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Effect of Al2O3 doping on the structure and performance of an Al2O3/Fe2O3 catalyst for mercury oxidation

Journal of Environmental Sciences 2020年第4期32卷 138-145页

作者： Ruihui Liu Tingyu Zhu Li Tong Wenqing Xu School of Resources and Civil Engineering Northeastern UniversityShenyang 110819China Research Center for Process Pollution Control National Engineering Laboratory for Hydrometallurgical Cleaner Production TechnologyInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdao 066004China Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province Qinhuangdao 066004China Department of Air Pollution Control Beijing Municipal Institute of Labor ProtectionBeijing 100054China

In this study,the thermal stability of a Fe2 O3 catalyst for mercury oxidation was significantly improved by doping with Al2 *** 1 hr,the catalyst doped with 10 wt.%Al2 O3 still exhibited a mercury conversion efficiency of 70.9%,while the undoped sample even lost its catalytic *** with Al2 O3 retarded the collapse of the catalyst mesoporous structure during high-temperature calcination,and the doped samples maintained a higher specific surface area,smaller pore size,and narrower pore size *** electron microscope images revealed that after calcination at 350℃,the average size of the catalyst grains in Fe2 O3 was 23.4 nm;however,the corresponding values for 1%Al2 O3/Fe2 O3,3%Al2 O3/Fe2 O3,and 10%Al2 O3/Fe2 O3 were only 13.3,7.1,and 4.7 nm,*** obtained from X-ray diffraction and thermogravimetry coupled with differential scanning calorimetry confirmed that doping with Al2 O3 also retards the crystallization of the catalysts at high temperature,constraining catalyst grains to a smaller size.

关键词： Mercury Catalytic oxidation Fe2O3 Al2O3 Thermal stability

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One-pot scalable in situ growth of highly corrosion-resistant MgAl-LDH/MBT composite coating on magnesium alloy under mild conditions

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Journal of materials Science & technology 2021年第33期92卷 225-235页

作者： Ting Hu Yuejun Ouyang Zhi-Hui Xie Liang Wu Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China Hunan Engineering Laboratory for Preparation Technology of Polyvinyl Alcohol(PVA)Fiber Material Huaihua UniversityHuaihua 418000China College of Materials Science and Engineering/National Engineering Research Center for Magnesium Alloys Chongqing UniversityChongqing 400044China

Current corrosion-resistant layered double hydroxide(LDH)coating on Mg alloy is usually in situ grown in autoclave by hydrothermal methods under high temperature and high-pressure conditions,which is unfavorable for industrial *** report that an inhibitor(2-mercaptobenzothiazole,MBT)incorporated composite(Mg Al-LDH/MBT)coating can be in situ deposited on bare AZ31 Mg alloy surface with the assistance of a chelating agent(ethylenediaminetetraacetic acid)under a relatively low temperature(95℃)and ambient pressure by a one-pot *** successful formation of LDH/MBT composite coating is confirmed by a series of characterizations,such as X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),and energy dispersive spectroscopy(EDS).The corrosion resistance of the composite coating is evaluated by means of hydrogen evolution measurement,electrochemical impedance spectroscopy(EIS),Tafel polarization curves,and neutral salt spray *** tests show that the LDH/MBT composite coating has a very low corrosion current density(1.7310^(-8)A cm^(-2)),an extremely high charge transfer resistance(2.336 M cm^(2)),and does not show any corrosion pits even after 15 d of exposure to a Na Cl solution or 7 d of exposure to salt fog environment,manifesting the good and robust corrosion ***,the deposition and corrosion protection mechanisms of the Mg Al-LDH/MBT composite coating are also discussed and proposed based on the EDS characterization of the coating after long-time exposure.

关键词： Magnesium alloy Coating Corrosion resistance Layered double hydroxide

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Distinct roles of pH and organic ligands in the dissolution of goethite by cysteine

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Journal of Environmental Sciences 2022年第3期34卷 260-268页

作者： Ji Li Chenlu Shi Wenbin Zeng Yaru Wang Zebin Hong Yibing Ma Liping Fang Faculty of Material Sciences and Chemistry China University of GeosciencesWuhan 430074China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangzhou 520650China Macao Environmental Research Institute Macao University of Science and TechnologyTaipa 999078MachaoChina

