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Facile synthesis of azobenzene-embedded conjugated macrocycles for optically switchable single-crystal transistors and tunable supramolecular assemblies

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Aggregate 2023年第6期4卷 101-109页

作者： Dongdong Chang Xuetao Xiao Dongyue An Rong Zhang Xianyu Song Yunqi Liu Yan Zhao Xuefeng Lu Department of Materials Science State Key Laboratory of Molecular Engineering of PolymersFudan UniversityShanghaiChina Key Laboratory of Water Environment Evolution and Pollution Control in Three Gorges Reservoir School of Environmental and Chemical EngineeringChongqing Three Gorges UniversityChongqingChina

A series of newπ-conjugated macrocycles(AzoM-n-E,n 1–3)incorporating=azobenzene units have been synthesized by a facile strategy in one-pot *** resultant azobenzene-embedded macrocycles feature intrinsic photoresponsive behaviors and intriguing supramolecular assembling *** smallest macro-cycle AzoM-1-E with a rigid planar conjugated backbone structure is used to prepare the single crystal transistors,showing reversible optical *** moderate size macrocycle AzoM-2-E assembles into a dimer in the form of interpenetration throughπ-πstacking between azobenzene *** largest macrocycle AzoM-3-E with enhancedﬂexibility can adaptively assemble with various types of electron-deﬁcient guests accompanied by distortion of ***,AzoM-3-E assembles with the planar F4-TCNQ to form a tetragonal geometry by C-F⋅⋅⋅π and π-π interactions,while the assembly with ellipsoidal C70 viaπ-πinteractions induces AzoM-3-E to form a boat-shaped *** work will shed new light on the development of functional conjugated macrocycles in organic electronics.

关键词： azobenzene conjugated macrocycle host-guest interaction photoresponsive transistors supramolecular assembly

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Honeycomb-like biochar framework coupled with Fe_(3)O_(4)/FeS nanoparticles as efficient heterogeneous Fenton catalyst for phenol degradation

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Journal of environmental Sciences 2024年第2期36卷 390-399页

作者： Aihua Cheng Yi He Xiaohe Liu Chi He Department of Environmental Engineering College of Geology and EnvironmentXi’an University of Science and TechnologyXi’an 710054China State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi’an Jiaotong UniversityXi’an 710049China National Engineering Laboratory for VOCs Pollution Control Material and Technology University of Chinese Academy of SciencesBeijing 101408China

Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater ***,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by *** prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the ***,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation ***,biochar can effectively promote cycling stability by limiting Fe *** work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.

关键词： Biomass Biochar Fenton reaction Fe_(3)O_(4)/FeS(Fe/S) Phenol degradation

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Drivers of microbial beta-diversity in wastewater treatment plants in China

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Journal of environmental Sciences 2022年第5期34卷 341-349页

作者： Bing Zhang Ting Yang Chenxiang Sun Xianghua Wen College of Life and Environmental Sciences Minzu University of ChinaBeijing 100081China Environmental Simulation and Pollution Control State Key Joint Laboratory School of EnvironmentTsinghua UniversityBeijing 100084China

As one of the most well-documented biogeographic patterns,the distance-decay relation-ship provides insights into the underlying mechanisms driving biodiversity ***-though wastewater treatment plants(WWTPs)are well-controlled engineered ecosystems,this pattern has been seen among microbial communities in activated sludge(AS).However,little is known about the relative importance of environmental heterogeneity and dispersal limitation in shaping AS microbial community across China;especially they are related to spatial scale and organism ***,we assessed the distance-decay relationship based on different spatial scales and microbial phylogenetic groups by analyzing 132 activated sludge(AS)samples across China comprising 3,379,20016S rRNA *** results in-dicated that the drivers of distance-decay pattern in China were *** biogeographic patterns in WWTPs were mainly driven by dispersal limitation at both local and national *** contrast,conductivity,SRT,and pH played dominant roles in shaping AS microbial community compositions at the regional *** rates and the drivers of beta-diversity also varied with microorganism ***,a quantitative re-lationship between dispersal limitation ratio and AS microbial turnover rate was ***,these results highlighted the importance of considering multiple spatial scales and micro-organism types for understanding microbial biogeography in WWTPs and pro-vided new insights into predicting variations in AS community structure in response to environmental disturbance.

