_(4)-ZSM-5 catalysts synthesized by different hydrothermal methods for the catalytic oxidation of dichloromethane

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Chinese Chemical Letters 2021年第3期32卷 1224-1228页

作者： Xiaoqi Fei Shuang Cao Weilong Ouyang haiqiang wang Zhongbiao Wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental&Resources ScienceZhejiang UniversityHangzhou 310058China Zhejiang Provincial Engineering Research Center of Industrial Boiler&Furnace Flue Gas Pollution Control Hangzhou 310058China Department of Environmental Engineering China Jiliang UniversityHangzhou 310018China

In this work,various Co_(3)O_(4)-ZSM-5 catalysts were prepared by the microwave hydrothermal method(MH-Co_(3)O_(4)@ZSM-5),dynamic hydrothermal method(DH-Co_(3)O_(4)@ZSM-5),and conventio nal hydrothermal method(CH-Co_(3)O_(4)/ZSM-5).Their catalytic oxidation of dichloromethane(DCM)was *** characterizations such as X-ray diffractometer(XRD),scanning microscopy(SEM),X-ray photoelectron spectroscopy(XPS),Brunauer-Emmett-Teller(BET),H2 temperature-programmed reduction(H2-TPR),temperature-programmed desorption of O_(2)(O_(2)-TPD),temperature-programmed desorption of NH_(3)(NH_(3)-TPD),diffuse reflectance infrared Fourier-transform spectra with NH_(3)molecules(NH_(3)-DRIFT),and temperature-programmed surface reaction(TPSR)were *** showed that with the assistance of microwave,MH-Co_(3)O_(4)@ZSM-5 formed a uniform core-shell structure,while the other two samples did ***-Co_(3)O_(4)@ZSM-5 possessed rich surface adsorbed oxygen species,higher ratio of Co^(3+)/Co^(2+),strong acidity,high reducibility,and oxygen mobility among the three Co_(3)O_(4)-ZSM-5 catalysts,which was beneficial for the improvement of DCM *** the oxidation of dichloromethane,MH-Co_(3)O_(4)@ZSM-5 presented the best activity and mineralization,which was consistent with the characterizations ***,according to the TPSR test,HCl or Cl_(2)removal from the catalyst surface was also promoted in MH-Co_(3)O_(4)@ZSM-5 by their abundant Bronsted acid sites and the promotion of Deacon reaction by Co_(3)O_(4)or the synergistic effect of Co_(3)O_(4)and *** to the results of in situ DRIFT studies,a possible reaction pathway of DCM oxidation was proposed over the MH-Co_(3)O_(4)@ZSM-5 catalysts.

关键词： Dichloromethane Catalytic oxidation Co_(3)O_(4) ZSM-5 Core-shell structure Microwave hydrothermal method

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