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Four decades of full-scale nitrous oxide emission inventory in china

national science Review 2024年第3期11卷 137-149页

作者： Minqi Liang Zheyan Zhou Peiyang Ren Han Xiao Xu-Ri Zhongmin Hu Shilong Piao Hanqin Tian Qing Tong Feng Zhou Jing Wei Wenping Yuan School of Atmospheric sciences Guangdong Province Data Center of Terrestrial and Marine Ecosystems Carbon Cycle Sun Yat-sen University State Key Laboratory of Tibetan Plateau Earth System Resources and Environment Institute of Tibetan Plateau Research Chinese Academy of Sciences Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province Hainan University Sino-French Institute for Earth System science College of Urban and Environmental SciencesPeking University Schiller Institute for Integrated science and Society Department of Earth and Environmental Sciences Boston College Institute of Energy Environment and Economy Tsinghua University Southern Marine science and Engineering Guangdong Laboratory(Zhuhai)

china is among the top nitrous oxide（N2O）-emitting countries, but existing national inventories do not provide full-scale emissions including both natural and anthropogenic sources. We conducted a four-decade（1980–2020） of comprehensive quantification of Chinese N2O inventory using empirical emission factor method for anthropogenic sources and two up-to-date process-based models for natural sources. Total N2O emissions peaked at 2287.4（1774.8–2799.9） Gg N2O yr-1in 2018, and agriculture-developed regions, like the East, Northeast, and Central, were the top N2O-emitting regions. Agricultural N2O emissions have started to decrease after 2016 due to the decline of nitrogen fertilization applications, while, industrial and energetic sources have been dramatically increasing after 2005. N2O emissions from agriculture, industry,energy, and waste represented 49.3%, 26.4%, 17.5%, and 6.7% of the anthropogenic emissions in 2020,respectively, which revealed that it is imperative to prioritize N2O emission mitigation in agriculture,industry, and energy. natural N2O sources, dominated by forests, have been steadily growing from 317.3（290.3–344.1） Gg N2O yr-1in 1980 to 376.2（335.5–407.2） Gg N2O yr-1in 2020. Our study produces a Full-scale Annual N2O dataset in china（FAN2020）, providing emergent counting to refine the current national N2O inventories.

关键词： nitrous oxide four decades anthropogenic sources natural sources

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Dual-Defect Engineering Strategy Enables High-Durability Rechargeable Magnesium-Metal Batteries

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Nano-Micro Letters 2024年第9期16卷 449-461页

作者： Fuyu Chen Bai‑Qing Zhao Kaifeng Huang Xiu‑Fen Ma Hong‑Yi Li Xie Zhang Jiang Diao Jili Yue Guangsheng Huang Jingfeng Wang Fusheng Pan national Innovation Center for Lndustry‑Education Integration of Energy Storage Technology School of Materials Science and EngineeringChongqing UniversityChongqing 400044People’s Republic of China national Magnesium Alloy Material Engineering Technology Research Center Chongqing UniversityChongqing 400044People’s Republic of China Materials and Energy Division Beijing Computational Science Research CenterBeijing 100193People’s Republic of China School of Materials science and Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China national Key Laboratory of Advanced Casting Technologies Chongqing UniversityChongqing 400044People’s Republic of China

Rechargeable magnesium-metal batteries(RMMBs)are promising next-generation secondary batteries;however,their development is inhibited by the low capacity and short cycle lifespan of cathodes.Although various strategies have been devised to enhance the Mg^(2+)migration kinetics and structural stability of cathodes,they fail to improve electronic conductivity,rendering the cathodes incompatible with magnesium-metal anodes.Herein,we propose a dual-defect engineering strategy,namely,the incorporation of Mg^(2+)pre-intercalation defect(P-Mgd)and oxygen defect(Od),to simultaneously improve the Mg^(2+)migration kinetics,structural stability,and electronic conductivity of the cathodes of RMMBs.Using lamellar V_(2)O_(5)·nH_(2)O as a demo cathode material,we prepare a cathode comprising Mg0.07V_(2)O_(5)·1.4H_(2)O nanobelts composited with reduced graphene oxide(MVOH/rGO)with P-Mgd and Od.The Od enlarges interlayer spacing,accelerates Mg^(2+)migration kinetics,and prevents structural collapse,while the P-Mgd stabilizes the lamellar structure and increases electronic conductivity.Consequently,the MVOH/rGO cathode exhibits a high capacity of 197 mAh g^(−1),and the developed Mg foil//MVOH/rGO full cell demonstrates an incredible lifespan of 850 cycles at 0.1 A g^(−1),capable of powering a light-emitting diode.The proposed dual-defect engineering strategy provides new insights into developing high-durability,high-capacity cathodes,advancing the practical application of RMMBs,and other new secondary batteries.

