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Effects of surface fluoride modification on TiO_(2)for the photocatalytic oxidation of toluene

Journal of environmental Sciences 2025年第1期147卷 561-570页

作者： Shaoyu Yuan Min Chen Xiaoxiao Qin Xueyan Chen Jianghao Zhang Changbin Zhang State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

In the present study,we investigated the influence of surface fluorine(F)on TiO_(2)for the photocatalytic oxidation(PCO)of ***_(2)modified with different F content was prepared and *** was found that with the increasing of F content,the toluene conversion rate first increased and then ***,CO_(2)mineralization efficiency showed the opposite *** on the characterizations,we revealed that F substitutes the surface hydroxyl of TiO_(2)to form the structure of≡*** presence of the appropriate amount of surface≡Ti-F on TiO_(2)greatly enhanced the separation of photogenerated carriers,which facilitated the generation of·OH and promoted the activity for the PCO of *** was further revealed that the increase of only·OH promoted the conversion of toluene to ring-containing intermediates,causing the accumulation of intermediates and then conversely inhibited the·OH generation,which led to the decrease of the CO_(2)mineralization *** above results could provide guidance for the rational design of photocatalysts for toluene oxidation.

关键词： Photocatalysis TiO_(2) Toluene Fluorine

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Applying heteroatom co-doped carbon nanotube for manifesting high performance in the electrochemical reduction of aqueous nitrogen oxide by gold nanoparticles

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Nano Research 2024年第3期17卷 1151-1164页

作者： Jane Chung Haibo Yin Rong Wang Yunlong Wang Junyang Zhang Yue Peng Joung Woo Han Seongyun Ryu Junhua Li State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China EHS Research Center Samsung Electronics Co.Ltd.Gyeonggi-do 18448Republic of Korea

Electrochemical NO-to-NH_(3) under ambient conditions could be a viable alternative having advantages in terms of energy consumption and exhaust gas recycling of NO,replacing a traditional ammonia synthesis method of the Haber–Bosch *** synthesizing boron(B-)and nitrogen(N-)co-doped carbon nanotube(CNT)based gold(Au)catalysts,B-dopants elevate the conductivity of carbon nanotube by sp2 hybridization on graphene and implant B–N domains within the graphene layer,and result in facilitating the embedding amount of Au accompanied by high dispersibility with low particle *** density functional theory(DFT)calculations elucidate that the electron cloud transmitted from B-dopant to the active site of Au induces the Lewis acidic site,and the O-distal pathway occurs following a spontaneous *** of the electron-deficient B-doping area accompanied by N-defects and B–O edges retains the major valence state of Au as Au^(δ+),and suppresses hydrogen evolution reaction(HER)by repulsing the hindrance of H*.This record exhibits the highest faradaic efficiency(FE)of 94.7%,and NH_(3) yield rate of 1877.4μg·h^(-1)·mg_(cat)^(-1),which is the optimal yield over energy consumption in the field of the ambient reduction of aqueous NO.

关键词： boron heteroatom nitrogen defect gold nanoparticles valence states of gold electrochemical NO-to-NH3

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Promotional effect of stannum on Pd/CeO_(2)catalysts for CO and C_(3)H_(6)co-oxidation

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Journal of Rare Earths 2025年第3期43卷 508-515,I0003页

作者： Congwei Liu Jie Li Meng Wang Jieying Cai Miaomiao Liu Yulong Shan Yan Zhang Wenpo Shan Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academyof SciencesXiamen361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationInstitute of Urban EnvironmentChinese Academy of SciencesNingbo315800China University of Chinese Academy of Sciences Beijing100049China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academyof SciencesBeijing100085China

The successful control of hydrocarbon and CO emissions from low-temperature diesel exhausts requires the use of highly active co-oxidation *** this study,Sn was used to enhance the catalytic performance of Pd/CeO_(2)in CO and C_(3)H_(6)co-oxidation ***_(2)with added stannum(Sn)was prepared as a support using the co-precipitation method,and Pd was loaded onto the support using the impregnation *** Sn addition(the optimal Ce/Sn ratio is 0.75:0.25),the T_(50)values of CO and C_(3)H_(6)are reduced by 20 and 32℃,respectively.A series of characterization methods indicates that the addition of Sn to the support greatly enhances its lattice oxygen mobility and increases the proportion of *** the co-oxidation process,stronger lattice oxygen mobility allows CO to react faster through the Mars-van Krevelen mechanism,weakening the competition with C_(3)H_(6)for O_(2).A higher PdO content enhances the C_(3)H_(6)oxidation ***,CO can more readily reduce PdO than Pd^(2+)in solid solution with the support,which consequently further enhances co-oxidation ***,the addition of Sn is a simple and effective strategy for enhancing the performance of Pd/CeO_(2)catalysts in CO and C_(3)H_(6)co-oxidation ***,the promotional effect of CO achieved in this study contributes to a deeper understanding of the interactions that occur during the co-oxidation of C_(3)H_(6)and CO.

