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Legacy and emerging per-and polyfluoroalkyl substances(PFAS) in the atmosphere: A comprehensive review

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science China Technological sciences 2024年第10期67卷 3032-3050页

作者： QIAO BiTing SONG DongBao CHEN Hao YAO YiMing SUN HongWen MOE Key laboratory of Pollution Processes and environmental Criteria College of Environmental Science and EngineeringNankai University

With long-term production and widespread application, per-and polyfluoroalkyl substances(PFAS) have been detected in various media worldwide, including the atmosphere. Since the gradual restriction and phase-out of C8perfluoroalkyl acids(PFAAs), environmental contamination by emerging PFAS substitutes such as short-chain PFAA homologues, perfluoroether carboxylic, and sulfonic acids has been reported. Although there has been extensive monitoring of emerging PFAS substitutes in the aquatic environment, few studies have conducted target analysis and nontarget screening(NTS) of emerging unknown PFAS in the atmosphere over the past decade. To fill the gap, this review focused on emerging PFAS in the atmosphere in addition to legacy PFAS. The reported sampling, pretreatment, and instrumental analysis methods for target analysis and NTS of both neutral and ionic PFAS in the atmosphere are summarized, along with the advantages and current limitations of different sampling and NTS methods for PFAS in the atmosphere. The global levels, composition, and spatiotemporal distribution characteristics of legacy and emerging PFAS in the atmosphere are summarized and their transport, transformation, and dry/wet deposition are elucidated. The review highlights the importance of developing and applying the all-in-one strategy integrating target, suspect screening, and NTS to gain insights into emerging PFAS in the atmosphere and provide a reference for future research.

关键词： emerging PFAS atmosphere nontarget screening spatiotemporal distribution fate

Peracetic acid catalytic activation using Co3O4 nanocluster decorated graphitic carbon nitride for cefapirin degradation in water

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science China Technological sciences 2024年第10期67卷 3103-3115页

作者： YIN ShiMei GAO YiXuan CHEN Long LI Fan LIU XiaoNa QI Fei LIU Wen Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry University Key laboratory of Water and Sediment sciences (Ministry of Education) College of Environmental Sciences and EngineeringPeking University School of environmental science and Engineering Taiyuan University of Technology State environmental Protection Key laboratory of All Material Fluxes in River Ecosystems Peking University Beijing National laboratory for molecular sciences Peking University

This study innovated cobalt-based catalytic nanocomposites（CCNs） for the heterogeneous activation of peracetic acid（PAA）,a green and efficient advanced oxidation process for removing antibiotics from *** Co3O4catalysts exhibit limited activity due to stable electronic *** overcome this,CCNs were synthesized using a one-step condensation method,incorporating a size control strategy that anchors Co3O4nanoclusters within 4-5 nm onto six-fold cavity of g-C3N4,simultaneously modifying the coordination environment of *** alteration significantly enhances the adsorption energy of PAA and catalytic activity compared to commercial *** improved performance of CCN2,in particular,is attributed to a shift in the cobalt d band center towards the Fermi level,facilitating electron delocalization and transfer,enhancing Co-O bonding,and accelerating PAA ***2's superior activity,with a cefapirin（CFP） degradation kinetic rate constant(k1=0.760 min-1)～11 times that of PAA direct oxidation(k1=0.070 min-1) and～5 times that of commercial Co3O4/PAA system(k1=0.164 min-1),is due to its ability to generate dominant reactive species for antibiotic degradation,including alkoxy radicals(CH3C（=O）OO·),high valence metal(CoⅣ（=O）2+),and singlet oxygen（1O2）,with the latter two being crucial for the degradation *** degradation of CFP involved three mechanisms,including direct oxidation by PAA,decarboxylation,and open-ring reactions at nitrogen *** research provides insights into developing high-activity catalysts for efficient PAA activation and antibiotic removal,leveraging the strategy of shifting the transition metal d band center.

关键词： peracetic acid Co3O4 nanocluster high valence metal singlet oxygen cefapirin

Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan MOE Key laboratory of Pollution Processes and environmental Criteria/Tianjin Key laboratory of environmental Remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen ***,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major ***,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/*** feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom *** article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting *** article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

Catalytic recycling of polyesters via a binuclear catalyst

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science China Chemistry 2024年第2期67卷 426-427页

作者： Bo Sun Ding Ma Beijing National laboratory for molecular science New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

Plastics play a crucial role in modern society life. While the increasing use of plastics and rapid accumulation of plastic waste in nature environment have caused severe environmental crisis and the waste of carbon resources. Catalytic upcycling is a promising approach to transform plastic waste into high value-added chemicals to achieve a sustainable circular economy.

关键词： Catalytic polyester catalyst

Capturing metal clusters at the strong-interaction region to reverse Ostwald ripening

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science China Materials 2024年第4期67卷 1363-1364页

作者： Shuheng Tian Ding Ma Beijing National laboratory for molecular sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

High-temperature interactions induce sintering of metal nanoparticles(NPs) on heterogeneous catalyst surfaces, leading to reduced surface area and active site loss through Ostwald ripening [1]. This irreversible deactivation necessitates costly catalyst replacement, notably impacting metals like copper in hydrogenation and reforming reactions [2].

