塑料添加剂的环境迁移、毒性测试与风险筛查:进展与挑战
Environmental Migration, Toxicity Testing and Risk Screening for Plastic Additives:Advances and Challenges
-
摘要: 塑料和微塑料污染日益严峻,因此引发了对塑料添加剂释放现象的广泛关注,塑料添加剂在固废处置和回收过程中会大量向环境中释放。塑料添加剂种类繁多,功能多样,数量庞大,其复杂性使得其评估工作面临巨大挑战,尤其是目前塑料添加剂的风险评估工作尚未建立起完善的体系。本研究对现有塑料添加剂的释放迁移研究、毒性测试及风险预测方法进行梳理,并基于塑料添加剂在种类、功能、添加量、监管、数据可用性等方面对公开信息的塑料添加剂逐级筛查,最终从1万多种现有塑料添加剂中筛选出106种值得关注的未监管添加剂物质。然后综合以下4项危害性指标,包括基于QSAR模型预测的物质毒性作用方式和危害等级、各化学品机构评估的PBT/PMT性质(持久性、生物累积性、迁移性、毒性)、生态毒性数据可用性、是否纳入化学品未来评估计划(CoRAP,ECHA),使用毒理学优先指数(ToxPi)方法按照等权重计算综合得分并排序,通过层次聚类分析对其进行优先级分类,提出相应风险评估优先序和研究关注的建议。结果表明,这其中很多尚未监管的塑料添加剂物质的潜在生态风险可能被低估。最后,我们提出对微塑料未来的研究挑战应主要聚焦在填补危害数据缺口和技术方法空白,包括其迁移释放机制、环境转化、混合效应及对生态系统的潜在影响等方面。Abstract: Plastic and microplastic pollution have become increasingly severe, raising widespread concern, and specifically regarding the risk of the release of plastic additives (PAs). The disposal and recycling of plastic solid waste, particularly in landfill and incineration processes, result in the substantial release of PAs into the environment. These additives are predominantly discharged by wastewater treatment plants, and infiltrate the water environment through various processes such as atmospheric deposition, soil erosion, groundwater infiltration, and surface runoff. The leaching of PAs poses threats to aquatic organisms as these additives can persistently migrate through various biological carriers. Micro- and nano-plastics (MNPs), acting as carriers, also make key contributions to the continuous release and accumulation of PAs in aquatic environments. However, the extensive variety, functions, quantities and complex compositions of plastic additives present formidable challenges in their assessment. This study presented the state-of-the-art research on the environmental release and migration, toxicity testing and risk prediction methods of existing PAs, and screened the risk of typical currently unregulated PAs via a step-by-step workflow combining toxicological priority index (Tox Pi) framework. The public information of existing PAs was retrieved and screened step by step based on the factors such as type, function, additive proportion, regulation, data availability, and so on. Finally, 106 currently unregulated PAs of concern were selected for further risk evaluation. Then, four hazard variables were selected, including the mode of action and hazard classification level predicted by QSAR models, the PBT/PMT hazard (P-persistence, B-bioaccumulation, M-migration, T-toxicity), the ecotoxicity data availability (abundance of available toxicity data for aquatic organisms), as well as the hit count to be included in the community rolling action plan (CoRAP) by ECHA. Comprehensive scale-transformed scores of the variables were calculated and ranked via the framework of ToxPi. The 106 evaluated plastic additives were finally classified into five priority levels for risk assessment and three classifications for research concerns using hierarchical cluster analysis. The results suggested that the ecological risk of currently unregulated PAs might be underestimated. Due to the data gap of hazard (especially for ecotoxicity) and limitations in methodology, we proposed the challenges in the scientific research and risk management of PAs, including the mechanism of migration and transformation, the mixture effects, and potential threats on ecosystems.
