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Cu-optimized long-range interaction between Co nanoparticles and Co single atoms:Improved Fenton-like reaction activity

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science Bulletin 2024年第16期69卷 2529-2542页

作者： Fan Mo Zelin Hou Qixing Zhou Xixi Chen Weitao Liu Wendan Xue Qi Wang Jianling Wang Tong Zheng Zongxin Tao Key Laboratory of Pollution Processes and environmental Criteria(Ministry of Education)/Tianjin Key Laboratory of environmental Remediation and Pollution Control Carbon Neutrality Interdisciplinary Science CenterCollege of Environmental Science and EngineeringNankai UniversityTianjin 300350China National engineering research center of Pesticide Nankai UniversityTianjin 300350China

The interplay between multi-atom assembly configurations and single atoms(SAs)has been gaining attention in ***,the effect of long-term range interactions between SAs and multi-atom assemblies on the orbital filling characteristics has yet to be *** this context,we introduced copper(Cu)doping to strengthen the interaction between cobalt(Co)nanoparticles(NPs)and Co SAs by promoting the spontaneous formation of Co-Cu alloy NPs that tends toward aggregation owing to its negative cohesive energy(-0.06454),instead of forming Cu *** incorporation of Cu within the Co-Cu alloy NPs,compared to the pure Co NPs,significantly expedites the kinetics of peroxymonosulfate(PMS)oxidation processes on Co *** Co NPs,Co-Cu NPs facilitate electron rearrangement in the d orbitals(especially dz^(2)and dxz)near the Fermi level in Co SAs,thereby optimizing the dz^(2)-O(PMS)and dxz-O(SO_(5)^(-))orbital ***,the Co-Cu alloy NPs embedded in nitrogen-doped carbon(CC@CNC)catalysts rapidly eliminated 80.67% of 20 mg L^(-1)carbamazepine(CBZ)within 5 *** performance significantly surpasses that of catalysts consisting solely of Co NPs in a similar matrix(C@CNC),which achieved a 58.99% reduction in 5 *** quasi in situ characterization suggested that PMS acts as an electron donor and will transfer electrons to Co SAs,generating^(1)O_(2)for contaminant *** study offers valuable insights into the mechanisms by which composite active sites formed through multi-atom assembly interact at the atomic orbital level to achieve high-efficiency PMS-based advanced oxidation processes at the atomic orbital level.

关键词： Spontaneous alloying Co-Cu alloy NPs Co SAs Synergism Orbital electron filling

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In-situ sludge reduction based on Mn^(2+)-catalytic ozonation conditioning:Feasibility study and microbial mechanisms

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Journal of environmental sciences 2024年第1期135卷 185-197页

作者： Haozhe Huang Tingting Wei Hui Wang Bing Xue Sisi Chen Xiankai Wang Haibin Wu Bin Dong Zuxin Xu College of environmental science and engineering Tongji UniversityShanghai 200092China YANGTZE Eco-Environment engineering research center China Three Gorges CorporationBeijing 100038China

To improve the sludge conditioning efficiency without increasing the ozone dose,an in-situ sludge reduction process based on Mn^(2+)-catalytic ozonation conditioning was *** ozone conditioning alone as a control,a lab-scale sequencing batch reactor coupled with ozonated sludge recycle was evaluated for its operating performance at an ozone dose of 75 mg O_(3)/g VSS and 1.5 mmol/L Mn^(2+)*** results showed a 39.4%reduction in MLSS and an observed sludge yield of 0.236 kg MLSS/kg COD for the O_(3)+Mn^(2+)group compared to the O_(3)group (15.3%and 0.292 kg MLSS/kg COD),accompanied by better COD,NH_(4)^(+)-N,TN and TP removal,improved effluent SS and limited impact on excess sludge ***,activity tests,BIOLOG ECO microplates and 16S rRNA sequencing were applied to elucidate the changing mechanisms of Mn^(2+)-catalytic ozonation related to microbial action:(1) Dehydrogenase activity reached a higher peak.(2) Microbial utilization of total carbon sources had an elevated effect,up to approximately 18%,and metabolic levels of six carbon sources were also increased,especially for sugars and amino acids most pronounced.(3) The abundance of Defluviicoccus under the phylum Proteobacteria was enhanced to 12.0%and dominated in the sludge,they had strong hydrolytic activity and metabolic *** bacteria of the genus Ferruginibacter also showed an abundance of 7.6%,they contributed to the solubilization and reduction of sludge *** results could guide researchers to further reduce ozonation conditioning costs,improve sludge management and provide theoretical support.