Electron shuttles such cysteine play an important role in Fe cycle and its availability in soils,while the roles of pH and organic ligands in this process are poorly ***,the reductive dissolution process of goethite by cysteine were explored in the presence of organic *** results showed that cysteine exhibited a strong reactivity towards goethite-a typical iron minerals in paddy soils with a rate constant ranging from 0.01 to0.1 hr^(-1).However,a large portion of Fe(Ⅱ) appeared to be "structural species" retained on the *** decline of pH was favorable to generate more Fe(Ⅱ) ions and enhancing tendency of Fe(Ⅱ) release to *** decline of generation of Fe(Ⅱ) by increasing pH was likely to be caused by a lower redox potential and the nature of cysteine pH-dependent adsorption towards ***,the co-existence of oxalate and citrate ligands also enhanced the rate constant of Fe(Ⅱ) release from 0.09 to 0.15 hr-1;nevertheless,they negligibly affected the overall generation of Fe(Ⅱ) in opposition to the pH *** spectroscopic evidence demonstrated that two molecules of cysteine could form disulfide bonds(S-S) to generate cystine through oxidative dehydration,and subsequently,inducing electron transfer from cysteine to the structural Fe(Ⅲ) on goethite;meanwhile,those organic ligands act as Fe(Ⅱ) "strippers".The findings of this work provide new insights into the understanding of the different roles of pH and organic ligands on the generation and release of Fe induced by electron shuttles in soils.

关键词： Electron transfer Reductive dissolution Iron cycling Organic ligands

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Surfactant-assisted removal of 2,4-dichlorophenol from soil by zero-valent Fe/Cu activated persulfate

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Chinese Journal of Chemical engineering 2022年第4期35卷 447-455页

作者： Ling Xu Ji Li Wenbin Zeng Kai Liu Yibing Ma Liping Fang Chenlu Shi Faculty of Material Science and Chemistry China University of GeosciencesWuhan 430074China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangzhou 510650China Macao Environmental Research Institute Macao University of Science and TechnologyTaipaMacaoChina

The organic compounds contaminated soil substantially threatens the growth of plants and food *** this study,we synthesis zero-valent bimetallic Fe/Cu catalysts for the degradation of 2,4-dichlorophenol(DCP)in soils with persulfate(PS)in combination of organic surfactants and exploring the main environmental impact *** kinetic experiments show that the 5%(mass)dosage of Fe/Cu exhibits a higher degradation efficiency(86%)of DCP in soils,and the degradation efficiency of DCP increases with the increase of the initial PS *** conditions are favorable for the DCP degradation in *** importantly,the addition of Tween-80,and Triton-100 can obviously desorb DCP from the soil surface,which enhances the degradation efficiency of DCP in soils by Fe/Cu and PS reaction ***,the Quenching experiments demonstrate that SO_(4)^(-1)·and·OH are the predominant radicals for the degradation of DCP during the Fe/Cu and PS reaction system as well as non-radical also *** findings of this work provide an effective method for remediating DCP from soils.

关键词： Zero-valent iron and copper Advanced oxidation process Persulfate Chlorinated organic pollutants Surfactant

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Dual-Atom Cu2/N-Doped Carbon Catalyst for Electroreduction of Co2 to C2h4

SSRN

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SSRN 2022年

作者： Sun, Guodong Cao, Yanan Hu, Mingzhen Liang, Xinhu Wang, Zhe Cai, Zengjian Shen, Fengyi Zhou, Kebin School of Chemical Sciences China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing100049 China

CO2 can be reduced to C1 products over single-atom electrocatalysts but hardly achieve C-C coupling, which is a crucial step to producing multi-carbon products. In this work, we developed a dual-atom catalyst (Cu2/NC) with a Cu-Cu bond distributed over a nitrogen-doped carbon support, possessing a unique catalytic site for CO2 electroreduction. The Cu2/NC catalyst can efficiently reduce CO2 to C2H4 with a Faradaic efficiency of ~34.9% and a current density of more than 33.6 mA·cm-2. In contrast, Cu single-atom catalysts exhibit significantly different selectivity of CO2 reduction reactions (CO2RR), mainly generating C1 products. According to theoretical calculations, the existence of the Cu-Cu bond enhances the adsorption of *CO and reduces the energy barrier of C-C coupling. Our work is expected to open up new opportunities to develop highly efficient electrocatalysts for making multi-carbon products. © 2022, The Authors. All rights reserved.

