Mishonga yezvipembenene muhova iri kuramba ichinetsa pasi rose, asi pane ruzivo rushoma pamusoro pekuchengetedzeka kwezvipenyu zvemumvura.Muchiyedzo chemazuva makumi matatu chemesocosmic, zvipembenene zvemumvura zvinonzi benthic invertebrates zvakafumurwa kune yakajairika insecticide fipronil nemhando ina dzezvigadzirwa zvinosvibisa.Iyo fipronil compound yakakonzera shanduko mukubuda uye trophic cascade.Iyo inoshanda yekuisa (EC50) iyo fipronil uye sulfide yayo, sulfone uye desulfinyl degradation zvigadzirwa zvinokonzeresa 50% mhinduro yakagadzirwa.Mitero haina hanya ne fipronil.Iyo njodzi yekumisikidzwa kwe5% yemhando dzakakanganisika kubva gumi neshanu mesocosmic EC50 kukosha inoshandiswa kushandura kusanganiswa kwefipronil mumunda sampuro kuita huwandu hwehupfu hwezvikamu (∑TUFipronils).Muchikamu che16% chehova dzakatorwa kubva muzvidzidzo zvishanu zvedunhu, avhareji ∑TUFipronil yakapfuura 1 (ichiratidza huturu).Invertebrate zviratidzo zvezvipenyu zviri panjodzi zvakabatana zvisina kunaka neTUTUipronil mune ina yenzvimbo shanu dzesampling.Iyi ongororo yengozi yezvakatipoteredza inoratidza kuti kudzika kwakadzikira kwefipronil komisheni kunoderedza nharaunda dzinoyerera munzvimbo zhinji dzeUnited States.
Kunyangwe kugadzirwa kwemakemikari ekugadzira kwakawedzera zvakanyanya mumakumi emakore achangopfuura, kukanganisa kwemakemikari aya pane zvisiri-zvinotangwa zveecosystem hakuna kunyatsonzwisiswa (1).Mumvura yepamusoro apo 90% yeminda yepasi rose inorasika, hapana data pamusoro pemishonga yekurima yezvipembenene, asi pane data, nguva yekuti mishonga yezvipembenene ipfuure zvikumbaridzo zvekutonga ihafu (2).Meta-kuongororwa kwemishonga yekurima mumvura yepamusoro muUnited States yakawana kuti mu70% yenzvimbo dzesampling, imwe mushonga wekuuraya zvipembenene yakapfuura muganhu wekutonga (3).Nekudaro, idzi meta-kuongorora (2, 3) inongotarisa pamvura yepasi yakakanganiswa nekushandiswa kwevhu rekurima, uye ipfupiso yezvidzidzo zvakapusa.Mishonga yezvipembenene, kunyanya mishonga yezvipembenene, inowanikwawo munzvimbo dzakakwirira mumadhorobha emvura (4).Kashoma kuita ongororo yakazara yemishonga yezvipembenene mumvura yepamusoro inoburitswa kubva mukurima uye mumaguta;naizvozvo, hazvizivikanwi kana mishonga yezvipembenene inokonzera ngozi huru kune zviwanikwa zvemvura pamusoro pemvura uye kuvimbika kwayo kwezvakatipoteredza.