关键词： Wastewater treatment plant Distance-decay pattern Scale-dependent Microbial assembly Dispersal limitation

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New mechanism of FA in composted sludge inducing Cu fixation on Albite in open-pit mine soil

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Journal of environmental Sciences 2022年第6期34卷 142-150页

作者： Jiapeng Wan Yifan Zeng Mei Wang Bin Dong Zuxin Xu State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China YANGTZE Eco-Environment Engineering Research Center China Three Gorges CorporationBeijing 100038China Shanghai Investigation Design&Research Institute Co.Ltd Shanghai 200335China

Fulvic acid(FA),typical organic matter derived from humification process in composted sludge,possesses the potential to remediate mine soils contaminated by heavy *** understand the cooper(Cu)immobilizing process in open-pit mine soil induced by FA,changes of Cu speciation in mixture of open-pit mine soil and composted sludge was tracked over 180 *** was observed that the organic-bound and residual fraction of Cu increased dramatically with the corresponding decrease of Fe/Mn oxide-bound Cu in the first 60 days,then the organic-bound fraction decreased to about its initial proportion during 60-120 days,while residual fraction still increased,and the proportion of residual Cu accounted for over85%and became stable after 120 *** reveal the mechanism of FA inducing Cu fixation on Albite which is the main phase of soil primary ore,two groups of Cu adsorption experiments with and without FA were *** the addition of FA,the adsorption capacity of Cu by Albite increased by 1.55 times and the content of residual Cu in Albite increased by7.7 *** was found that the Cu absorbed in smaller Albite particle induced by FA formed a secondary mineral——Chrysocolla,causing increase of residual fraction of *** results revealed the mechanism:FA was absorbed on the surface of Albite after complexing with Cu ions in the solution,and then it induced Cu into the interlayer and pore channels of *** Cu in the Albite was immobilized by forming Chrysocolla finally.

关键词： Fulvic acid Composted sludge Heavy metal Open-pit mine Mineralization

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Pumping and sliding of droplets steered by a hydrogel pattern for atmospheric water harvesting

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National Science Review 2023年第12期10卷 181-192页

作者： Wei Zhang Qinghua Ji Gong Zhang Zhenao Gu Haozhi Wang Chengzhi Hu Huijuan Liu Zhiyong Jason Ren Jiuhui Qu Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of Environment Tsinghua University Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences University of Chinese Academy of Sciences Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) School of Materials Science and EngineeringTianjin University Department of Civil and Environmental Engineering and Andlinger Center for Energy and the Environment Princeton University

Atmospheric water harvesting is an emerging strategy for decentralized and potable water supplies. However,water nucleation and microdroplet coalescence on condensing surfaces often result in surface flooding owing to the lack of a sufficient directional driving force for shedding. Herein, inspired by the fascinating properties of lizards and catfish, we present a condensing surface with engineered hydrogel patterns that enable rapid and sustainable water harvesting through the directional pumping and drag-reduced sliding of water droplets. The movement of microscale condensed droplets is synergistically driven by the surface energy gradient and difference in Laplace pressure induced by the arch hydrogel patterns. Meanwhile, the superhydrophilic hydrogel surface can strongly bond inner-layer water molecules to form a lubricant film that reduces drag and facilitates the sliding of droplets off the condensing surface. Thus, this strategy is promising for various water purification techniques based on liquid–vapor phase-change processes.