关键词： Activated sludge In-situ reduction Catalytic ozonation conditioning Dehydrogenase activity Carbon source utilization Microbial community

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Design of Resilient Sensor Networks Balancing Resilience and Efficiency

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International Journal of Disaster Risk science 2024年第1期15卷 107-115页

作者： Sergey N.Vecherin Kiril D.Ratmanski Luke Hogewood Igor Linkov Cold Regions research and engineering Laboratory Engineering Research and Development CenterHanoverNH 03755USA environmental Laboratory Engineering Research and Development CenterVicksburgMS 39180USA

In recent years,the notion of resilience has been developed and applied in many technical areas,becoming exceptionally pertinent to disaster risk *** a disaster situation,accurate sensing information is the key to efficient recovery *** general,resilience aims to minimize the impact of disruptions to systems through the fast recovery of critical functionality,but resilient design may require redundancy and could increase *** this article,we describe a method based on binary linear programming for sensor network design balancing efficiency with *** application of the developed framework is demonstrated for the case of interior building surveillance utilizing infrared sensors in both twoand three-dimensional *** method provides optimal sensor placement,taking into account critical functionality and a desired level of resilience and considering sensor type and *** problem formulation,resilience requirements,and application of the optimization algorithm are described in *** of sensor locations with and without resilience requirements shows that resilient configuration requires redundancy in number of sensors and their intelligent *** tasks are successfully solved by the described method,which can be applied to strengthen the resilience of sensor networks by *** proposed methodology is suitable for large-scale optimization problems with many sensors and extensive coverage areas.

关键词： Binary linear programming Optimal sensor placement Redundant networks Resilience and efciency Resilient sensor networks

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Insight into the microbial community of denitrification process using different solid carbon sources: Not only bacteria

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Journal of environmental sciences 2024年第10期144卷 87-99页

作者： Congyu Li Yu Ling Yanjie Zhang Haiyan Wang Huan Wang Guokai Yan Weiyang Dong Yang Chang Liang Duan State Key Laboratory of environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China College of environmental science and engineering Tongji UniversityShanghai 200092China College of Water sciences Beijing Normal UniversityBeijing 100875China research center of environmental Pollution Control Technology Chinese Research Academy of Environmental ScienceBeijing 100012China State environmental Protection Key Laboratory of Estuarine and Coastal Environment Chinese Research Academy of Environmental SciencesBeijing 100012China

There is a lack of understanding about the bacterial,fungal and archaeal communities’composition of solid-phase denitrification(SPD)*** investigated four SPD systems with different carbon sources by analyzing microbial gene sequences based on operational taxonomic unit(OTU)and amplicon sequence variant(ASV).The results showed that the corncob-polyvinyl alcohol sodium alginate-polycaprolactone(CPSP,0.86±0.04 mg NO_(3)^(−)-N/(g·day))and corncob(0.85±0.06 mg NO_(3)^(−)-N/(g·day))had better denitrification efficiency than polycaprolactone(PCL,0.29±0.11 mg NO_(3)^(−)-N/(g·day))and polyvinyl alcoholsodium alginate(PVA-SA,0.24±0.07 mg NO_(3)^(−)-N/(g·day)).The bacterial,fungal and archaeal microbial composition was significantly different among carbon source types such as Proteobacteria in PCL(OTU:83.72%,ASV:82.49%)and Rozellomycota in PVA-SA(OTU:71.99%,ASV:81.30%).ASV methods can read more microbial units than that of OTU and exhibit higher alpha diversity and classify some species that had not been identified by OTU such as Nanoarchaeota phylum,unclassified_f_Xanthobacteraceae genus,etc.,indicating ASV may be more conducive to understand SPD microbial *** co-occurring network showed some correlation between the bacteria fungi and archaea species,indicating different species may collaborate in SPD *** KEGG function prediction results were obtained in two bioinformatic methods generally and some fungi and archaea functions should not be ignored in SPD *** results may be beneficial for understanding microbial communities in SPD systems.

关键词： Solid-phase denitrification Solid carbon source Microbial community ASV analysis OTU analysis

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Cardiac energy metabolism disorder mediated by energy substrate imbalance and mitochondrial damage upon tebuconazole exposure

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Journal of environmental sciences 2024年第2期136卷 270-278页

作者： Tingting Ku Jindong Hu Mengmeng Zhou Yuanyuan Xie Yutong Liu Xin Tan Lin Guo Guangke Li Nan Sang College of environmental science and Resources Research Center of Environment and HealthShanxi UniversityTaiyuan 030006China

Tebuconazole exposure has been described as an increasing hazard to human *** increasing number of recent studies have shown a positive association between tebuconazole exposure and cardiovascular disease risk,which is characterized by the reduction of adenosine triphosphate(ATP)***,researches on the damage of tebuconazole exposure to energy metabolism and the related molecular mechanisms are *** the present study,male C57BL/6 mice were treated with tebuconazole at different low concentrations for 4 *** results indicated that tebuconazole could accumulate in the heart and further induce the decrease of ATP content in the mouse ***,tebuconazole induced an obvious shift in substrate utilization of fatty acid and glucose by disrupting their corresponding transporters(GLUT1,GLUT4,CD36,FABP3 and FATP1)expression,and significantly repressed the expression of mitochondrial biogenesis(Gabpa and Tfam)and oxidative phosphorylation(CS,Ndufa4,Sdhb,Cox5a and Atp5b)related genes in a dosedependent *** investigation revealed that these alterations were related to the IRS1/AKT and PPARγ/RXRα*** findings contribute to a better understanding of triazole fungicide-induced cardiovascular disease by revealing the key indicators associated with this phenomenon.