Benzopyrazoles uye neonicotinoids yakaverengera chikamu chimwe muzvitatu chemusika wepasi rose wemishonga yezvipembenene muna 2010 (5).Mumvura pamusoro pemvura muUnited States, fipronil uye zvigadzirwa zvayo zvekuora (phenylpyrazoles) ndiyo inonyanya kusanganiswa nemishonga yezvipembenene, uye huwandu hwayo hunowanzopfuura huwandu hwemvura (6-8).Kunyange zvazvo neonicotinoids yakakwezva kutarisa nekuda kwemigumisiro yavo kune nyuchi neshiri uye kuwanda kwavo (9), fipronil inonyanya kutyisa hove neshiri (10), nepo mamwe maphenylpyrazoles Class compounds ane herbicidal effects (5).Fipronil ndeye systemic mishonga yezvipembenene inoshandiswa kudzora tupukanana mumaguta nekurima nharaunda.Sezvo fipronil yakapinda mumusika wepasi rose muna 1993, kushandiswa kwefipronil muUnited States, Japan neUnited Kingdom kwakawedzera zvakanyanya (5).MuUnited States, fipronil inoshandiswa kudzora majuru nemajuru, uye inoshandiswa muzvirimwa zvinosanganisira chibage (kusanganisira kurapwa kwembeu), mbatatisi neminda yemichero (11, 12).Kushandiswa kwekurima kwefipronil muUnited States kwakakwira muna 2002 (13).Kunyangwe pasina ruzivo rwekushandiswa kwemadhorobha rwenyika rwuripo, kushandiswa kwemadhorobha muCalifornia kwakakwira muna 2006 na2015 (https://calpip.cdpr.ca) .gov/main .cfm, yakasvika Zvita 2, 2019).Kunyangwe yakakwira yakakwira yefipronil (6.41μg/L) ichiwanikwa muhova mune dzimwe nzvimbo dzekurima dzine mazinga akakwira ekushandisa (14), zvichienzaniswa nehova dzekurima, hova dzemumaguta muUnited States dzinowanzo kuve nekuonekwa kwakanyanya uye kukwirisa kwakanyanya, kwakanaka kune kuitika kwemadutu kwakabatana nebvunzo (6, 7, 14-17).
Fipronil inopinda mumvura ye ecosystem yekumhanya kana kudonha kubva muvhu kupinda murukova (7, 14, 18).Fipronil ine low volatility (mutemo waHenry unogara 2.31 × 10-4 Pa m3 mol-1), yakaderera kusvika pakati pemvura solubility (3.78 mg/l pa20 ° C), uye ine mwero hydrophobicity (log Kow iri 3.9 kusvika 4.1)), iyo kufamba muvhu kudiki kwazvo (log Koc ndeye 2.6 kusvika 3.1) (12, 19), uye inoratidza kudzika-kusvika-pakati kushingirira munharaunda (20).Finazepril yakasvibiswa ne photolysis, oxidation, pH-dependent hydrolysis uye kuderedza, kuumba zvinhu zvina zvikuru zvinosvibisa: dessulfoxyphenapril (kana sulfoxide), phenaprenip sulfone (sulfone), Filofenamide (amide) uye filofenib sulfide (sulfide).Fipronil degradation zvigadzirwa zvinowanzove zvakanyanya kugadzikana uye kusimba kupfuura iyo mubereki kommoni (21, 22).
Iyo huturu hwefipronil uye kuderera kwayo kuita dzisiri-zvinangwa zvipenyu (zvakadai semvura invertebrates) yakanyatso kunyorwa (14, 15).Fipronil inhengo yeurotoxic iyo inovhiringidza chloride ion ndima kuburikidza ne chloride chiteshi inodzorwa negamma-aminobutyric acid muzvipembenene, zvichikonzera kusungirirwa kwakakwana kukonzeresa kufara kwakanyanya uye kufa (20).Fipronil inosarudza muchetura, saka ine yakakura receptor inosunga hukama hwezvipembenene kupfuura mhuka dzinoyamwisa (23).Iyo insecticidal chiitiko chefipronil degradation zvigadzirwa zvakasiyana.Hupfu hwe sulfone uye sulfide kumvura yakachena invertebrates hwakafanana kana kukwira kupfuura hwemukomboni wemubereki.Desulfinyl ine mwero muchetura asi ine muchetura mushoma pane musanganiswa wemubereki.Zvishoma zvisina muchetura (23, 24).Kushungurudzika kwemvura invertebrates kune fipronil uye fipronil degradation inosiyana zvikuru mukati uye pakati petaxa (15), uye mune dzimwe nguva inodarika kurongeka kwehukuru (25).Chekupedzisira, pane humbowo hwekuti phenylpyrazoles ine muchetura kune ecosystem pane yaimbofungwa (3).
