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A review of whole-process control of industrial volatile organic compounds in China

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Journal of Environmental Sciences 2023年第1期123卷 127-139页

作者： Hailin Wang Shumei Sun Lei Nie Zhongshen Zhang Wenpeng Li zhengping hao Beijing Key Laboratory for Urban Atmospheric VOCs Pollution Control and Technology Application Beijing Municipal Research Institute of Environmental ProtectionBeijing 100037China College of Resources Environment and Tourism Capital Normal UniversityBeijing 100048China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

Volatile organic compounds(VOCs)play an important role in the formation of ground-level ozone and secondary organic aerosol(SOA),and they have been key issues in current air pollution prevention and control in China.Considerable attention has been paid to industrial activities due to their large and relatively complex VOCs emissions.The present research aims to provide a comprehensive review on whole-process control of industrial VOCs,which mainly includes source reduction,collection enhancement and end-pipe treatments.Lower VOCs materials including water-borne ones are the keys to source substitution in industries related to coating and solvent usage,leak detection and repair(LDAR)should be regarded as an efficient means of source reduction in refining,petrochemical and other chemical industries.Several types of VOCs collection methods such as gas-collecting hoods,airtight partitions and others are discussed,and airtight collection at negative pressure yields the best collection efficiency.Current end-pipe treatments like UV oxidation,low-temperature plasma,activated carbon adsorption,combustion,biodegradation,and adsorption-combustion are discussed in detail.Finally,several recommendations are made for future advanced treatment and policy development in industrial VOCs emission control.

关键词： Volatile organic compounds Materials substitution Collection enhancement End-pipe treatments

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

Promotional effect of Cu additive for the selective catalytic oxidation of n-butylamine over CeZrO_(x)catalyst

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Chinese Chemical Letters 2022年第6期33卷 3065-3072页

作者： Xin Xing Ting Zhao Jie Cheng Xiaoxiao Duan Wenpeng Li Ganggang Li Zhongshen Zhang zhengping hao 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 Environmental Science and Engineering Taiyuan University of Science and TechnologyTaiyuan 030024China

The catalytic elimination of nitrogen-containing volatile organic compounds(NVOCs)still encounters bottlenecks in NO_(x)formation and low N_(2)selectivity.Here,a series of Cu-promoted Ce-Zr mixed oxide catalysts were synthesized using a simple precipitation approach,and n-butylamine was adopted as the probe pollutant to evaluate their catalytic performance.The Ce Cu_(10%)ZrO_(x)catalyst exhibited the best catalytic activity,with 100%n-butylamine conversion and 90%N_(2)selectivity at 250℃.Concurrently,this sample also displayed good water resistance.A detailed characterization of the catalyst was performed through a series of experimental studies and theoretical calculations.The addition of Cu increased the redox property and promoted the production of oxygen vacancies,all of which were favorable for the greatest nbutylamine selective catalytic oxidation performance.The changes of oxygen vacancies over Ce Cu_(10%)ZrO_(x)in reaction process were studied by in situ Raman spectra.Moreover,in situ diffuse reflectance infrared Fourier transform spectra(DRIFTs)and theoretical calculations were employed to explore the reaction mechanism of n-butylamine selective oxidation.The high activity and selectivity of this catalyst confirm the practical feasibility of the selective oxidation of n-butylamine to CO_(2)and N_(2),and the exploration of the reaction mechanism provides new insights into the further design of catalysts.

关键词： N-Butylamine CeCu_(a)ZrO_(x)mixed oxide Selective oxidation Oxygen vacancies Reaction mechanism

Study of DDT and its derivatives DDD, DDE adsorption and degradation over Fe-SBA-15 at low temperature

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Journal of Environmental Sciences 2012年第3期24卷 536-540页

作者： Hailin Wang Hua Tian zhengping hao Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China Institute of Physics and Chemistry Chinese Academy of SciencesBeijing 100190China