关键词： Tebuconazole Cardiotoxicity Energy metabolic disorders Energy substrate Mitochondrial damage

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Boosting oxygen vacancies by modulating the morphology of Au decorated In_(2)O_(3)with enhanced CO_(2)hydrogenation activity to CH_(3)OH

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Journal of environmental sciences 2024年第6期140卷 91-102页

作者： Ruxian Hou Jiewen Xiao Qian Wu Tianyu Zhang Qiang Wang Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for Water Pollution Source Control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

CO_(2)hydrogenation to methanol has become one of the most promising ways for CO_(2)utilization,however,the CO_(2)conversion rate and methanol selectivity of this reaction still need to be improved for industrial *** we investigated the structure-activity relationship for CO_(2)conversion to methanol of In_(2)O_(3)-based catalysts by modulating morphology and decorating *** different Au/In_(2)O_(3)catalysts were prepared,their activity follow the sequence of Au/In_(2)O_(3)-nanosphere(Au/In_(2)O_(3)-NS)>Au/In_(2)O_(3)-nanoplate(Au/In_(2)O_(3)-NP)>Au/In_(2)O_(3)-hollow microsphere(Au/In_(2)O_(3)-HM).Au/In_(2)O_(3)-NS exhibited the best performance with good CO_(2)conversion of 12.7%,high methanol selectivity of 59.8%,and large space time yield of 0.32 g CH_(3)OH/(hr·gcat)at 300℃.The high performance of Au/In_(2)O_(3)-NS was considered as the presence of *** contributes to the creation of more surface oxygen vacancies,which further promoted the CO_(2)adsorption and facilitated CO_(2)activation to form the formate intermediates towards *** work clearly suggests that the activity of In_(2)O_(3)catalyst can be effective enhanced by structure engineering and Au decorating.

关键词： CO_(2)hydrogenation Methanol Au/In_(2)O_(3) Morphology Oxygen vacancies

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Analyzing the spatiotemporal evolution and driving forces of gross ecosystem product in the upper reaches of the Chaobai River Basin

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Frontiers of environmental science & engineering 2024年第8期18卷 117-132页

作者： Jiacheng Li Qi Han Liqiu Zhang Li Feng Guihuan Liu Beijing Key Laboratory for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for Water Pollution Source Control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China center of Eco-compensation Chinese Academy of Environmental PlanningMinistry of Ecology of EnvironmentBeijing 100041China

The Chaobai River Basin,which is a crucial ecological barrier and primary water source area within the Beijing-Tianjin-Hebei region,possesses substantial ecological *** gross ecosystem product(GEP)in the Chaobai River Basin is a reflection of ecosystem conditions and quantifies nature’s contributions to humanity,which provides a basis for basin ecosystem service management and *** study investigated the spatiotemporal evolution of GEP in the upper Chaobai River Basin and explored the driving factors influencing GEP spatial *** patterns from 2005 to 2020 were analyzed,and GEP was calculated for 2005,2010,2015,and *** driving factors influencing GEP spatial differentiation were identified using the optimal parameter-based geographical detector(OPGD)*** key findings are as follows:(1)From 2005 to 2020,the main ecosystem types were forest,grassland,and *** areas experienced significant changes,and conversions mainly occurred among urban,water,grassland and agricultural ecosystems.(2)Temporally,the GEP in the basin increased from 2005 to 2020,with regulation services *** the county(district)scale,GEP exhibited a north-west-high and south-east-low pattern,showing spatial differences between per-unit-area GEP and county(district)GEP,while the spatial variations in per capita GEP and county(district)GEP were similar.(3)Differences in the spatial distribution of GEP were influenced by regional natural geographical and socioeconomic *** these factors,gross domestic product,population density,and land-use degree density contributed *** among different driving forces noticeably impacted GEP spatial *** findings underscore the necessity of incorporating factors such as population density and the intensity of land-use development into ecosystem management decision-making processes in the upper reaches of the Chaobai River *** policies

关键词： Ecosystem pattern Gross ecosystem product(GEP) Spatiotemporal evolution Optimal parameter-based geographical detector(OPGD) Chaobai River Basin