-
-
Plastics Europe.Plastics:The facts 2022[R/OL].(2024-01-14)[2022-10-01].https://plasticseurope.org/ Napper I E,Thompson R C.Marine Plastic Pollution:Other than Microplastic[M].New York:Academic Press,2019:425-442 Reisser J,Slat B,Noble K,et al.The vertical distribution of buoyant plastics at sea:An observational study in theNorth Atlantic Gyre[J].Biogeosciences,2015,12(4):1249-1256 Obbard R W,Sadri S,Wong Y Q,et al.Global warmingreleases microplastic legacy frozen in Arctic Sea ice[J].Earth's Future,2014,2(6):315-320 Chea J D,Yenkie K M,Stanzione J F 3rd,et al.A genericscenario analysis of end-of-life plastic management:Chemical additives[J].Journal of Hazardous Materials,2023,441:129902 Beiras R,Tato T,López-Ibáñez S.A 2-Tier standardmethod to test the toxicity of microplastics in marine water using Paracentrotus lividus and Acartia clausi larvae[J].Environmental Toxicology and Chemistry,2019,38(3):630-637 Schrank I,Trotter B,Dummert J,et al.Effects of microplastic particles and leaching additive on the life historyand morphology of Daphnia magna[J].EnvironmentalPollution (Barking,Essex:1987),2019,255(Pt 2):113233 Bringer A,le Floch S,Kerstan A,et al.Coastal ecosysteminventory with characterization and identification of plastic contamination and additives from aquaculture materials[J].Marine Pollution Bulletin,2021,167:112286 Phillips R,Whelton A J,Eckelman M J.Incorporating usephase chemical leaching and water quality testing for lifecycle toxicity assessment of cross-linked polyethylene (PEX) piping[J].Science of the Total Environment,2021,782:146374 Zimmermann L,Bartosova Z,Braun K,et al.Plastic products leach chemicals that induce in vitro toxicity under realistic use conditions[J].Environmental Science&Technology,2021,55(17):11814-11823 Ternes T A,Joss A,Siegrist H.Peer reviewed:Scrutinizing pharmaceuticals and personal care products inwastewater treatment[J].Environmental Science&Technology,2004,38(20):392A-399A Liu Z N,Deng M J,Wu Q H,et al.Occurrence,seasonalvariation and environmental impact of phosphorus flameretardants in a large scale wastewater treatment plant[J].Environmental Science and Pollution Research International,2019,26(36):36333-36342 Fang W D,Peng Y,Muir D,et al.A critical review of synthetic chemicals in surface waters of the US,the EUand China[J].Environment International,2019,131:104994 Christensen P R,Scheuermann A M,Loeffler K E,et al.Closed-loop recycling of plastics enabled by dynamic covalent diketoenamine bonds[J].Nature Chemistry,2019,11(5):442-448 Hahladakis J N,Velis C A,Weber R,et al.An overview of chemical additives present in plastics:Migration,release,fate and environmental impact during their use,disposal and recycling[J].Journal of Hazardous Materials,2018,344:179-199 Lei C.Progress on release and migration of plastic additives to ecological environment[J].Acta Ecologica Sinica,2021,41(8):3315-3324 Brossa L,MarcéR M,Borrull F,et al.Occurrence of twenty-six endocrine-disrupting compounds in environmental water samples from Catalonia,Spain[J].Environmental Toxicology and Chemistry,2005,24(2):261-267 Fries E,Grewal T,Sühring R.Persistent,mobile,and toxic plastic additives in Canada:Properties and prioritization[J].Environmental Science Processes&Impacts,2022,24(10):1945-1956 Bolívar-Subirats G,Cortina-Puig M,Lacorte S.Multiresidue method for the determination of high production volume plastic additives in river waters[J].EnvironmentalScience and Pollution Research International,2020,27(33):41314-41325 Bolívar-Subirats G,Rivetti C,Cortina-Puig M,et al.Occurrence,toxicity and risk assessment of plastic additivesin Besos River,Spain[J].Chemosphere,2021,263:128022 Schiavo S,Oliviero M,Chiavarini S,et al.Adverse effects of oxo-degradable plastic leachates in freshwater environment[J].Environmental Science and Pollution ResearchInternational,2020,27(8):8586-8595 Law K L.Plastics in the marine environment[J].AnnualReview of Marine Science,2017,9:205-229 Song J,Na J,An D,et