关键词： CO and C_(3)H_(6)co-oxidation Pd/CeSn Oxygen mobility Pd species Rare earths

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Chemical characteristics of long-term acid rain and its impact on lake water chemistry:A case study in Southwest China

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Journal of environmental Sciences 2024年第4期138卷 121-131页

作者： Liuyi Zhang JiaWang Shuxiao Wang Chunbo Wang Fumo Yang Tingzhen Li Chongqing Key Laboratory of Water Environment Evolution and Pollution Control in Three Gorges Reservoir Chongqing Three Gorges UniversityWanzhou 404000China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China College of Carbon Neutrality Future Technology Sichuan UniversityChengdu 610065China National Engineering Research Center on Flue Gas Desulfurization Chengdu 610065China

The chemical composition of acid rain and its impact on lake water chemistry in Chongqing,China,from 2000 to 2020 were studied in this *** regional acid rain intensity is affected jointly by the acid gas emissions and the neutralization of alkaline *** pH of precipitation experienced three stages of fluctuating decline,continuous improvement,and a slight *** pH showed inflection points in 2010,mainly due to the total control actions of SO_(2)and NO_(x)implemented in *** total ion concentrations in rural areas and urban areas were 489.08μeq/L and 618.57μeq/L,*** top four ions were SO_(4)^(2-),Ca^(2+),NH_(4)^(+)and NO_(3)^(-),which accounted for more than 90%of the total ion concentration,indicating the anthropogenic *** 2010,SO_(4)^(2-)fluctuated greatly while NO_(3)^(-)continued to rise;however,after 2010,both SO_(4)^(2-)and NO_(3)^(-)began to decline rapidly,with the rates of-12.03μeq/(L·year)and-4.11μeq/(L·year).Because the decline rate of SO_(4)^(2-)was 2.91 times that of NO_(3)^(-),the regional acid rain has changed from sulfuric acid rain to mixed sulfuric and nitric acid *** lake water is weakly acidic,with an average pH of 5.86,and the acidification frequency is 30.00%.Acidification of lake water is jointly affected by acid deposition and acid neutralization capacity of lake *** deposition has a profound impact on water acidification,and nitrogen(N)deposition,especially reduced N deposition,should be the focus of future research.

关键词： Acid rain Chemical composition Neutralization Nitrogen deposition Water acidification

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Underestimated benefits of NO_(x) control in reducing SNA and O_(3) based on missing heterogeneous HONO sources

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Frontiers of environmental Science & Engineering 2024年第3期18卷 57-67页

作者： Shuping Zhang Haotian Zheng Jun Liu Yao Shi Tianzeng Chen Chaoyang Xue Fenfen Zhang Yueqi Jiang Xiangping Zhang Shovan Kumar Sahu Biwu Chu Jia Xing State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China China Academy of Civil Aviation Science and Technology Beijing 100028China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Yellow River Institute of Hydraulic Research Zhengzhou 450003China Centre for Climate Research Singapore Meteorological Service SingaporeSingapore 537054Singapore

Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in *** traditional air quality model does not consider heterogeneous HONO chemistry,leading to uncertainties in estimating the benefits of NO_(x) *** studies have shown that the parameterization of heterogeneous HONO formation increases both the simulated value of sulfate–nitrate–ammonium(SNA)and that of O_(3),thus adding the heterogeneous reactions of HONO into air quality models inevitably leads to changes in the estimated benefits of NO_(x) *** we investigated the changes in SNA and O_(3)concentrations from NO_(x) emission reduction before and after adding heterogeneous HONO reactions in the Community Multi-Scale Air Quality(CMAQ)*** heterogeneous HONO reactions in the simulation improved the benefits of NO_(x) reduction in terms of SNA control in *** 80%NO_(x) reduction,the reduction in SNA increased from 36.9%without considering heterogeneous HONO reactions to 42.8%with heterogeneous HONO *** reduction in the maximum daily 8h average(MDA8)O_(3)in summer caused by NO_(x) reduction increased slightly from 4.7%to 5.2%after adding heterogeneous HONO *** results in this study highlight the enhanced effectiveness of NO_(x) controls for the reduction of SNA and O_(3)after considering heterogeneous HONO formation in a complex chemical ambient,demonstrating the importance of NO_(x) controls in reducing PM2.5 and O_(3)pollution in China.