关键词： Rechargeable magnesium-metal batteries Dual-defect engineering Vanadium-based cathode High durability Lamellar structure

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Fine particle trace elements at a mountain site in southern china:Source identification,transport,and health risks

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Journal of Environmental sciences 2024年第7期141卷 166-181页

作者： Jiaoping Xing Runping Ding Feifeng Chen Linyu Peng Wenhua Wang Xiaoyan Song Qing Ye Yuanqiu Liu Key Laboratory of State Forestry and Grassland Administration on Forest Ecosystem Protection and Restoration of Poyang Lake Watershed School of ForestryJiangxi Agricultural UniversityNanchang 330045China School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdao 066004China College of Geosciences and Engineering North China University of Water Resources&Electric PowerZhengzhou 450046China

Trace elements in atmospheric particulate matter play a significant role in air quality,human health,and biogeochemical cycles.In this study,the trace elements(Ca,Al,K,Fe,Na,Mg,Zn,Pb,Mn,Ti,Cu,Cr,Sr,Ni)in PM2.5samples collected at the summit of Mt.Lushan were analyzed to quantify their abundance,source,transport,and health risks.During the whole sampling period,the major trace elements was Ca,Al,and K.While the trace metals with the lowest concentrations were Sr,Ni,Rb,and Cd.The trace elements were influenced by air mass transport routes,exhibiting an increasing trend of crustal elements in the northwesterly airmass and anthropogenic elements(Zn,Mn,Cu,and Ni)in the easterly air masses.Construction dust,coal+biomass burning,vehicle emission,urban nitrate-rich+urban waste incineration emissions,and soil dust+industry emissions were common sources of PM2.5on Mt.Lushan.Different air mass transport routes had various source contribution patterns.These results indicate that trace elements at Mt.Lushan are influenced by regional anthropogenic emissions and monsoon-dominated trace element transport.The total resulting cancer risk value that these elements posed were below the acceptable risk value of 1×10^(-6),while the non-carcinogenic risk value(1.72)was higher than the safety level,suggesting that non-carcinogenic effects due to these trace elements inhalation were likely to occur.Vehicle emission and coal+biomass burning were the common dominant sources of non-cancer risks posed by trace elements at Mt.Lushan.

关键词： Trace elements Risk assessment Cluster analysis Source apportionment

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Laboratory and field evaluation of a low-cost optical particle sizer

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Journal of Environmental sciences 2024年第8期142卷 215-225页

作者： Mingzhen Tang Yicheng Shen Yanzhen Ge Jian Gao Chong Wang Liqing Wu Shuchun Si State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China Jinan Grid-Based Supervision Center of Ecological and Environmental Protection Jinan 250100China Tai’an Ecological Environment Protection Control Center Tai’an 271000China School of Physics Shandong UniversityJinan 250013China