al.Role of benzophenone-3 additive in chronic toxicity of polyethylene microplastic fragments to Daphnia magna[J].The Science of the Total Environment,2021,800:149638 Lithner D,Larsson A,Dave G.Environmental and healthhazard ranking and assessment of plastic polymers basedon chemical composition[J].The Science of the Total Environment,2011,409(18):3309-3324 Mu X Y,Huang Y,Li J,et al.New insights into themechanism of phthalate-induced developmental effects[J].Environmental Pollution,2018,241:674-683 Singh B,Sharma N.Mechanistic implications of plasticdegradation[J].Polymer Degradation and Stability,2008,93(3):561-584 Al-Odaini N A,Shim W J,Han G M,et al.Enrichment of hexabromocyclododecanes in coastal sediments near aquaculture areas and a wastewater treatment plant in a semienclosed bay in South Korea[J].The Science of the TotalEnvironment,2015,505:290-298 Hermabessiere L,Dehaut A,Paul-Pont I,et al.Occurrence and effects of plastic additives on marine environments and organisms:A review[J].Chemosphere,2017,182:781-793 Huang W,Song B,Liang J,et al.Microplastics and associated contaminants in the aquatic environment:A reviewon their ecotoxicological effects,trophic transfer,and potential impacts to human health[J].Journal of HazardousMaterials,2021,405:124187 Liu W,Zhao Y Q,Shi Z Y,et al.Ecotoxicoproteomic assessment of microplastics and plastic additives in aquaticorganisms:A review[J].Comparative Biochemistry andPhysiology Part D,Genomics&Proteomics,2020,36:100713 Gallo F,Fossi C,Weber R,et al.Marine litter plastics andmicroplastics and their toxic chemicals components:Theneed for urgent preventive measures[J].EnvironmentalSciences Europe,2018,30(1):13 Guzzetti E,Sureda A,Tejada S,et al.Microplastic in marine organism:Environmental and toxicological effects[J].Environmental Toxicology and Pharmacology,2018,64:164-171 Kwon J H,Chang S,Hong S H,et al.Microplastics as avector of hydrophobic contaminants:Importance of hydrophobic additives[J].Integrated Environmental Assessment and Management,2017,13(3):494-499 Gunaalan K,Fabbri E,Capolupo M.The hidden threat of plastic leachates:A critical review on their impacts on aquatic organisms[J].Water Research,2020,184:116170 Brandsma S H,Leonards P E,Leslie H A,et al.Tracingorganophosphorus and brominated flame retardants andplasticizers in an estuarine food web[J].The Science of the Total Environment,2015,505:22-31 Batel A,Linti F,Scherer M,et al.Transfer of benzo[a]pyrene from microplastics to Artemia nauplii and further tozebrafish via a trophic food web experiment:CYP1A induction and visual tracking of persistent organic pollutants[J].Environmental Toxicology and Chemistry,2016,35(7):1656-1666 Di Renzo L,Mascilongo G,Berti M,et al.Potential impact of microplastics and additives on the health status of loggerhead turtles (Caretta caretta) stranded along theCentral Adriatic Coast[J].Water,Air,&Soil Pollution,2021,232(3):98 Eulaers I,Jaspers V L B,Halley D J,et al.Brominatedand phosphorus flame retardants in White-tailed EagleHaliaeetus albicilla nestlings:Bioaccumulation and associations with dietary proxies (δ13 C,δ15 N and δ34 S)[J].TheScience of the Total Environment,2014,478:48-57 Demirtepe H,Melymuk L,Codling G,et al.Targeted andsuspect screening of plasticizers in house dust to assesscumulative human exposure risk[J].The Science of theTotal Environment,2021,781:146667 Cox K D,Covernton G A,Davies H L,et al.Human consumption of microplastics[J].Environmental Science&Technology,2019,53(12):7068-7074 Akoueson F,Paul-Pont I,Tallec K,et al.Additives in polypropylene and polylactic acid food packaging:Chemicalanalysis and bioassays provide complementary tools forrisk assessment[J].The Science of the Total Environment,2023,857(Pt 2):159318 Fan P,Yu H,Xi B D,et al.A review on the occurrenceand influence of biodegradable microplastics in soil ecosystems:Are biodegradable plastics substitute or threat?