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Novel Al-doped carbon nanotubes with adsorption and coagulation promotion for organic pollutant removal

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Journal of Environmental Sciences 2017年第4期29卷 1-12页

作者： Dongjuan Kang Xiaolin Yu maofa ge Feng Xiao Hui Xu State Key Laboratory for Structural Chemistry of Unstable and Stable Species Beijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of Sciences

Al-doped carbon nanotubes（Al-doped CNTs） were prepared as a multifunctional integrated material of adsorbent and coagulant aid for organic pollutant removal from aqueous solution. It was observed that aluminum species were dispersed homogeneously on the surface of CNTs, and mainly anchored onto defect structures of the CNTs. The introduction of aluminium efficiently improved adsorption ability for methyl orange（MO） onto the CNTs,and maximum adsorption capacity calculated from the Langmuir isotherm model can reach 69.7 mg/g. The MO adsorption kinetics can be better described by the pseudo-second-order and pore diffusion kinetic models, and the diffusion of MO anions into pores of the Al-doped CNT adsorbent should be the rate-determining *** analyses indicated that the adsorption of MO onto Al-CNTs-2.0 was endothermic and spontaneous. Moreover, adsorption capacity for MO on the Al-doped CNTs was evidently dependent on the CNT dose, solution p H and adsorbent dose. From the perspective of low-cost and multifunctional, suspension obtained during the Al-doped CNT adsorbent preparation, was tested as coagulant to remove humic acid（HA）. A significant observation is that the suspension exhibited an excellent coagulation performance for HA,because abundant aluminous polymer and Al-doped CNTs existed in the suspension.

关键词： Al-doped carbon nanotubes Adsorption Organic pollutants Methyl orange Aqueous solution

Reaction between sulfur dioxide and iron oxide cationic clusters

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Chinese Science Bulletin 2009年第21期54卷 4017-4020页

作者： YIN Shi HE ShengGui ge maofa Beijing National Laboratory for Molecular Sciences (BNLMS) and State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Graduate University of the Chinese Academy of Sciences Beijing 100049 China

The reactivity of sulfur dioxide (SO2) molecules toward iron oxide cationic clusters (FemOn+) is studied by a homemade time-of-flight mass spectrometer coupled with a laser ablation/supersonic expansion cluster source and a fast flow reactor. The association products FemOnSO2+ can be observed for most of the clusters. The interesting result is that the cooperation effect of SO2 and water is in favor of the adsorption of gas phase water on specific scale iron oxide clusters (Fe2O2+ and Fe3O3+ ). The reactivity information obtained may be useful to investigate atmospheric heterogeneous chemistry of related systems.

关键词：二氧化硫反应器离子簇氧化铁飞行时间质谱仪快速流动激光烧蚀协同效应

Kinetic study of the reaction of chlorine atoms with 3-methyl-3-buten-1-ol

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Chinese Science Bulletin 2009年第20期54卷 3808-3812页

作者： WANG Lei ge maofa WANG WeiGang Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

The reaction of a typical unsaturated alcohol,3-methyl-3-buten-1-ol(MBO331),with Cl atoms,was investigated for the first *** reaction was investigated using discharged flow-tube coupled with electron impact mass *** experiments were performed over the temperature range of 248 K―298 K and at pressure of 1 torr in He as the bath *** obtained kinetic data were used to derive the Arrhenius expression:k1 =(3.47 ± 1.21) × 10-11 exp[(599 ± 69)/T] cm3 molecule-1 ***,atmospheric lifetimes of the MBO331 with respect to OH radicals,NO3 radicals and Cl atoms have been calculated and the atmospheric implications are considered briefly.

关键词：反应动力学不饱和醇丁烯-1 氯原子 OH自由基电子轰击质谱动力学数据煤气灶

Anthropogenic Effects on Biogenic Secondary Organic Aerosol Formation

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Advances in Atmospheric Sciences 2021年第7期38卷 1053-1084页