Mesoporous SBA-15 with different Fe2O3 loading were synthesized by an in-situ coating progress for removals of dichlorodiphenyl- trichloroethane （DDT） and its derivatives, i.e., 1,1-dichloro-2,2-bis-（p-chlorophenyl）ethane （DDD） and 1,1-dichloro-2,2-bis-（4-chloro -phenyl） ethane （DDE）. The results from XRD （X-ray diffractometer）, TEM （transmission electron microscopy） indicated that the iron could be well dispersed on SBA-15 within 6 wt.% Fe2O3 loading. Nitrogen adsorption-desorption tests indicated that the synthesized materials were characterized by ordered meso-structure, high surface area and large pore volume. DDTs were removed from aqueous media in 12-hr treatment and high removal efficiency of DDTs was achieved at over 94%. DDTs could be completely degraded at 350°C under the existence of SBA-15 with 4 wt.% Fe2O3 loading. The final degradation products of DDT were dichlorobenzophenone （DCB） and bis-（4-chloro-phenyl） methane （DDM）, suggesting a complete dechlorination from trichloromethyl.

关键词： DDTs SBA-15 iron adsorption catalytic dechlorination

Novel Co-Mg-Al-Ti-O catalyst derived from hydrotalcite-like compound for NO storage/decomposition

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Journal of Environmental Sciences 2012年第3期24卷 488-493页

作者： Jie Cheng Xiaoping Wang Chunyan Ma zhengping hao Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China

Catalysts of Co1.5Mg1.5/Al0.9Ti0.1O and Co1.5Mg1.5/AlO were successfully prepared by calcinations of corresponding hydrotalcite-like compounds at 800°C for 4 hr. The derived oxides were of spinel phase and a small quantity of Ti substitution did not change the crystal purity. Their catalytic performance for the NO storage/decomposition was investigated. Ti incorporation enhanced the NO decomposition activity while has an opposite effect on the storage capacity of catalyst. In situ FT-IR spectra of the catalysts showed that the final adsorption species on the catalysts was coordinated nitrates/nitrites. In addition, NO storage/decomposition mechanism has been discussed on the basis of these observations.

关键词： NO decomposition storage hydrotalcite-like compounds

Effects of metal and acidic sites on the reaction by-products of butyl acetate oxidation over palladium-based catalysts

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Journal of Environmental Sciences 2014年第3期26卷 702-707页

作者： Lin Yue Chi He zhengping hao Shunbing Wang Hailin Wang Department of Environmental Nano-materials Research Center for Eco-Environmental SciencesChinese Academy of Sciences The Administrative Center for China's Agenda 21 National Urban Environmental Pollution Control Engineering Techniques Research Center Beijing Municipal Research Institute of Environmental Protection

Catalytic oxidation is widely used in pollution control technology to remove volatile organic compounds. In this study, Pd/ZSM-5 catalysts with different Pd contents and acidic sites were prepared via the impregnation method. All the catalysts were characterized by means of N2 adsorption- desorption, X-ray fluorescence （XRF）, HE temperature programmed reduction （H2-TPR）, and NH3 temperature programmed desorption （NH3-TPD）. Their catalytic performance was investigated in the oxidation of butyl acetate experiments. The by-products of the reaction were collected in thermal desorption tubes and identified by gas chromatography/mass spectrometry. It was found that the increase of Pd content slightly changed the catalytic activity of butyl acetate oxidation according to the yield of CO2 achieved at 90%, but decreased the cracking by-products, whereas the enhancement of strong acidity over Pd-based catalysts enriched the by-product species. The butyl acetate oxidation process involves a series of reaction steps including protolysis, dehydrogenation, dehydration, cracking, and isomerization. Generally, butyl acetate was cracked to acetic acid and 2- methylpropene and the latter was an intermediate of the other by-products, and the oxidation routes of typical by-products were proposed. Trace amounts of 3-methylpentane, hexane, 2-methylpentane, pentane, and 2-methylbutane originated from iso4merization and protolysis reactions.