关键词： Carbon dioxide

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Pyrrolic N-Doped Carbon Catalysts for Electrocatalytic Reduction of Co2 to Co with 100% Selectivity Over a Wide Potential Window

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SSRN 2023年

作者： Sun, Guo-Dong Cao, Ya-Nan Hu, Ming-Zhen Liang, Xin-Hu Wang, Zhe Cai, Zeng-Jian Shen, Feng-Yi He, Hua Wang, Zhi-Xiang Zhou, Ke-Bin School of Chemical Sciences China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing100049 China

The electrocatalytic reduction of CO2 to CO is an attractive approach for converting the greenhouse gas to value-added chemicals. However, current catalysts still suffer from low catalytic reactivity and low CO selectivity. Here, we report the synthesis of a series of N-doped carbon catalysts by thermal annealing of the mixture of urea and carbon in argon under varied temperatures, enabling the rational modulation of N species in carbon. The as-prepared NC-650 catalyst with pyrrolic N as the dominant N species can preferentially reduce CO2 to CO with almost 100% CO selectivity over a broad potential range (−0.45 to −1.05 V), coupled with remarkable long-term stability for over 300 hours. DFT calculations reveal that the pyrrolic N site is unsaturated, which favors the formation of the N-COOH unit geometrically and electronically via proton-coupled electron transfer while inhibit hydrogen liberation, resulting in high CO2RR reactivity and CO selectivity of the NC-650 catalyst. © 2023, The Authors. All rights reserved.

关键词： Carbon dioxide

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Improving hole transfer of boron nitride quantum dots modified PDI for efficient photodegradation

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Frontiers of Chemical Science and engineering 2023年第11期17卷 1718-1727页

作者： Shiqing Ma Chundong Peng Zeyu Jia Yanmei Feng Kai Chen Hao Ding Daimei Chen Zhong-Yong Yuan Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid WastesNational Laboratory of Mineral MaterialsSchool of Material Sciences and TechnologyChina University of GeosciencesBeijing 100083China School of Materials Science and Engineering Nankai UniversityTianjin 300350China Collaborative Innovation Center of Atmospheric Environment and Equipment Technology Jiangsu Key Laboratory of Atmospheric Environment Monitoringand Pollution Control School of Environmental Science and EngineeringNanjing University of Information Science and TechnologyNanjing 210044China

In recent years,organic photocatalyst under visible-light absorption has shown significant potential for solving environmental ***,it is still a great challenge for constructing a highly active organic photocatalyst due to the low separation efficiency of photogenerated ***,an effective and robust photocatalyst perylene-3,4,9,10-tetracarboxylic diamide/boron nitride quantum dots(PDI/BNQDs),consisting of selfassemble PDI withπ–πstacking structure and BNQDs,has been constructed and researched under visible light *** PDI/BNQDs composite gradually increases organic pollutant photodegradation with the loading amount of *** 10 mL of BNQDs solution added(PDI/BNQDs-10),the organic pollutant photodegradation performance reaches a maximum,about 6.16 times higher with methylene blue and 1.68 times higher with ciprofloxacin than that of pure PDI *** enhancement is attributed to improved separation of photogenerated carriers from self-assembled PDI by BNQDs due to their preeminent ability to extract *** work is significant for the supplement of PDI supramolecular composite *** believe that this photocatalytic design is capable of expanding organic semiconductors’potential for their applications in photocatalysis.

关键词： PDI boron nitride quantum dots photocatalysis hole transfer

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Effect of Mg modification on the catalytic performance of Co/γ-Al 2 O 3 -TiO 2 in the combustion of propane

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Journal of Fuel Chemistry and technology 2020年第7期48卷 867-874页

作者： Zhao LIU Li-jun CHENG Xin HU Shan-liang YUAN Qi-fei BO Biao ZHANG Yi JIANG National Engineering Laboratory for VOCs Pollution Control Material & Technology (Chengdu) Chengdu Institute of Organic Chemistry Chinese Academy of Sciences Chengdu 610041 China University of the Chinese Academy of Sciences Beijing 100049 China