[J].Environment International,2022,163:107244 Zimmermann L,Dombrowski A,Völker C,et al.Are bioplastics and plant-based materials safer than conventionalplastics?in vitro toxicity and chemical composition[J].Environment International,2020,145:106066 Kühn S,Booth A M,Sørensen L,et al.Transfer of additive chemicals from marine plastic debris to the stomachoil of northern fulmars[J].Frontiers in EnvironmentalScience,2020,8:138 Silviya E K,Varma S,Unnikrishnan G,et al.Compounding and Mixing of Polymers[M]//Sabu T,Yang W M.Advances in Polymer Processing:From Macro to NanoScales.Woodhead,2009:71-105 United States Environmental Protection Agency (USEPA).Use of additive in plastic compounding:Genericscenario for estimating occupational exposures and environmental releases (Draft)[R].Washington DC:US EPA,2014 Groh K J,Backhaus T,Carney-Almroth B,et al.Overview of known plastic packaging-associated chemicalsand their hazards[J].The Science of the Total Environment,2019,651(Pt 2):3253-3268 Ügdüler S,van Geem K M,Roosen M,et al.Challengesand opportunities of solvent-based additive extractionmethods for plastic recycling[J].Waste Management,2020,104:148-182 Carmen S.Microbial capability for the degradation of chemical additives present in petroleum-based plasticproducts:A review on current status and perspectives[J].Journal of Hazardous Materials,2021,402:123534 Guo J,Zhang J.The application and development of additives in plastic packaging material[J].China Plastics Industry,2010,38(5):8-11 Bridson J H,Gaugler E C,Smith D A,et al.Leaching andextraction of additives from plastic pollution to inform environmental risk:A multidisciplinary review of analyticalapproaches[J].Journal of Hazardous Materials,2021,414:125571 Cramer G M,Ford R A,Hall R L.Estimation of toxichazard:A decision tree approach[J].Food and CosmeticsToxicology,1978,16(3):255-276 Reingruber E,Himmelsbach M,Sauer C,et al.Identification of degradation products of antioxidants in polyolefinsby liquid chromatography combined with atmosphericpressure photoionisation mass spectrometry[J].PolymerDegradation and Stability,2010,95(5):740-745 Aurisano N,Weber R,Fantke P.Enabling a circular economy for chemicals in plastics[J].Current Opinion inGreen and Sustainable Chemistry,2021,31:100513 European Chemicals Agency (ECHA).Mapping exercise:Plastic additives initiative[R/OL].[2023-12-11].https://echa.europa.eu/mapping-exercise-plastic-additives-initiative Stales C A,Peterson D R,Parkerton T F,et al.The environmental fate of phthalate esters:A literature review[J].Chemosphere,199735(4):667-749 Du J,Li H X,Xu S D,et al.A review of organophosphorus flame retardants (OPFRs):Occurrence,bioaccumulation,toxicity,and organism exposure[J].EnvironmentalScience and Pollution Research International,2019,26(22):22126-22136 Tagatz M E,Plaia G R,Deans C H.Toxicity of dibutylphthalate-contaminated sediment to laboratory-and fieldcolonized estuarine benthic communities[J].Bulletin of Environmental Contamination and Toxicology,1986,37(1):141-150 Morris S,Allchin C R,Zegers B N,et al.Distribution andfate of HBCD and TBBPA brominated flame retardants inNorth Sea estuaries and aquatic food webs[J].Environmental Science&Technology,2004,38(21):5497-5504 United States Environmental Protection Agency (USEPA).Plastic additives initiative:Supplementary information on scope and methods[R].Washington DC:US EPA,2019 Kida M,Koszelnik P.Investigation of the presence andpossible migration from microplastics of phthalic acid esters and polycyclic aromatic hydrocarbons[J].Journal of Polymers and the Environment,2021,29(2):599-611 Ye X Y,Wang P Y,Wu Y C,et al.Microplastic acts as avector for contaminants:The release behavior of dibutylphthalate from polyvinyl chloride pipe fragments in waterphase[J].Environmental Science and Pollution ResearchInternational,2020,27(33):42082-42091 Luo H W,Li Y,Zhao Y Y,et al.Effects of accelerated aging on characteristics,leaching,and toxicity of commercial lead chromate pigmented microplastics[J].Environmental Pollution,2020,257:113475 Noyes P D,Haggard