作者： Li XU Lin DU Narcisse T.TSONA maofa ge Environment Research Institute Shandong UniversityQingdao 266237China State Key Laboratory for Structural Chemistry of Unstable and Stable Species Chinese Academy of Sciences Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Anthropogenic emissions alter biogenic secondary organic aerosol(SOA)formation from naturally emitted volatileorganic compounds(BVOCs).We review the major laboratory and field findings with regard to effects of anthropogenicpollutants(NO_(x),anthropogenic aerosols,SO_(2),NH_(3))on biogenic SOA ***_(x) participate in BVOC oxidationthrough changing the radical chemistry and oxidation capacity,leading to a complex SOA composition and yield sensitivitytowards NO_(x) level for different or even specific hydrocarbon *** aerosols act as an importantintermedium for gas-particle partitioning and particle-phase reactions,processes of which are influenced by the particlephase state,acidity,water content and thus associated with biogenic SOA mass ***_(2)modifies biogenic SOAformation mainly through sulfuric acid formation and accompanies new particle formation and acid-catalyzedheterogeneous *** new SO_(2)-involved mechanisms for organosulfate formation have also been ***_(3)/amines,as the most prevalent base species in the atmosphere,influence biogenic SOA composition and modify theoptical properties of *** response of SOA formation behavior to these anthropogenic pollutants varies amongdifferent BVOCs *** on anthropogenic-biogenic interactions in some areas of China that aresimultaneously influenced by anthropogenic and biogenic emissions are *** on this review,somerecommendations are made for a more accurate assessment of controllable biogenic SOA formation and its contribution tothe total SOA *** study also highlights the importance of controlling anthropogenic pollutant emissions witheffective pollutant mitigation policies to reduce regional and global biogenic SOA formation.

关键词： biogenic volatile organic compounds anthropogenic pollutants secondary organic aerosol anthropogenic-biogenic interactions China

Temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust

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Journal of Environmental Sciences 2017年第3期29卷 107-112页

作者： Qifan Liu Yidan Wang Lingyan Wu Bo Jing Shengrui Tong Weigang Wang maofa ge Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeifing 100190China State Key Laboratory of Severe Weather&Key Laboratory of Atmospheric Chemistry of CMA Chinese Academy of Meteorological SciencesBeijing100081China

In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust （ATD） has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy （DRIFTS） experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient （yt） of acrylic acid on ATD decreases from （4.02 ± 0.12） x 10-5 to （1.73 ± 0.05） x 10-5 with a temperature increase from 255 to 315 K. According to the temperature dependence of uptake coefficients, the enthalpy （AHobs） and entropy （ASobs） of uptake processes were determined to be -（9.60± 0.38） KJ/mol and -（121.55 ± 1.33） l.K/mol, respectively. The activation energy for desorption （Edes） was calculated to be （14.57 ± 0.60） KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.

关键词： Heterogeneous uptakeAcrylic acidKnudsen cellUptake coefficients

Kinetic study of the gas-phase reaction of O3 with three unsaturated alcohols

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Journal of Environmental Sciences 2018年第9期30卷 292-299页

作者： Weiran Li Yi Chen Shengrui Tong Yucong Guo Yunhong Zhang maofa ge The Institute of Chemical Physics School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 China State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of SciencesBeijing 100190 China State Key Laboratory for Structural Chemistry of Unstable and Stable Species Peking University Beijing 100871 China University of Chinese Academy of Sciences Beijing 100049 China CAS Research/Education Center for Excellence in Molecular Sciences Beijing 100190 China

Rate constants for the reactions of ozone with 1-octen-3-ol, 1-nonen-3-ol and 1-nonen-4-ol have been determined at 298 ±1 K and atmospheric pressure for the first time. The experiments were performed in a 100-L FEP Teflon film bag using absolute rate method; the rate constants were （1.91 ± 0.19） ×10^-17, （1.89 ± 0.20） × 10^-17, and （0.83 ± 0.08） × 10^-17 cm^3/（***） for 1-octen-3-ol, 1-nonen-3-ol, and 1-nonen-4-ol, respectively. The rate constants have been compared with those of unsaturated alcohols structural homologs, and used to estimate the reaction reactivity. The electronegativity of carbon-carbon double bond was calculated by atomic charges analysis. The calculated results show that the electronic effect of the lone pair electrons of hydroxyl oxygen is the main cause of the difference in rate coefficient. According to the obtained rate constants, the atmospheric lifetimes of studied unsaturated alcohols were also estimated, which indicates that the reaction with ozone is an important loss pathway in the atmosphere, especially in polluted areas.