Aquatic biological benchmarks yakavakirwa pakuongororwa kwehupfu murabhoritari inogona kurerutsa njodzi yehuwandu hwemumunda (26-28).Mitemo yemvura inowanzotangwa nemhando imwe chete yerabhoritari yekuongorora toxicity uchishandisa imwe kana akati wandei emvura invertebrate mhuka (semuenzaniso, Diptera: Chironomidae: Chironomus uye Crustacea: Daphnia magna uye Hyalella azteca).Izvi zvipenyu zvekuedza zvinowanzova nyore kurima kupfuura mamwe ma benthic macroinvertebrates (somuenzaniso, phe genus ::), uye mune dzimwe nguva haanyanyi kunzwa kune zvinosvibisa.Semuenzaniso, D. Magna haanyanyi kunzwa kune simbi dzakawanda pane zvimwe zvipembenene, nepo A. zteca isinganyanyi kunzwisiswa nepyrethroid insecticide bifenthrin pane kunzwa kwayo kune makonye (29, 30).Chimwe chidziviso chezviyero zviripo ndezvemagumo anoshandiswa mukuverenga.Acute mabhenji akavakirwa pakufa (kana kugadzirirwa crustaceans), nepo zvisingaperi mabhenji anowanzo akavakirwa pane sublethal endpoints (sekukura uye kubereka) (kana iripo).Nekudaro, kune zvakapararira zvinokonzeresa zvinokonzeresa, sekukura, kubuda, kuremara, uye kunonoka kwekusimudzira, izvo zvinogona kukanganisa budiriro yemutero uye masimba enharaunda.Nekuda kweizvozvo, kunyangwe iyo benchmark ichipa kumashure kwekukosha kwebiological kwemhedzisiro, kukosha kwe ecological sechikumbaridzo chehupfu hakuna chokwadi.
Kuti tinzwisise zviri nani mhedzisiro yefipronil makomisheni pane benthic aquatic ecosystems (invertebrates uye algae), nharaunda dzechisikigo dzebenthic dzakaunzwa murabhoritari uye dzakavhenekerwa kune maconcentration gradients panguva ye30-day kuyerera Fipronil kana imwe yechina fipronil degradation miedzo.Chinangwa chetsvagurudzo ndechekugadzira mhando-chaiyo 50% mhedzisiro yekumisikidza (EC50 kukosha) kune yega yega fipronil inomiririra mutero wakafara wenharaunda yerwizi, uye kuona kukanganiswa kwezvinosvibisa pamagariro nekushanda kwenharaunda [kureva, njodzi yekuisa] 5. % Yezvipenyu zvakakanganisika (HC5) uye zvisina kunanga mhedzisiro senge kuchinjwa kubuda uye trophic dynamics].Ipapo chikumbaridzo (chakakosha-chaiyo HC5 kukosha) chakawanikwa kubva mukuedza kwemesoscopic chakaiswa kumunda wakaunganidzwa neUnited States Geological Survey (USGS) kubva kumatunhu mashanu eUnited States (Northeast, Southeast, Midwest, Northwest Pacific, uye Central California. Coastal Zone) Dhata) sechikamu cheUSGS yedunhu rwizi rwemhando yekuongorora (https://webapps.usgs.gov/rsqa/#!/).Sekuziva kwedu, iyi ndiyo yekutanga yekuongorora njodzi yezvakatipoteredza.Inoongorora zvizere mhedzisiro yefipronil makomisheni pane zvipenyu zvebenthic mune inodzorwa meso-environment, yobva yaisa izvi mhedzisiro kune continental-scale field assessments.
Iyo yemazuva makumi matatu mesocosmic kuyedza yakaitwa paUSGS Aquatic Laboratory (AXL) muFort Collins, Colorado, USA kubva Gumiguru 18th kusvika Mbudzi 17th, 2017, kwezuva 1 rekuvharirwa uye mazuva makumi matatu ekuyedza.Iyo nzira yakambotsanangurwa (29, 31) uye yakatsanangurwa mune yekuwedzera zvinyorwa.Iyo meso space setting ine 36 inotenderera inoyerera mune ina inoyerera inoyerera (inotenderera matangi emvura).Rukova rwega rwega runogara rwakashongedzerwa neinotonhorera kuchengetedza tembiricha yemvura uye inovhenekerwa ne16:8 chiedza-chakasviba kutenderera.Iyo meso-level inoyerera isimbi isina tsvina, iyo inokodzera hydrophobicity yefipronil (log Kow = 4.0) uye inokodzera organic yekuchenesa zvinonyungudutsa (Mufananidzo S1).Mvura yakashandiswa pakuedza kwemeso-scale yakaunganidzwa kubva kuCache La Poudre River (nzvimbo dziri kumusoro dzinosanganisira Rocky Mountain National Park, National Forest uye Continental Divide) uye yakachengetwa mumatangi mana eAXL ekuchengetera polyethylene.Ongororo dzakapfuura dzemasampu uye emvura masampuli akaunganidzwa kubva panzvimbo haana kuwana mishonga yezvipembenene (29).