关键词： atmospheric water harvesting droplet manipulation bio-inspired condensation

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Comparative study of raw and HNO_(3)-modified porous carbon from waste printed circuit boards for sulfadiazine adsorption: Experiment and DFT study

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Chinese Chemical Letters 2023年第7期34卷 256-259页

作者： Yujiao Kan Ruxin Zhang Xing Xu Bo Wei Yanan Shang School of Safety and Environmental Engineering Shandong University of Science and TechnologyQingdao 266590China Faculty of Light Industry Qilu University of Technology(Shandong Academy of Sciences)Ji'nan 250353China Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Environment Research Institute ShandongUniversityQingdao266237China

A huge amount of waste printed circuit boards(WPCBs) was produced while the electronic manufacturing industry developed rapidly. WPCBs mainly consist of organic compounds, which makes it possible to prepare them into porous carbon as valuable adsorbent. However, WPCBs are also rich in valuable *** makes up the most of these metals. It is worth studying whether the residual metal will affect the application of carbon materials. In this study, the porous active carbon(AC) was prepared from WPCBs as an adsorbent. Sulfadiazine(SD), a widely detected antibiotic contaminant, was used as a target *** acid(HNO_(3)) was used to modify AC(AC-HNO_(3)) to remove the residual Cu. The experiment results showed that the adsorption kinetics of SD by AC(k = 0.0025) and AC-HNO_(3)(k = 0.0029) can be described better using a pseudo-second-order kinetic equation. The adsorption isotherms of AC and AC-HNO_(3) on SD could be fitted by the Langmuir model. AC had a larger adsorption capacity than AC-HNO_(3). Density functional theory(DFT) calculation results suggested that the-OH group and Cu on the surface of AC could be the adsorption sites and promote the SD adsorption. This work provides practical methods to recycle WPCBs into wealth and realized waste control by waste.

关键词： WPCBs DFT Sulfadiazine Porous carbon

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Facile low-temperature supercritical carbonization method to prepare high-loading nickel single atom catalysts for efficient photodegradation of tetracycline

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Journal of environmental Sciences 2024年第4期36卷 373-384页

作者： Han Qiao Lirong Zheng Shiwen Hu Gang Tang Hongri Suo Chongxuan Liu School of Environment Harbin Institute of TechnologyHarbin 150090China State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China Beijing Synchrotron Radiation Facility(BSRF) Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

environmental photocatalysis is a promising technology for treating antibiotics in *** this study,a supercritical carbonization method was developed to synthesize a single-atom photocatalyst with a high loading of Ni(above 5 wt.%)anchored on a carbonnitrogen-silicate substrate for the efficient photodegradation of a ubiquitous environmental contaminant of tetracycline(TC).The photocatalyst was prepared from an easily obtained metal-biopolymer-inorganic supramolecular hydrogel,followed by supercritical drying and carbonization *** low-temperature(300℃)supercritical ethanol treatment prevents the excessive structural degradation of hydrogel and greatly reduces the metal clustering and aggregation,which contributed to the high Ni *** characterizations confirmed that Ni was present at isolated sites and stabilized by Ni-N and Ni-O bonds in a Ni-(N/O)_(6)-C/SiC configuration.A 5%Ni-C-Si catalyst,which performed the best among the studied catalysts,exhibited a wide visible light response with a narrow bandgap of 1.45 eV that could efficiently and repeatedly catalyze the oxidation of TC with a conversion rate of almost 100% within 40 *** reactive species trapping experiments and electron spin resonance(ESR)tests demonstrated that the h+,and·O_(2)-were mainly responsible for TC *** TC degradation mechanism and possible reaction pathways were provided ***,this study proposed a novel strategy to synthesize a high metal loading singleatom photocatalyst that can efficiently remove TC with high concentrations,and this strategy might be extended for synthesis of other carbon-based single-atom catalysts with valuable properties.

关键词： Carbon-based single-atom catalyst Nickel Photocatalytic degradation Tetracycline Visible light

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Mesoporous molecular sieve-based materials for catalytic oxidation of VOC: A review

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Journal of environmental Sciences 2023年第3期35卷 112-134页

作者： Wei Gao Xiaolong Tang Honghong Yi Shanxue Jiang Qingjun Yu Xizhou Xie Ruijie Zhuang Department of Environmental Science and Engineering School of Energy and Environmental EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Environmental Protection Key Laboratory of Food Chain Pollution Control Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also *** review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.