Low-cost sensors are widely used to collect high-spatial-resolution particulate matter data that traditional reference monitoring devices cannot.In addition to the mass concentration,the number concentration and size distribution are also fundamental in determining the origin and hazard level of particulate pollution.Therefore,low-cost optical sensors have been improved to establish optical particle sizers(OPSs).In this study,a low-cost OPS,the Nova SDS029,is introduced,and it is evaluated in comparison to two reference instruments—the GRIMM 11-D and the TSI 3330.We first tested the sizing accuracy using polystyrene latex spheres.Then,we assessed the mass and number size distribution accuracy in three application scenarios:indoor smoking,ambient air quality,and mobile monitoring.The evaluations suggest that the low-cost SDS029 rivals research-grade optical sizers in many aspects.For example,(1)the particle diameters obtained with the SDS029 are close to the reference instruments(usually<10%)in the 0.3-5μm range;(2)the number of particles and mass concentration are highly correlated(r≥0.99)with the values obtained with the reference instruments;and(3)the SDS029 slightly underestimates the number concentration,but the derived PM_(2.5)values are closer to monitoring station than the reference instruments.The successful application of the SDS029 in multiple scenarios suggests that a plausible particle size distribution can be obtained in an easy and cost-efficient way.We believe that low-cost OPSs will increasingly be used to map the sources and risk levels of particles at the city scale.

关键词： Optical particle sizer Particle size distribution Low-cost sensor Evaluation Field application

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Optoelectronic Synapses Based on MXene/Violet Phosphorus van der Waals Heterojunctions for Visual‑Olfactory Crossmodal Perception

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Nano-Micro Letters 2024年第6期16卷 38-52页

作者： Hailong Ma Huajing Fang Xinxing Xie Yanming Liu He Tian Yang Chai Center for Advancing Materials Performance From the Nanoscale(CAMP‑Nano) State Key Laboratory for Mechanical Behavior of MaterialsXi’an Jiaotong UniversityXi’an 710049People’s Republic of China Institute of Microelectronics and Beijing national Research Center for Information science and Technology(BNRist) Tsinghua UniversityBeijing 100084People’s Republic of China Department of Applied Physics The Hong Kong Polytechnic UniversityHong KongPeople’s Republic of China

The crossmodal interaction of different senses,which is an important basis for learning and memory in the human brain,is highly desired to be mimicked at the device level for developing neuromorphic crossmodal perception,but related researches are scarce.Here,we demonstrate an optoelectronic synapse for vision-olfactory crossmodal perception based on MXene/violet phosphorus(VP)van der Waals heterojunctions.Benefiting from the efficient separation and transport of photogenerated carriers facilitated by conductive MXene,the photoelectric responsivity of VP is dramatically enhanced by 7 orders of magnitude,reaching up to 7.7 A W^(−1).Excited by ultraviolet light,multiple synaptic functions,including excitatory postsynaptic currents,pairedpulse facilitation,short/long-term plasticity and“learning-experience”behavior,were demonstrated with a low power consumption.Furthermore,the proposed optoelectronic synapse exhibits distinct synaptic behaviors in different gas environments,enabling it to simulate the interaction of visual and olfactory information for crossmodal perception.This work demonstrates the great potential of VP in optoelectronics and provides a promising platform for applications such as virtual reality and neurorobotics.

关键词： Violet phosphorus MXene Van der Waals heterojunctions Optoelectronic synapses Crossmodal perception

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Decomposition mechanisms of nuclear-grade cationic exchange resin by advanced oxidation processes:Statistical molecular fragmentation model and DFT calculations

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Journal of Environmental sciences 2024年第1期135卷 433-448页

作者： Xiang Meng Pierre Désesquelles Lejin Xu Department of Nuclear Engineering and Technology School of Energy and Power EngineeringHuazhong University of Science&TechnologyWuhan 430074China CNRS Laboratoire de Physique des Gaz et des PlasmasUniversitéParis-SaclayOrsay 91405France State Key Laboratory of Coal Combustion School of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The treatment and disposal of radioactive waste are presently facing great challenges.Spent ion exchange resins have become a focus of attention due to their high production and serious environmental risks.In this paper,a simplified model of cationic exchange resin is proposed,and the degradation processes of cationic resin monomer initiated by hydroxyl radicals(·OH)are clarified by combining statistical molecular fragmentation(SMF)model and density functional theory(DFT)calculations.The prediction of active sites indicates that the S-O bonds and the C-S bond of the sulfonic group are more likely to react during the degradation.The meta-position of the sulfonic group on the benzene ring is the most active site,and the benzene ring without the sulfonic group has a certain reactivity.The C11-C14 and C17-C20 bonds,on the carbon skeleton,are the most easily broken.It is also found that dihydroxy addition and elimination reactions play a major role in the process of desulfonation,carbon skeleton cleavage and benzene ring separation.The decomposition mechanisms found through the combination of physical models and chemical calculations,provide theoretical guidance for the treatment of complex polycyclic aromatic hydrocarbons.