Iyo meso-scale yekuyedza dhizaini ine makumi matatu ekugadzirisa hova uye 6 kutonga hova.Rukova rwekurapa runogamuchira mvura yakarapwa, imwe neimwe ine isingadzokororwe inogara yakagadziriswa yefipronil komputa: fipronil (fipronil (Sigma-Aldrich, CAS 120068-37-3), amide (Sigma-Aldrich, CAS 205650-69-7), desulfurization boka. [US Environmental Protection Agency (EPA) Pesticide Library, CAS 205650-65-3], sulfone (Sigma-Aldrich, CAS 120068-37-2) uye sulfide (Sigma-Aldrich, CAS 120067-83-6); kuchena kwose ≥ 97.8%. Zvinoenderana neyakaburitswa mhinduro kukosha (7, 15, 16, 18, 21, 23, 25, 32, 33). Nekunyungudutsa fipronil musanganiswa mumethanol ( Thermo Fisher Scientific, American Chemical Society certification level), uye dilute. nemvura ine deionized kusvika pahuwandu hunodiwa kugadzirira concentrated stock solution.Nekuda kwekuti huwandu hwemethanol mudosi hwakasiyana, zvinofanirwa kuwedzera methanol kune ese mahova ekurapa sezvinodiwa.Mukutonga kutatu, kuve nechokwadi cheiyo methanol concentration. 0.05 ml/L) muhova.Maonero epakati edzimwe nzizi nhatu dzekudzora dzakagamuchira mvura yerwizi isina methanol, kana zvisina kudaro dzaitorwa sedzimwe hova dzose.
Pazuva rechisere, zuva rechigumi nematanhatu uye zuva remakumi maviri nematanhatu, tembiricha, pH kukosha, conductivity yemagetsi uye kuderera kwefipronil uye fipronil zvakayerwa mukuyerera membrane.Kuti vatarise kushatiswa kwefipronil yemubereki panguva yekuedzwa kwenhau, fipronil (vabereki) yakashandiswa kurapa mucosa yemudumbu kwemamwe mazuva matatu [mazuva 5, 12 uye 21 (n = 6)] yekushisa, pH , Conductivity, fipronil uye fipronil degradation sampling.Mishonga yekuongorora mishonga yezvipembenene yakaunganidzwa nekusefa 10 ml yemvura inoyerera mu20 ml amber glass vial kuburikidza neWhatman 0.7-μm GF/F sirinji sefa ine dhayamita hombe tsono.Sampuli dzakabva dzaoma chando ndokutumirwa kuUSGS National Water Quality Laboratory (NWQL) muLakewood, Colorado, USA kuti iongororwe.Ichishandisa nzira yakavandudzwa yenzira yakamboburitswa, Fipronil uye 4 zvigadzirwa zvekusvibisa mumasampuli emvura zvakatemerwa neakananga aqueous jekiseni (DAI) liquid chromatography-tandem mass spectrometry (LC-MS / MS; Agilent 6495).Iyo nhanho yekuona chiridzwa (IDL) inofungidzirwa kuve iyo yakaderera calibration mwero inosangana nehunhu hwekuzivikanwa mwero;iyo IDL yefipronil i0.005 μg/L, uye IDL yemamwe mana fipronil i0.001 μg/L.Iyo yekuwedzera zvinhu inopa tsananguro yakazara yenzira dzinoshandiswa kuyera fipronil makomisheni, anosanganisira kudzora kwemhando uye maitiro ekuvimbisa (semuenzaniso, sampuli kudzoreredza, spikes, yechitatu bato kuongorora, uye blanks).