关键词： catalyst reforming irreversible

Lake microbiome composition determines community adaptability to warming perturbations

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Ecological Processes 2024年第2期13卷 177-191页

作者： Xiaotong Wu Qixing Zhou Hui Zeng Xiangang Hu Key laboratory of Pollution Processes and environmental Criteria (Ministry of Education) Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering Nankai University

Background Microbial communities are crucial for ecosystems. A central goal of microbial ecological research is to simplify the biodiversity in natural environments and quantify the functional roles to explore how the ecosystems respond under different environmental conditions. However, the research on the stability and dynamics of lake microbes in response to repeated warming stress is *** To exclude confounding environmental factors, we conducted a 20-day repeated warming simulation experiment to examine the composition and function dynamics of lake microbial *** Experimental warming significantly altered the community structure of bacteria instead of fungi. Microbial community structure, together with microbial biomass, jointly regulated the function of microbial communities. The plummeting of aerobic denitrifiers Pseudomonadaceae decreased by 99%(P < 0.001) after high temperature, leading to reduced microbial nitrogen metabolism on nitrogen respiration and nitrate respiration. Under warming conditions, the microbial community with higher adaptability showed more positive correlations and less competitive relationships in co-occurrence networks to acclimate to *** Microbiome composition controlled carbon and nitrogen metabolism, thus determining lake microbial communities' adaptability to heat stress. This study extended our insights on the lake microbial community response and adaptability under warming drivers.

关键词： Temperature environmental stress Bacteria Fungi Freshwater ecosystem

Colloid-facilitated release of polybrominated diphenyl ethers at an e-waste recycling site: evidence from undisturbed soil core leaching experiments

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Frontiers of environmental science & Engineering 2024年第2期18卷 91-101页

作者： Zebin Huo Mengjun Xi Lianrui Xu Chuanjia Jiang Wei Chen College of environmental science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300350China

Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.

关键词： Polybrominated diphenyl ether Colloid-facilitated transport E-waste recycling site Undisturbed soil core Groundwater quality

Abiotic transformation of chlorinated organics at the active surface of iron-bearing minerals in soils and sediments

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science China Technological sciences 2024年第10期67卷 2991-3008页

作者： LI XuXin YAN Chen ZENG YuXi LI WenBin PENG TianWei SONG Biao ZHOU ChengYun College of environmental science and Engineering Hunan University Key laboratory of environmental Biology and Pollution Control (Hunan University) Ministry of Education

Chlorinated organic compounds are emerging pollutants of widespread concern because of their toxicity, bioaccumulation,persistence, and lack of adequate regulatory measures. Their abiotic transformation, facilitated by iron-bearing minerals, is critical to their natural dissipation in soils and sediments. However, further exploration is needed to understand their underlying mechanisms and potential engineering applications under different redox conditions. This paper reviews the abiotic transformation behaviors and mechanisms of chlorinated organics at the active surface of iron-bearing minerals under anoxic and oxic conditions and summarizes the strategies for enhancing the abiotic transformation efficiency of chlorinated organics. The abiotic transformation rate under oxic conditions can be a few orders of magnitude higher than that under anoxic conditions. Under anoxic conditions, chlorinated organics undergo reductive dechlorination through reductive elimination, hydrogenolysis, dehydrohalogenation, and nucleophilic substitution. A close relationship between the abiotic transformation of chlorinated organics and the production of hydroxyl radicals by iron-bearing minerals under oxic conditions was discovered. Synthetic active iron-bearing minerals, carbonaceous materials, and biological synergy can facilitate abiotic dechlorination under anoxic conditions. Meanwhile, the regulation of redox conditions, the introduction of ligands, and the utilization of coexisting anions are proposed to enhance oxidative degradation. This study is expected to improve the comprehension of the abiotic degradation of chlorinated organics mediated by iron-bearing minerals and provide the theoretical foundation for developing new approaches aimed at addressing chlorinated organic pollution.

关键词： chlorinated organic compounds iron-bearing minerals dechlorination degradation remediation

Structural insights into the Oryza sativa cation transporters HKTs in salt tolerance

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Journal of Integrative Plant Biology 2024年第4期66卷 700-708页

作者： Ran Gao Yutian Jia Xia Xu Peng Fu Jiaqi Zhou Guanghui Yang State Key laboratory of Plant environmental Resilience Frontiers Science Center for Molecular Design BreedingCollege of Biological SciencesChina Agricultural UniversityBeijing 100193China

The high-affinity potassium transporters(HKTs),selectively permeable to either Na^(+)alone or Na^(+)/K^(+),play pivotal roles in maintaining plant Na^(+)/K^(+)*** their involvement in salt tolerance is widely reported,the molecular underpinnings of Oryza sativa HKTs remain *** this study,we elucidate the structures of OsHKT1;1 and OsHKT2;1,representing two distinct classes of rice *** dimeric assembled OsHKTs can be structurally divided into four *** the dimer interface,a half-helix or a loop in the third domain is coordinated by the C-terminal region of the opposite ***,we present the structures of OsHKT1;5 salt-tolerant and salt-sensitive variants,a key quantitative trait locus associated with salt *** salt-tolerant variant of OsHKT1;5 exhibits enhanced Na^(+)transport capability and displays a more flexible *** findings shed light on the molecular basis of rice HKTs and provide insights into their role in salt tolerance.

关键词： HKT salt-tolerant structure