关键词： Cationic exchange resin Statistical molecular fragmentation model Density functional theory Hydroxyl radical Decomposition mechanism

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Evaluating the performance and influencing factors of three portable black carbon monitors for field measurement

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Journal of Environmental sciences 2024年第5期139卷 320-333页

作者： Liqing Wu Yicheng Shen Fei Che Yuzhe Zhang Jian Gao Chong Wang State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China Jinan Ecological Environmental Protection Grid-Based Supervision Center Jinan 250013China

Black carbon(BC)is associated with adverse human health and climate change.Mapping BC spatial distribution imperatively requires low-cost and portable devices.Several portable BC monitors are commercially available,but their accuracy and reliability are not always satisfactory during continuous field observation.This study evaluated three models of portable black carbon monitors,C12,MA350 and DST,and investigates the factors that affect their performance.The monitors were tested in urban Beijing,where portable devices running for one month alongside a regular-size reference aethalometer AE33.The study considers several factors that could influence the monitors'performance,including ambient weather,aerosol composition,loading artifacts,and built-in algorithms.The results show that MA350and DST present considerable discrepancies to the reference instrument,mainly occurring at lower concentrations(0-500 ng/m^(3))and higher concentrations(2500-8000 ng/m^(3)),respectively.These discrepancies were likely caused by the anomalous noise of MA350 and the loading artifacts of DST.The study also suggests that the ambient environment has limited influence on the monitors'performance,but loading artifacts and accompanying compensation algorithms can result in unrealistic data.Based on the evaluation,the study suggests that C12 is the best choice for unsupervised field measurement,DST should be used in scenarios where frequent maintenance is available,and MA350 is suitable for research purposes with post-processing applicable.The study highlights the importance of assigning portable BC monitors to appropriate applications and the need for optimized real-time compensation algorithms.

关键词： Black carbon Aethalometer Loading artifact Performance evaluation Portable device

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Mass transfer characteristics of chiral pharmaceuticals on membrane used for polar organic chemical integrative sampler

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Journal of Environmental sciences 2024年第2期136卷 670-681页

作者： Liyang Wang Ruixia Liu Youya Zhou Peng Yuan Xiaoling Liu Hongjie Gao College of Water science Beijing Normal UniversityBeijing 100018China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental ScienceBeijing 100012China Technical Centre for Soil Agriculture and Rural Ecology and EnvironmentMinistry of Ecology and EnvironmentBeijing 100012China

Passive sampling technology has good application prospects for monitoring trace pollutants in aquatic environments.Further research on the sampling mechanism of this technology is essential to improve the measurement accuracy and extend the application scope of this approach.In this study,adsorption and permeation experiments were performed to investigate the sorption and mass transfer properties of five chiral pharmaceuticals at the enantiomeric level on polyethersulfone(PES)and polytetrafluoroethylene(PTFE)membranes used in a polar organic chemical integrative sampler.Batch adsorption experiments showed that the PES membrane had an adsorption phenomenon for most selected pollutants and an insignificant sorption behavior was observed for all selected pharmaceuticals on the PTFE membrane except for R(S)-fluoxetine.The diffusion coefficients of selected pharmaceuticals onto the PTFE membrane were approximately one order of magnitude higher than those onto the PES membrane.The permeation experiment indicated that under different hydraulic conditions,the change of the relative pollutant concentration through the PTFE membrane for the composite pollutant system was more obvious than that for the single pollutant system,and mass transfer hysteresis exists for both contaminant systems through PES membranes.Using the first-order equation or 3-component model to estimate the overall mass transfer coefficients,the results showed that the overall mass transfer coefficient values of pollutants in the composite pollutant system onto both membranes were higher than those in the single pollutant system.This parameter was mainly influenced by the synergistic effects of the multi-analyte interaction and diminished water boundary layers during the mass transfer process.