关键词： Heterogeneous HONO NO_(x) reduction PM_(2.5) O_(3)

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A combined evaluation of the characteristics and antibiotic resistance induction potential of antibiotic wastewater during the treatment process

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Journal of environmental Sciences 2024年第4期138卷 626-636页

作者： Sun Miao Yanyan Zhang Cong Men Yiou Mao Jiane Zuo State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China School of Energy and Environmental Engineering Beijing Key Laboratory of Resource-Oriented Treatment of Industrial PollutantsUniversity of Science and Technology BeijingBeijing 100083China High School Affiliated to Renmin University of China Beijing 100080China Tsinghua Shenzhen International Graduate School Shenzhen 518055China

Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the *** these substances are mostly in concentrations lower than those known to induce AR individually,it is possible that antibiotic wastewater discharge might still promote the AR transmission risk via additive or synergistic ***,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains ***,samples were collected from different stages of a cephalosporin production wastewater treatment plant,and the potential AR induction effect of their chemical mixtures was explored through the exposure of the antibiotic-sensitive Escherichia coli K12 *** with raw cephalosporin production wastewater significantly promoted mutation rates(3.6×10^(3)-9.3×10^(3)-fold)and minimum inhibition concentrations(6.0-6.7-fold)of *** against ampicillin and *** may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on *** AR induction effect of cephalosporin wastewater decreased after the coagulation sedimentation treatment and was completely removed after the full treatment process.A Pearson correlation analysis revealed that the reduction in the AR induction effect had a strong positive correlation with the removal of organics and biological *** indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction *** study illustrates the potential AR transmission risk of antibiotic wastewater and highlights the need for its adequate treatment.

关键词： Antibiotic wastewater treatment plant Antibiotic resistance Antibiotic resistance induction effect Correlation analysis Biological toxicity

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Aerosol exposure assessment during reclaimed water utilization in China and risk evaluation in case of Legionella

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Frontiers of environmental Science & Engineering 2022年第7期16卷 173-183页

作者： Menghao Chen Liangliang Shi Gang Liu Xiaojin Wu Yun Lu State Key Joint Laboratory of Environmental Simulation and Pollution Control State Environment Protection Key Laboratory of Microorganism Application and Risk ControlSchool of EnvironmentTsinghua UniversityBeijing100084China

Reclaimed water utilization provides an effective way to alleviate water ***,the residual pathogens in the recycled water like Legionella,could be spread into the air as aerosols through water-to-air transmission *** the aerosols by the people nearby increases their susceptibility to *** estimating the health risks associated with the potential exposure of airborne Legionella emitted from the urban use of reclaimed water in China,nationwide questionnaire was designed to investigate the exposure habits of Chinese population in different *** microbial risk assessment(QMRA)served as the suitable explanatory tool to estimate the *** results indicated that annual infection probability of populations exposed to Legionella for three scenarios,0.0764(95%CI:0.0032−0.6880)for road cleaning,1.0000(95%CI:0.1883−1.0000)for greenfield irrigation,0.9981(95%CI:0.0784−1.0000)for landscape fountain,were markedly higher than the threshold recommended by WHO(10^(−4) per person per year(pppy))according to the concentration distribution of Legionella in the reclaimed *** age-,educational background-,region-and gender-specific data in annual infection probability also showed different tendencies for some *** study provides some detailed information on the health risks from the water reuse in China and will be useful to promote the safe application of reclaimed water in water-deficient areas.

关键词： Legionella QMRA Reclaimed water Aerosol Water reuse

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Enhancing ozone catalytic decomposition through acid treatment ofα-MnO_(2) for improved activity and humidity resistance

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Journal of environmental Sciences 2025年第3期149卷 35-45页

作者： Shangchao Xiong Kai Zhang Zhenghao Xu Hongjun Ou Yuanyuan Zheng Xi Li Yue Peng Xubiao Luo Junhua Li School of Life Sciences Jinggangshan UniversityJi’an 343009China Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengdu 610031China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Post-etching method using dilute acid solutions is an effective technology to modulate the surface compositions of metal-oxide *** theα-MnO_(2) catalyst treated with 0.1 mol/L nitric acid exhibits higher ozone decomposition activity at high relative humidity than the counterpart treated with acetic *** the increases in surface area and lattice dislocation,the improved activity can be due to relatively higher Mn valence on the surface and newly-formed Brønsted acid sites adjacent to oxygen *** remnant nitro species deposited on the catalyst by nitric acid treatment is ideal hydrophobic groups at ambient *** decomposition route is also proposed based on the DRIFTS and DFT calculations:ozone is facile to adsorb on the oxygen vacancy,and the protonic H of Brønsted acid sites bonds to the terminal oxygen of ozone to accelerate its cleavage to O_(2),reducing the reaction energy barrier of O_(2) desorption.