A series of Mg-modified Co/MgO/γ-Al 2 O 3 -TiO 2 catalysts were prepared by multi-step impregnation method and characterized by X-ray diffraction (XRD), diffuse reflectance visible ultra violet spectroscopy (DR-UV-vis), N 2 adsorption-desorption, X-ray photoelectron spectroscopy (XPS) and H 2 temperature-programmed reduction (H 2 -TPR); the effect of Mg modification on the catalytic performance of Co/MgO/γ-Al 2 O 3 -TiO 2 in the combustion of propane was investigated. The results indicate that Co exists in the form of Co 3 O 4 on both the pristine γ-Al 2 O 3 -TiO 2 and Mg-modified MgO/γ-Al 2 O 3 -TiO 2 supports; Mg added in the MgO/γ-Al 2 O 3 -TiO 2 support interacts with Al 2 O 3 , forming MgAl 2 O 4 spinel, which can improve the textural properties and promote the dispersion of Co 3 O 4 . Moreover, the interaction between MgAl 2 O 4 and Co 3 O 4 can increase the proportions of Co 3+ /Co 2+ and O ads /O latt on the catalyst surface, weaken the Co–O bond, and thereby enhance the activity of Co-based catalyst in propane combustion. For the propane combustion over the Co/MgO(15%)/γ-Al 2 O 3 -TiO 2 catalyst with an Mg loading of 15%, the temperature to achieve a propane conversion of 90% is decreased by 45°C in comparison with that over the Mg-free Co/γ-Al 2 O 3 -TiO 2 catalyst; moreover, the Co/MgO(15%)/γ-Al 2 O 3 -TiO 2 catalyst exhibits excellent stability and no decrease in the activity is observed in a 40 h continuous reaction test for propane combustion.

关键词： Co 3 O 4 MgAl 2 O 4 spinel catalytic combustion propane interaction

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A Comprehensive Emission Inventory of Hazardous Air Pollutants from Municipal Solid Waste Incineration in China's Megacity, Beijing Based on the Field Measurements

SSRN

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SSRN 2024年

作者： Yan, Xiao Song, Guangwu Liu, Jiye Liu, Xiao Wang, Hailin Hao, Zhengping National Engineering Research Center of Urban Environmental Pollution Control Beijing Municipal Research Institute of Eco-Environmental Protection Beijing100037 China National Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing101408 China

The increase in pollutant emissions poses a significant challenge to improving air quality in China's megacities, largely attributed to the rising volume of municipal solid waste incineration (MSWI). This study focuses on Beijing and establishes a comprehensive historical emission inventory of hazardous air pollutants (HAPs) emitted from MSWI plants between 2004 and 2023. The inventory integrates detailed plant-level activity data and localized emission factors (EF) derived from field measurements, including data from continuous emissions monitoring systems (CEMS) and manual monitoring. Analysis of CEMS data reveals high compliance rates with emission limits for MSW in Beijing, with 99.9%, 99.5%, 99.8%, 98.7%, and 99.5% of units meeting standards for PM, SO2, NOx, CO and HC, respectively. This suggests effective implementation of emission standards in Beijing, though further strengthening of policies, particularly for CO emissions, is warranted. Overall, total HAP emissions have increased annually largely attributed to measures implemented for DeSOx, DeNOx, and DePM in the power industry since 1998. Most MSWI facilities are located in suburban areas rather than urban cores. Emissions of SO2, HCl, Hg, Cd+Ti, other metals, dioxins, vocs, and NH3 exhibit a spatially homogeneous distribution at the district level, while PM and CO emissions demonstrate heterogeneity. Scenario analysis underscores the importance of continuous improvement and upgrading of advanced air pollution control devices. This study contributes a methodological framework for estimating emissions, reducing uncertainties, and informing policy-making to mitigate HAPs emissions in megacities. It serves as a valuable reference for similar cities grappling with air quality challenges. © 2024, The Authors. All rights reserved.

关键词： Air quality

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Enhancing catalytic toluene oxidation over MnO2@Co3O4 by constructing a coupled interface

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Chinese Journal of Catalysis 2020年第12期41卷 1873-1883页

作者： Quanming Ren Shengpeng Mo Jie Fan Zhentao Feng Mingyuan Zhang Peirong Chen Jiajian Gao Mingli Fu Limin Chen Junliang Wu Daiqi Ye School of Environment and Energy South China University of TechnologyGuangzhou 510006GuangdongChina National Engineering Laboratory for VOCs Pollution Control Technology and Equipment South China University of TechnologyGuangzhou 510006GuangdongChina Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control Guangdong Provincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency DisposalSouth China University of TechnologyGuangzhou 510006GuangdongChina School of Chemical and Biomedical Engineering Nanyang Technological University62 Nanyang DriveSingapore 637459Singapore

Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@*** synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic *** resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,*** activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-*** catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and *** addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene ***,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.

关键词： MnO2@Co3O4 Toluene oxidation Synergistic effect Coupled interface In situ DRIFTS

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