关键词： Sorption phenomenon Permeation behavior Mass transfer properties Modeling calculation Chiral pharmaceuticals PES and PTFE membrane

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Performance and mechanism of La-Fe metal-organic framework as a highly efficient adsorbent for fluoride removal from mine water

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Journal of Environmental sciences 2024年第5期139卷 245-257页

作者： Chaomin Jia Jianbing Wang Huijiao Wang Sichao Zhu Xiaohui Zhang Yuxiang Wang School of Chemical&Environmental Engineering China University of Mining&Technology-BeijingBeijing 100083China Beijing Polytechnic Beijing 100176China Chinese Society for Urban Studies Beijing 100835China

Water fluoride pollution has caused non-negligible harm to the environment and humans,and thus it is crucial to find a suitable treatment technology.In this study,La-Fe@PTA adsorbent was synthesized for the defluoridation of mine water.The results showed that the optimum conditions for defluoridation by La-Fe@PTA were p H close to 7.0,the initial F-concentration of 10 mg/L,the dosage of 0.5 g/L and the adsorption time of 240 min.Compared with SO_4^(2-),Cl^(-),NO_(3)^(-),Ca^(2+)and Mg^(2+),CO_(3)^(2-)and HCO_(3)^(-)presented severer inhibition on fluoride uptake by La-Fe@PTA.The adsorption process fits well with the pseudo-second-order kinetic model and Freundlich model,and the maximum adsorption capacity of Langmuir model was 95 mg/g.Fixed-bed adsorption results indicated that fluoride in practical fluorinated mine water could be effectively removed from 3.6 mg/L to less than 1.5 mg/L within130 bed volume(BV)by using 1.5 g La-Fe@PTA.Furthermore,the adsorbent still had good adsorption capacity after regeneration,which confirms the great application potential of La-Fe@PTA as a fluoride ion adsorbent.The mechanism analysis showed that La-Fe@PTA adsorption of fluorine ions is a physicochemical reaction driven by electrostatic attraction and ion exchange.

关键词： Adsorption La-Fe@PTA Fluoride ion Mine water Mechanism

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Long-term exposure to aryl hydrocarbon receptor agonist neburon induces reproductive toxicity in male zebrafish(Danio rerio)

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Journal of Environmental sciences 2024年第8期142卷 193-203页

作者： Fucong Zhang Chen Tang Yue Zhu Qian Wang Xin Huang Chunyan Yang Chengyong He Zhenghong Zuo Key Laboratory of the Ministry of Education for Coastal and Wetland Ecosystems School of Life SciencesXiamen UniversityXiamen 361102China

Neburon is a phenylurea herbicide that is widely used worldwide,but its toxicity is poorly studied.In our previous study,we found that neburon has strong aryl hydrocarbon receptor(AhR)agonist activity,but whether it causes reproductive toxicity is not clear.In the present study,zebrafish were conducted as a model organism to evaluate whether environmental concentrations of neburon(0.1,1 and 10μg/L)induce reproductive disorder in males.After exposure to neburon for 150 days from embryo to adult,that the average spawning egg number in high concentration group was 106.40,which was significantly lower than 193.00in control group.This result was mainly due to the abnormal male reproductive behavior caused by abnormal transcription of genes associated with reproductive behavior in the brain,such as secretogranin-2a.The proportions of spermatozoa in the medium and high concentration groups were 82.40%and 83.84%,respectively,which were significantly lower than 89.45%in control group.This result was mainly caused by hormonal disturbances and an increased proportion of apoptotic cells.The hormonal disruption was due to the significant changes in the transcription levels of key genes in the hypothalamus-pituitary-gonadal axis following neburon treatment.Neburon treatment also significantly activated the AhR signaling pathway,causing oxidative stress damage and eventually leading to a significant increase in apoptosis in the exposed group.Together,these data filled the currently more vacant profile of neburon toxicity and might provide information to assess the ecotoxicity of neburon on male reproduction at environmentally relevant concentrations.

关键词： Zebrafish Neburon Male reproductive toxicity HPG axis AhR agonist

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