关键词： Ozone decomposition α-MnO_(2) Brønsted acid sites H-bonds Post-etching

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Uncovering the coupling effect with energy-related carbon emissions and human development variety in Chinese provinces

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Journal of environmental Sciences 2024年第5期139卷 527-542页

作者： Liu Chen Yiqi Tan Gengpei Lv Weiguang Cai Xiaofeng Gao Rui Li School of Management Science and Real Estate Chongqing UniversityChongqing 400044China State Key Joint Laboratory of Environment Simulation and Pollution Control(SKLESPC) School of EnvironmentTsinghua UniversityBeijing 100084China Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment Ministry of EducationCollege of Environment and EcologyChongqing UniversityChongqing 400044China

Lessening energy-related carbon emissions has become a crucial measure to achieve Chinese carbon *** study is the first to construct a Difference in Carbon pressures-adjusted Human Development Index(DCHDI)model for the purpose of exploring the coupling effect between carbon emissions and human development variety from 2000 to 2019 in Chinese *** demonstrate the following.(1)The total energy-related carbon footprint of 30 provinces in China reached 10.2 billion tons in 2019,with an average annual growth rate of 6.93% over the past two decades;and the provinces with the highest carbon emissions per capita are InnerMongolia,Ningxia,and Shanxi.(2)At the provincial level,we observed that the Human Development Index(HDI),which includes life expectancy,education,and income,has been rising,while Beijing,Shanghai,and Tianjin entered the super-high HDI level before 2008.(3)The entire coupling effect of 30 Chinese provinces has been broadly fortified in the last 20 years,but the growth rate of DCHDI values in 2011-2019 has slowed down compared with that in 2000-2010;the clustering phenomenon demonstrated that this discovery is associated with historical peaks in total carbon emissions.(4)The co-ordination degree of carbon emissions per capita and HDI was verified,and 96% of the data points were found in the range of super high coupling coordination ***,this study provides the government with worthwhile guidance for decision-making and carbon reduction strategies for other countries struggling to advance human sustainable development.

关键词： Energy-related carbon emissions Human sustainable development DCHDI model Coupling effect Chinese provinces

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Decomplexation of Cu-1-hydroxyethylidene-1,1-diphosphonic acid by a three-dimensional electrolysis system with activated biochar as particle electrodes

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Journal of environmental Sciences 2023年第2期124卷 630-643页

作者： Xing Wang Zilong Zhao Hongjie Wang Feng Wang Wenyi Dong School of Civil and Environmental Engineering Harbin Institute of Technology ShenzhenShenzhen 518055China Shenzhen Key Laboratory of Water Resource Utilization and Environmental Pollution Control Shenzhen 518055China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

The feasibility of decomplexation removal of typical contaminants in electroplating wastewater,complexed Cu(Ⅱ)with 1-hydroxyethylidene-1,1-diphosphonic acid(Cu-HEDP),was first performed by a three-dimensional electrode reactor with activated biochar as particle *** the case of 50 mg/L Cu-HEDP,Cu(Ⅱ)removal(90.7%)and PO_(4)^(3−)conversion(34.9%)were achieved under the conditions of electric current 40 mA,initial pH 7,acid-treated almond shell biochar(AASB)addition 20 g/L,and reaction time 180 min,with second-order rate constants of 1.10×10^(−3) and 1.94×10^(−5) min^(−1) *** growing chelating effect between Cu(II)and HEDP and the comprehensive actions of adsorptive accumulation,direct and indirect oxidation given by particle electrodes accounted for the enhanced removal of Cu-HEDP,even though the mineralization of HEDP was mainly dependent on anode *** performance attenuation of AASB particle electrodes was ascribed to the excessive consumption of oxygen-containing functionalities during the reaction,especially acidic carboxylic groups and quinones on particle electrodes,which decreased from 446.74 to 291.48μmol/g,and 377.55 to 247.71μmol/g,*** on the determination of adsorption behavior and indirect electrochemical oxidation mediated by in situ electrogenerated H_(2)O_(2) and reactive oxygen species(e.g.,•OH),a possible removal mechanism of Cu-HEDP by three-dimensional electrolysis was further proposed.

关键词： Cu-HEDP Electrochemical oxidation Particle electrode Reaction characteristics Removal mechanism

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