关键词： Volatile organic compound Mesoporous molecular sieves Supported catalyst Catalytic oxidation Reaction mechanism Influencing factors

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Challenging the contamination of per- and polyfluoroalkyl substances in water: advanced oxidation or reduction?

Environmental Functional Materials

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environmental Functional Materials 2022年第3期1卷 325-337页

作者： Zhanghao Chen Xinhao Wang Ruochen Dong Yutong Zhang Xin Jin Cheng Gu State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing 210023 PR China

Nowadays, the increasing discharge of persistent per- and polyfluoroalkyl substances (PFASs) caused serious environmental issues. In addition to advanced oxidation processes (AOPs), advanced reduction processes (ARPs) based on reducing radicals, e.g., hydrated electron and superoxide anions have attracted great attentions as promising methods for remediation of PFASs pollution. This review, based on 128 cited references, provides a critical overview on the performance of different AOPs and ARPs. The unique properties of reactive species, e.g., SO 4 •- and e aq − and their generation mechanisms in different systems were discussed. Moreover, the efficiencies of different systems were further compared from several aspects, e.g., PFASs decomposition rate, reaction time and energy consumption. More specially, for some model compounds of PFASs, such as perfluorooctanoic acid, perfluorooctane sulfonate and perfluoroalkyl ether carboxylic acids, we systematically discussed their degradation and defluorination pathways in both AOPs and ARPs. The reported literatures showed that the degradation pathways of these PFASs are closely related to their head groups in either AOPs or ARPs. Finally, some key conclusions were summarized, and the implications of the state-of-the-art knowledge on practical PFASs remediation in water treatments were summarized and the future priority research directions were proposed.

关键词： Advanced oxidation processes Advanced reduction processes Polyfluoroalkyl substances Degradation mechanism

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Characterization and source apportionment of pharmaceuticals in surface water of the Yangtze Estuary and adjacent sea

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environmental Science and pollution Research 2024年第39期31卷 52171-52180页

作者： Chen, Chunzhao Tang, Jian Li, Fei Xue, Rui Xiao, Yihua Chen, Ling Yu, Gang Advanced Interdisciplinary Institute of Environment and Ecology Beijing Normal University Zhuhai519087 China Department of Chemistry and Environmental Science New Jersey Institute of Technology NJ United States Institute of Science and Technology Information Beijing Academy of Science and Technology Beijing100089 China School of Environmental and Municipal Engineering Qingdao University of Technology Qingdao266520 China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China

Pharmaceuticals, which are closely linked to human activities, have attracted global attention. This study investigated the occurrence characteristics of 20 pharmaceuticals in surface water of the Yangtze Estuary and adjacent sea. A total of 14 targeted pharmaceuticals were detected in both spring and summer sampling campaigns. The mean concentrations of sulfonamides and non-sulfonamides were 36.60 ± 19.43 ng·L−1 and 50.02 ± 41.07 ng·L−1, respectively. As for non-antibiotics, their concentrations were in the range of 24.34 ± 916.8 ng·L−1 with caffeine accounting for 6.17 ~ 86.70% (average percentage of 42.22%). Meanwhile, spatial distribution patterns showed similarities between antibiotics and non-antibiotics, with high levels occurring near the upper estuary, aquaculture areas, wastewater treatment plants, and the maximum turbidity zone. This phenomenon could be related to the sources of pharmaceuticals and the physicochemical properties of water bodies. Obviously, the first three areas are highly impacted by human activities or serve as important sources of terrestrial contaminants entering the East China Sea. The last area retains high amounts of suspended particles which may exert strong trapping effects on hydrophobic chemicals. Principal component analysis revealed the presence of three potential sources for pharmaceuticals in the Yangtze Estuary, with a relatively high percentage originating from incompletely treated municipal sewage. As for the temporal trend, pharmaceutical contamination was found to be higher in spring compared to summer, potentially due to variations in pharmaceutical consumption patterns, local rainfalls, and water temperatures. These findings provide fundamental data support for implementing appropriate local management strategies for pharmaceutical usages. © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2024.

关键词： Antibiotics

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