Pakupera kwemazuva makumi matatu ekuedzwa kweMesocosmic, kuverengwa nekuzivikanwa kwevanhu vakuru uye varava invertebrates zvakapedzwa (iyo huru yekuunganidza data yekupedzisira).Vakuru vari kusimukira vanounganidzwa kubva mumambure mazuva ese uye voomeswa nechando mune yakachena 15 ml Falcon centrifuge chubhu.Pakupera kwekuedza (zuva 30), zviri mukati me membrane murukova rumwe norumwe zvakakweshwa kuti zvibvise chero zvipembenene, uye zvakasefa (250 μm) uye zvakachengetwa mu80% ethanol.Timberline Aquatics (Fort Collins, CO) yapedza kucherechedzwa kwetaxonomic yemakonye uye vanhu vakuru vasina vertebrates kusvika kune yakaderera taxonomic level inokwanisika, kazhinji mhando.Pamazuva 9, 19 ne29, chlorophyll a yakayerwa nekatatu mumesoscopic membrane yerukova rwega-hwega.Yese makemikari uye biological data sechikamu cheyedzo yemesoscopic inopihwa mune inoperekedza data kuburitswa (35).
Ongororo yezvakatipoteredza yakaitwa munzizi diki (dzinoyerera) munzvimbo shanu huru dzeUnited States, uye mishonga yezvipembenene yakatariswa mukati menguva yapfuura.Muchidimbu, zvichibva pane zvekurima uye zvemaguta ekushandiswa kwevhu (36-40), 77 kune 100 nzvimbo dzakasarudzwa munharaunda imwe neimwe (444 nzvimbo dzakazara).Munguva yechirimo uye zhizha regore rimwe (2013-2017), sampuli dzemvura dzinounganidzwa kamwechete pavhiki munharaunda imwe neimwe kwemavhiki mana kusvika gumi nemaviri.Nguva yakatarwa inoenderana nenharaunda uye kukura kwekukura.Zvisinei, zviteshi 11 zviri munharaunda yekuchamhembe kwakadziva kumabvazuva zvinenge zviri munzvimbo inoyerera mvura.Hapana budiriro, kunze kwekunge sampuli imwe chete yakaunganidzwa.Sezvo nguva dzekutariswa kwemishonga yezvipembenene muzvidzidzo zvematunhu dzakasiyana, kana tichienzanisa, masampuli mana ekupedzisira anounganidzwa panzvimbo yega yega anotariswa pano.Zvinofungidzirwa kuti sampuli imwe yakaunganidzwa panzvimbo isina kugadzirwa yeNortheast saiti (n = 11) inogona kumiririra iyo 4-vhiki sampling nguva.Iyi nzira inotungamirira kunhamba yakafanana yekucherechedza pamishonga yezvipembenene (kunze kwenzvimbo 11 muNortheast) uye nguva imwechete yekucherechedza;Zvinotendwa kuti mavhiki mana akareba zvakakwana kuti aonekwe kwenguva refu kune biota, asi ipfupi zvakakwana zvekuti nharaunda yezvipenyu haifanire kupora kubva kune avo vanobatika.
Muchiitiko chekuyerera kwakakwana, sampuli yemvura inounganidzwa nenzira yekugara kwevelocity uye inogara yakafara kuwedzera (41).Kana kuyerera kusina kukwana kushandisa nzira iyi, unogona kuunganidza sampuli nekubatanidzwa kwakadzika kwemasampuli kana kubata kubva pakati pesimba rekuyerera.Shandisa sirinji yakaboora uye dhisiki sefa (0.7μm) kuunganidza 10 ml yesampuli yakasefa (42).Kuburikidza neDAI LC-MS/MS/MS/MS, masampu emvura akaongororwa paNWQL nokuda kwemishonga inouraya zvipembenene ne225, kusanganisira fipronil uye 7 degradation products (dessulfinyl fipronil, fipronil) Sulfides, fipronil sulfone, deschlorofipronil, fipronildesthimide, fipronil uye fipronil).)Madiki ekushuma mazinga ezvidzidzo zvemumunda ndeaya: fipronil, desmethylthio fluorobenzonitrile, fipronil sulfide, fipronil sulfone, uye deschlorofipronil 0.004 μg/L;dessulfinyl fluorfenamide uye Kuwanda kwefipronil amide ndeye 0.009 μg/lita;huwandu hwefipronil sulfonate ndeye 0.096 μg/litre.