D E,Gonnerman G D,et al.Advanced morphological-behavioral test platform revealsneurodevelopmental defects in embryonic zebrafish exposed to comprehensive suite of halogenated and organophosphate flame retardants[J].Toxicological Sciences:An Official Journal of the Society of Toxicology,2015,145(1):177-195 Li J,Xu Y,Li N,et al.Thyroid hormone disruption by organophosphate esters is mediated by nuclear/membranethyroid hormone receptors:In vitro,in vivo,and in silicostudies[J].Environmental Science&Technology,2022,56(7):4241-4250 Lu L P,Zhan T J,Ma M,et al.Thyroid disruption by bisphenol S analogues via thyroid hormone receptor β:invitro,in vivo,and molecular dynamics simulation study[J].Environmental Science&Technology,2018,52(11):6617-6625 Tan H Y,Zhang R,Chen Q C,et al.Computational toxicology studies on the interactions between environmentalcontaminants and biomacromolecules[J].Chinese ScienceBulletin,2022,67:4180-4191 Jeong J,Choi J.Development of AOP relevant to microplastics based on toxicity mechanisms of chemical additives using ToxCastTM and deep learning models combined approach[J].Environment International,2020,137:105557 Qiu S Q,Huang G Y,Fang G Z,et al.Chemical characteristics and toxicological effects of leachates from plasticsunder simulated seawater and fish digest[J].Water Research,2022,209:117892 郭上,陈光仕,周静,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱非靶向筛查生物消化液浸滤作用下塑料制品中添加剂的释放[J].分析化学,2022,50(9):1373-1383 Guo S,Chen G S,Zhou J,et al.Non-target screening of plastic additives leaching under artificial biodigestive condition using ultra-high performance liquid chromatography coupled with quadrupole-orbitrap mass spectrometry[J].Chinese Journal of Analytical Chemistry,2022,50(9):1373-1383(in Chinese)
Skjevrak I,Brede C,Steffensen I L,et al.Non-targetedmulti-component analytical surveillance of plastic foodcontact materials:Identification of substances not includedin EU positive lists and their risk assessment[J].FoodAdditives and Contaminants,2005,22(10):1012-1022 Campanale C,Dierkes G,Massarelli C,et al.A relevantscreening of organic contaminants present on freshwaterand pre-production microplastics[J].Toxics,2020,8(4):100 Tian L,Zheng J Y,Goodyer C G,et al.Non-targetedscreening of plastic-related chemicals in food collected inMontreal,Canada[J].Food Chemistry,2020,326:126942 Kim H S,Lee Y J,Koo Y J,et al.Migration of monomers,plastic additives,and non-intentionally added substances from food utensils made of melamine-formaldehyde resin following ultraviolet sterilization[J].FoodControl,2021,125:107981 黎梓城,吴学峰,董犇,等.超高效液相色谱-四极杆飞行时间质谱法同时测定食品接触用塑料中50种添加剂的迁移量[J].分析测试学报,2022,41(6):903-909 Li Z C,Wu X F,Dong B,et al.Determination of migration of 50 additives in food contact plastics by ultra-performance liquid chromatography-quadrupole time-offlight mass spectrometry[J].Journal of Instrumental Analysis,2022,41(6):903-909(in Chinese)
Lestido-Cardama A,Barbosa-Pereira L,Sendón R,et al.Migration of dihydroxy alkylamines and their possibleimpurities from packaging into foods and food simulants:Analysis and safety evaluation[J].Polymers,2023,15(12):2656 Sapozhnikova Y, Nuñez A, Retired J J. Screening of chemicals migrating from plastic food contact materialsfor oven and microwave applications by liquid and gaschromatography-Orbitrap mass spectrometry[J]. Journal of Chromatography A, 2021, 1651:462261 Chen Q Q, Santos M M D, Tanabe P, et al. Bioassayguided analysis coupled with non-target chemical screening in polyethylene plastic shopping bag fragments afterexposure to simulated gastric juice of fish[J]. Journal of Hazardous Materials, 2021, 401:123421 Groh K J, Carney-Almroth B, Geueke B, et al. Database of chemicals associated with plastic packaging (CPPDB)[R/OL].[2023-12-11]. https://comptox.US EPA.gov/dashboard/chemical-lists/cppdblista. 2018. 10. 5281/zenodo.2658143 Aurisano N, Huang L, Milà i Canals L, et al. Chemicals of emerging concern (CECs) in plastic toys[J]. Environment International, 2021, 146:106194 United States Environmental Protection Agency (USEPA). Plastic map:Chemicals related to polymers[R/OL].