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On-surface synthesis and characterization of polyynic carbon chains

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National science Review 2024年第3期11卷 192-199页

作者： Wenze Gao Wei Zheng Luye Sun Faming Kang Zheng Zhou Wei Xu Interdisciplinary Materials research center School of Materials Science and Engineering Tongji University

Carbyne, an elusive sp-hybridized linear carbon allotrope, has fascinated chemists and physicists for decades. Due to its high chemical reactivity and extreme instability, carbyne was much less explored in contrast to the sp2-hybridized carbon allotropes such as graphene. Herein, we report the on-surface synthesis of polyynic carbon chains by demetallization of organometallic polyynes on the Au（111） surface;the longest one observed consists of ～60 alkyne units（120 carbon atoms）. The polyynic structure of carbon chains with alternating triple and single bonds was unambiguously revealed by bond-resolved atomic force microscopy. Moreover, an atomically precise polyyne, C14, was successfully produced via tip-induced dehalogenation and ring-opening of the decachloroanthracene molecule(C14Cl10) on a bilayer NaCl/Au（111） surface at 4.7 K, and a band gap of 5.8 eV was measured by scanning tunnelling spectroscopy,in a good agreement with the theoretical HOMO–LUMO gap（5.48 eV）.

关键词： polyyne scanning probe microscopy carbon allotrope on-surface synthesis organometallic polyyne

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Source apportionment and specific-source-site risk of quinolone antibiotics for effluent-receiving urban rivers and groundwater in a city, China

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Journal of environmental sciences 2024年第10期144卷 185-198页

作者： Yu Zhao Yuanmeng Song Lulu Zhang Bo Zhao Mengqi Lu Jiansheng Cui Wenzhong Tang State Key Laboratory of environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of ScienceBeijing 100085China College of Environment science and engineering Hebei University of Science and TechnologyShijiazhuang 050000China University of Chinese Academy of sciences Beijing 100049China

There is a large surface-groundwater exchange downstream ofwastewater treatment plants(WWTPs),and antibiotics upstream may influence sites downstream of ***,samples from 9 effluent-receiving urban rivers(ERURs)and 12 groundwater sites were collected in Shijiazhuang City in December 2020 and April *** ERURs,8 out of 13 target quinolone antibiotics(QNs)were detected,and the total concentration of QNs in December and April were 100.6-4,398 ng/L and 8.02–2,476 ng/L,*** groundwater,all target QNs were detected,and the total QNs concentration was 1.09–23.03 ng/L for December and 4.54–170.3 ng/L for *** distribution of QNs was dissimilar between ERURs and *** QN concentrations were weakly correlated with land use types in the *** results of a positive matrix factorization model(PMF)indicated four potential sources of QNs in both ERURs and groundwater,and WWTP effluents were the main source of *** December to April,the contribution of WWTP effluents and agricultural emissions increased,while livestock activities *** value decomposition(SVD)results showed that the spatial variation of most QNs was mainly contributed by sites downstream(7.09%-88.86%)of ***,a new method that combined the results of SVD and PMF was developed for a specific-source-site risk quotient(SRQ),and the SRQ for QNs was at high level,especially for the sites downstream of *** temporal variation,the SRQ for WWTP effluents,aquaculture,and agricultural emissions ***,in order to control the antibiotic pollution,more attention should be paid to WWTP effluents,aquaculture,and agricultural emission sources for the benefit of sites downstream of WWTPs.

关键词： Source apportionment Singular value decomposition Positive matrix factorization model Quinolone antibiotics(QNs) Specific-source-site risk quotient(SRQ) WWTP effluents

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Prediction model on hydrolysis kinetics of phthalate monoester:A density functional theory study

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Journal of environmental sciences 2024年第1期135卷 51-58页

作者： Tong Xu Jingwen Chen Deming Xia Weihao Tang Jiansheng Cui Chun Liu Shuangjiang Li College of environmental science and engineering Hebei University of Science and TechnologyShijiazhuang 050000China Key Laboratory of Industrial Ecology and environmental engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China National-Regional Joint engineering research center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China

As primary degradation products of phthalate esters,phthalate monoesters(MPEs)have been widely detected in various aquatic environments and drawn growing toxicological *** kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for ***,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory *** indicate that MPEs with leaving groups having p Kaof<10 prefer dissociative transition *** are more persistent than their parents,and their hydrolysis half-lives were calculated to vary from 3.4 min to 79.2 years(p H=7–9).A quantitative structure-activity relationship model was developed for predicting the hydrolysis kinetics *** was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis *** work may lay a theoretical foundation for better understanding the chemical process that governs MPE persistence in aquatic environments.

关键词： Phthalate monoesters Phthalate esters Hydrolysis Density functional theory Quantitative structure-activity relationship

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