Nharaunda dzisina vertebrate dzinotorwa pakupera kwechidzidzo chega chega (chirimo/chirimo), kazhinji panguva imwe chete nechiitiko chekupedzisira chekuongorora mishonga yezvipembenene.Mushure memwaka wekukura uye kushandiswa kwakanyanya kwemishonga yezvipembenene, nguva yekuenzanisa inofanira kuenderana nemamiriro ekuyerera kwepasi, uye inofanira kuenderana nenguva iyo nharaunda yerwizi invertebrate inokura uye inonyanya kuve muchikamu chehupenyu hwemakonye.Kushandisa Surber sampler ine 500μm mesh kana D-frame net, invertebrate community sampling yakapedzwa mu437 kunze kwe444 masaiti.Iyo sampling nzira inotsanangurwa zvakadzama mune yekuwedzera zvinhu.PaNWQL, marudzi ese asina vertebrates anowanzo zivikanwa uye akanyorwa pane genus kana mhando yemhando.Yese makemikari uye biological data yakaunganidzwa mundima iyi uye yakashandiswa mune ino manyoro inogona kuwanikwa mune inoperekedza data kuburitswa (35).
Pamakomisheni mashanu efipronil anoshandiswa mukuedza kwemesoscopic, kuwanda kwezvipembenene zvisingaite zvakaderedzwa ne20% kana 50% zvakaverengerwa maererano nekutonga (kureva EC20 uye EC50).Iyo data [x = nguva-yakaremerwa fipronil concentration (ona supplementary material for details), y = larval abundance kana mamwe ma metrics] yakaiswa kuR(43) yakawedzerwa pasuru uchishandisa matatu-parameter logarithmic regression method" drc".Iyo curve inoenderana nemarudzi ese (mapunga) ane huwandu hwakakwana uye inosangana nemamwe ma metrics ekufarira (semuenzaniso, taxa kupfuma, yakazara mayfly kuwanda, uye yakazara kuwanda) kuti uwedzere kunzwisisa maitiro enharaunda.Iyo Nash-Sutcliff coefficient (45) inoshandiswa kuongorora iyo modhi inokodzera, apo yakashata modhi inokwana inogona kugashira kusingaperi maitiro asina kunaka, uye kukosha kwekukwana kwakakwana i1.
Kuti uongorore migumisiro yefipronil compounds pakubuda kwezvipembenene mukuedza, data yakaongororwa nenzira mbiri.Chekutanga, nekubvisa avhareji yekutaridzika kwekuyerera kwekutonga meso kubva pakuonekwa kwega kwega kurapwa kuyerera meso, kuwanda kwezuva nezuva kwezvipembenene kubva kune yega yega kuyerera meso (huwandu hwese hwevanhu vese) hwakave hwakajairwa kukutonga.Ronga aya hunhu uchipokana nenguva kuti unzwisise kutsauka kwemurevereri wemvura yekurapa kubva kumurevereri wemvura yekudzora muyedzo yemazuva makumi matatu.Chechipiri, verenga huwandu hwekuitika kwepeji yega yega inoyerera mesophyll, iyo inotsanangurwa sereshiyo yehuwandu hwehuwandu hwemesophyll mukuyerera kwakapihwa kune avhareji yenhamba yehonye nevakuru muboka rekutonga, uye inokodzera matatu-parameter logarithmic regression. .Zvipembenene zvese zvinomera zvakaunganidzwa zvaibva kumhuri mbiri dzeChironomidae, saka ongororo yakasanganiswa yakaitwa.
Shanduko muchimiro chenharaunda, sekurasikirwa kwemutero, inogona kupedzisira ichitsamira pane yakananga uye isina kunanga mhedzisiro yezvinhu zvine chepfu, uye inogona kutungamira shanduko mukushanda kwenharaunda (semuenzaniso, trophic cascade).Kuedza iyo trophic cascade, yakapusa causal network yakaongororwa uchishandisa nzira yekuongorora nzira (R package "piecewiseSEM") (46).Pakuongorora kwemesoscopic, inofungidzirwa kuti fipronil, desulfinyl, sulfide uye sulfone (isina kuedzwa amide) mumvura kuderedza biomass ye scraper, zvisina kunanga zvinotungamirira kuwedzera kwebiomass ye chlorophyll a (47).Iko kusungirirwa kwekomboni ndiko kushanduka kwekufanotaura, uye scraper uye chlorophyll biomass ndiwo maitiro emhinduro.Fisher's C nhamba inoshandiswa kuongorora modhi yakakodzera, kuitira kuti P kukosha <0.05 iratidze yakanaka modhi inokodzera (46).