[2023-12-11]. https://comptox. US EPA. gov/dashboard/chemical-lists/PLASTICMAP.2023 Wiesinger H, Wang Z Y, Hellweg S. Deep dive into plastic monomers, additives, and processing aids[J]. Environmental Science&Technology, 2021, 55(13):9339-9351 Verhaar H J M, Hermens J L M. Classifying environmental pollutants. 1:Structure-activity relationships for prediction of aquatic toxicity[J]. Chemosphere, 1992, 25(4):471-491 Verhaar H J M, Speksnijder J, Van Leeuwen C J, et al.Classifying environmental pollutants:Part 3. External validation of the classification system[J]. Chemosphere,2000, 40:875-883 Kienzler A, Bopp S, Halder M, et al. Application of newstatistical distribution approaches for environmental mixture risk assessment:A case study[J]. The Science of theTotal Environment, 2019, 693:133510 European Chemicals Agency (ECHA). PBT assessmentlist[R/OL].[2023-12-11]. https://echa.europa.eu/pbt_p_p_id=disslists_WAR_disslistsportlet&p_p_lifecycle=1&p_p_state=normal&p_p_mode=view&_disslists_WAR_disslistsportlet_javax.portlet.action=searchDissLists. 2023 Federal Environment Agency Germany (UBA). UBAPMT[EB/OL].[2023-12-11]. https://www.umweltbundesamt. de/publikationen/reach-improvement-of-guidancemethods-for-the. European Chemicals Agency (ECHA). Substance evaluation-CoRAP[R/OL].[2023-12-11]. https://echa.europa.eu/information-on-chemicals/evaluation/community-rollingaction-plan/corap-table_p_p_id=disslists_WAR_disslistsportlet&p_p_lifecycle=1&p_p_state=normal&p_p_mode=view&_disslists_WAR_disslistsportlet_javax.portlet.action=searchDissLists.2023 Marvel S W, To K, Grimm F A, et al. ToxPi GraphicalUser Interface 2. 0:Dynamic exploration, visualization,and sharing of integrated data models[J]. BMC Bioinformatics, 2018, 19(1):80 Reif D M, Martin M T, Tan S W, et al. Endocrine profiling and prioritization of environmental chemicals usingToxCast data[J]. Environmental Health Perspectives,2010, 118(12):1714-1720 Cao M, Fan J P, Guo C S, et al. Comprehensive investigation and risk assessment of organic contaminants inYellow River Estuary using suspect and nontarget screening strategies[J]. Environment International, 2023, 173:107843 Feng X X, Sun H L, Liu X, et al. Occurrence and ecological impact of chemical mixtures in a semiclosed sea bysuspect screening analysis[J]. Environmental Science&Technology, 2022, 56(15):10681-10690 Kwan C S, Takada H. Release of Additives and Monomers from Plastic Wastes[M]//The Handbook of Environmental Chemistry. Cham:Springer International Publishing, 2016:51-70 Sridharan S, Kumar M, Saha M H, et al. The polymersand their additives in particulate plastics:What makesthem hazardous to the fauna?[J]. The Science of the TotalEnvironment, 2022, 824:153828 Menicagli V, Balestri E, Biale G, et al. Leached degradation products from beached microplastics:A potentialthreat to coastal dune plants[J]. Chemosphere, 2022, 303(Pt 3):135287 Bignardi C, Cavazza A, Laganà C, et al. UHPLC-highresolution mass spectrometry determination of bisphenolA and plastic additives released by polycarbonate tableware:Influence of ageing and surface damage[J]. Analytical and Bioanalytical Chemistry, 2015, 407(26):7917-7924 Tanaka K, Takada H, Yamashita R, et al. Facilitated leaching of additive-derived PBDEs from plastic by seabirds'stomach oil and accumulation in tissues[J]. Environmental Science&Technology, 2015, 49(19):11799-11807 Lithner D, Nordensvan I, Dave G. Comparative acute toxicity of leachates from plastic products made of polypropylene, polyethylene, PVC, acrylonitrile-butadiene-styrene, and epoxy to Daphnia magna[J]. EnvironmentalScience and Pollution Research International, 2012, 19(5):1763-1772 -
仁和网刊-华英迪-20231211002-附表1.docx
-
![WeChat](http://eekw.rcees.ac.cn//eekw-data/stdlxb/2024/2/PIC/wechat_cn5b8870f1-20b2-4867-992a-329aa7409dd8.jpg)
计量
- 文章访问数: 653
- HTML全文浏览数: 653
- PDF下载数: 190
- 施引文献: 0