关键词： catalytic oxidation butyl acetate reaction by-product Pd/ZSM-5 VOCs

Layered sphere-shaped TiO_2 capped with gold nanoparticles on structural defects and their catalysis of formaldehyde oxidation

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Journal of Environmental Sciences 2016年第1期28卷 77-85页

作者： Chunyan Ma Guanglong Pang Guangzhi He Yang Li Chi He zhengping hao Department of Environmental Nano-materials Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Department of Environmental Science and Engineering State Key Laboratory of Multiphase Flow in Power EngineeringSchool of Energy and Power Engineering Xi'an Jiaotong University

We describe here a one-step method for the synthesis of Au/TiO2 nanosphere materials,which were formed by layered deposition of multiple anatase TiO2 nanosheets.The Au nanoparticles were stabilized by structural defects in each TiO2 nanosheet,including crystal steps and edges,thereby fixing the Au-TiO2 perimeter interface.Reactant transfer occurred along the gaps between these TiO2 nanosheet layers and in contact with catalytically active sites at the Au-TiO2 interface.The doped Au induced the formation of oxygen vacancies in the Au-TiO2 interface.Such vacancies are essential for generating active oxygen species（-＊O^-） on the TiO2 surface and Ti^3＋ ions in bulk TiO2.These ions can then form Ti^3＋-O^--Ti^4＋species,which are known to enhance the catalytic activity of formaldehyde（HCHO） oxidation.These studies on structural and oxygen vacancy defects in Au/TiO2 samples provide a theoretical foundation for the catalytic mechanism of HCHO oxidation on oxide-supported Au materials.

关键词： Layered Au/TiO2 nanospheres Structural defects Oxygen vacancy defects Reaction mechanism Formaldehyde oxidation

Adsorption of benzene, cyclohexane and hexane on ordered mesoporous carbon

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Journal of Environmental Sciences 2015年第4期27卷 65-73页

作者： Gang Wang Baojuan Dou Zhongshen Zhang Junhui Wang Haier Liu zhengping hao Research Center for Eco-Environmental Sciences Chinese Academy of Sciences School of Materials Science and Engineering University of Science and Technology Beijing

Ordered mesoporous carbon（OMC） with high specific surface area and large pore volume was synthesized and tested for use as an adsorbent for volatile organic compound（VOC）disposal. Benzene, cyclohexane and hexane were selected as typical adsorbates due to their different molecular sizes and extensive utilization in industrial processes. In spite of their structural differences, high adsorption amounts were achieved for all three adsorbates, as the pore size of OMC is large enough for the access of these VOCs. In addition, the unusual bimodal-like pore size distribution gives the adsorbates a higher diffusion rate compared with conventional adsorbents such as activated carbon and carbon molecular sieve. Kinetic analysis suggests that the adsorption barriers mainly originated from the difficulty of VOC vapor molecules entering the pore channels of adsorbents. Therefore, its superior adsorption ability toward VOCs, together with a high diffusion rate, makes the ordered mesoporous carbon a promising potential adsorbent for VOC disposal.

关键词： Volatile organic compounds Adsorption Ordered mesoporous carbon Isosteric heat of adsorption Knudsen diffusion

Removal of cobalt(II) ion from aqueous solution by chitosan–montmorillonite

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Journal of Environmental Sciences 2014年第9期26卷 1879-1884页

作者： Hailin Wang haoqing Tang Zhaotie Liu Xin Zhang zhengping hao Zhongwen Liu Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Key Laboratory of Applied Surface and Colloid Chemistry Shanxi Normal University School of Chemistry & Chemical Engineering Shanxi Normal University

Montmorillonite （MMT） modified with chitosan （CTS, molecular weight = S x 104） was applied to remove heavy metal cations by using Co2＋ as a model ion. An increase in MMT interlayer distance observed from X-ray diffraction indicates the intercalation of CTS into MMT. Together with the results of scanning electron microscopy and Fourier transform infrared spectroscopy, it was concluded that the composite material of CTS and MMT （CTS-- MMT） was prepared successfully. The mass ratio of CTS to MMT had a strong influence on the adsorption performance of CTS-MMT. The highest adsorption value of 150 mg/g was obtained over the composite material with CTS to MMT mass ratio of 0.25, which is much higher than those reported in other studies. The adsorption isotherms and kinetic results indicated that Co2＋ was adsorbed over CTS-MMT in a multilayer model, and the chemical sorption of Co2＋ was determined to be the rate-limiting step.

关键词： Chitosan Montmorillonite Co2＋Isotherm Kinetics