关键词： Rate constant Ozone Unsaturated alcohols Atmospheric lifetime

Study on the reaction of 3-methyl-2-butenal and 3-methylbutanal with Cl atoms: kinetics and reaction mechanism

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Journal of Environmental Sciences 2022年第6期34卷 25-33页

作者： Bo Shi Weigang Wang Cici Fan Yuchan Zhang Zheng Sun Yanli Zeng maofa ge College of Chemistry and Material Sciences Hebei Normal UniversityShijiazhuang 050024China State Key Laboratory for Structural Chemistry of Unstable and Stable Species Beijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of SciencesBeijing 100190China Lanfang Normal University Langfang 065000China National Demonstration Center for Experiment Chemistry Hebei Normal UniversityShijiazhuang 050024China Key Laboratory of Inorganic Nano-material of Hebei Province Shijiazhuang 050024China

The reaction of Cl atoms with two C5aldehydes(3-methyl-2-butenal and 3-methylbutanal)were investigated by proton-transfer-reaction mass spectrum(PTR-MS)using smog chamber at 298±1 K and 760 Torr.A relative rate method was used to determine the rate constants of the title reactions with m-xylene and trans-2-butene as reference compounds:(3.04±0.18)×10^(-10)and(2.07±0.14)×10^(-10)cm^(3)/(molecule·sec)for 3-methyl-2-butenal and 3-methylbutanal,***,the gas-phase products were also identified by PTR-MS,and the possible reaction mechanisms were proposed basing on the identified *** detected gas-phase products are similar for two C5aldehydes reactions,mainly including small molecules of aldehydes,ketones and chlorinated aldehyde *** atmospheric lifetimes(τ)calculated for 3-methyl-2-butenal(τ=7.0 hr,marine boundary layer(MBL))and 3-methylbutanal(τ=10.3 hr,MBL)according to the obtained rate *** results indicate that Cl atoms at MBL are competitive with OH radicals for the degradation contribution of C5aldehyde compounds.

关键词： Smog chamber Kinetic Reaction mechanism Cl atoms

Development and application of the multi-wavelength cavity ring-down aerosol extinction spectrometer

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Journal of Environmental Sciences 2019年第2期31卷 227-237页

作者： Junling Li Weigang Wang Kun Li Wenyu Zhang maofa ge Chao Peng State Key Laboratory for Structural Chemistry of Unstable and Stable Species CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of Sciences University of Chinese Academy of Sciences Air Quality Research Division Environment and Climate Change Canada Center for Excellence in Urban Atmospheric Environment (CEUAE) Institute of Urban EnvironmentChinese Academy of Sciences

To better characterize the optical properties of atmospheric aerosols, the multi-wavelength cavity ring-down aerosol extinction spectrometer(MCRD-AES) is developed and applied in this study. By using tunable light source and four parallel cavities, the MCRD-AES covers a wide and atmospherically relevant wavelength range from 360 to 663 nm. Four wavelengths(375 nm, 440 nm, 532 nm, and 620 nm) are particularly tested with ammonium sulfate and nigrosine. The refractive index values obtained from this study agree well with literature data. The stability and accuracy of the MCRD-AES are tested, and the minimum detectable extinction coefficient is 0.5 1/Mm. The high sensitivity, high precision, and wavelength changeable of MCRD-AES indicate its great application prospect in comprehensively quantifying the optical properties of atmospheric aerosols.

关键词： MCRD-AES Optical property Refractive indices Wavelength dependence

Kinetic and mechanism studies of the ozonolysis of three unsaturated ketones

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Journal of Environmental Sciences 2020年第9期32卷 23-32页

作者： Weiran Li Meifang Chen Yi Chen Shengrui Tong maofa ge Yucong Guo Yunhong Zhang State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China College of Chemistry and Material Science The key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecule-Based MaterialsAnhui Normal UniversityWuhu 241000China CAS Research/Education Center for Excellence in Molecular Sciences Beijing 100190China Institute of Chemical Physics School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

Reaction rate constants and products of 1-octen-3-one,3-octen-2-one and 4-hexen-3-one with ozone were studied in a 100-L fluorinated ethylene propylene(FEP) Teflon film bag using absolute rate method at 298 ± 1 K and atmospheric *** rate constants were(1.09 ± 0.12) × 10-17,(3.48 ± 0.36) × 10-17 and(5.70±0.60) × 10-17 cm3/(molecule·sec),*** to the obtained rate constants,the effects of carbonyl were *** carbonyl group in β position has a net withdrawing effect with respect to an olefinic bond,then causing the decline of rate *** quantum chemical calculation was used to explain the results of rate *** products of ozonolysis were mainly aldehydes,which have significant influence on the formation of SOA,and hence play an important role in the *** this work,we detected the main products of reaction and proposed the reaction mechanism by combining the results of quantum chemical *** lifetime for three unsaturated ketones reacted with ozone was 36.4,11.4 and 6.9 hr for 1-octen-3-one,3-octen-2-one and 4-hexen-3-one,respectively.

关键词： unsaturated ozone mechanism