Kuti ugadzire njodzi-yakavakirwa eco-community pachikumbaridzo chekudzivirira, imwe neimwe komputa yakawana 95% yemhando dzakakanganisika (HC5) dzisingaperi mhando senitivity kugovera (SSD) uye njodzi yekudzivirira.Matatu eSSD data seti akagadzirwa: (i) chete meso data set, (ii) seti yedata ine ese meso data uye data yakaunganidzwa kubva kuEPA ECOTOX dhatabhesi mubvunzo (https://cfpub.epa.gov/ecotox) /, inowanikwa pa Kurume 14, 2019), nguva yekudzidza imazuva mana kana kureba, uye (iii) seti yedata ine ese mesoscopic data uye ECOTOX data, umo data reECTOX (acute exposure) rakakamurwa neacute kusvika The ratio of chronic D. magna ( 19.39) kutsanangura mutsauko wenguva yekuratidzwa uye kuenzanisa iyo isingaperi EC50 kukosha (12).Chinangwa chedu chekugadzira akawanda maSSD modhi ndeye (i) kugadzira HC5 kukosha kwekuenzanisa nedata remumunda (chete reSSD remidhiya), uye (ii) kuongorora kuti midhiya data inogamuchirwa zvakanyanya kupfuura masangano anodzora kuti abatanidzwe mune yeaquaculture. kusimba kwehupenyu mabhenji uye yakajairwa kugadzika kwe data zviwanikwa, uye nekudaro kugona kwekushandisa mesoscopic zvidzidzo zvekugadzirisa maitiro.
SSD yakagadziridzwa yega yega data seti uchishandisa iyo R package "ssdtools" (48).Shandisa bootstrap (n = 10,000) kufungidzira avhareji yeHC5 uye nguva yekuvimba (CI) kubva kuSSD.Makumi mana nepfumbamwe emutero mhinduro (yese taxa yakaonekwa serudzi kana mhuka) yakagadzirwa kuburikidza netsvagiridzo iyi inosanganiswa nemhinduro makumi matatu nembiri dzemitero dzakaunganidzwa kubva muzvidzidzo zvitanhatu zvakaburitswa mudhatabhesi reECOTIX, kune inokwana makumi masere neimwe mhinduro yeTaxon inogona kushandiswa kusimudzira SSD. .Sezvo pasina data yakawanikwa muECTOX dhatabhesi yeamides, hapana SSD yakagadziridzwa mamides uye mhinduro imwe chete yeEC50 yakawanikwa kubva kuchidzidzo chazvino.Kunyangwe kukosha kweEC50 yeboka rimwe chete resulfide yakawanikwa mudhatabhesi reECOTX, mudzidzi akapedza kudzidza iye zvino ane gumi nemaviri EC50.Naizvozvo, maSSD emapoka esulfinyl akagadzirwa.
Iwo chaiwo HC5 makomisheni efipronil makomisheni akawanikwa kubva kuSSD data set yeMesocosmos chete akasanganiswa nedata remumunda kuti aongorore kuratidzwa uye huturu hwehupfu hwefipronil makomisheni mu444 hova kubva kumatunhu mashanu muUnited States.Mune yekupedzisira 4-vhiki sampling hwindo, yega yega yefipronil komisheni yakaonekwa (isina kuoneswa concentration ndeye zero) inokamurwa neiyo HC5, uye chiyero chechikamu chemuenzaniso wega wega chinopfupikiswa kuwana Iyo yakazara toxicity unit yefipronil (ΣTUFipronils), uko. ΣTUFipronils> 1 zvinoreva chepfu.
Nekuenzanisa kusangana kwengozi ye50% yezvipenyu zvakakanganisika (HC50) neEC50 kukosha kwekupfuma kwemutero kunobva muyedzo yemembrane yepakati, SSD yakawanikwa kubva kune yepakati membrane data yakaongororwa kuratidza kunzwisiswa kwenharaunda yakafara yenharaunda kune fipronil. degree..Kuburikidza nekuenzanisa uku, kuwirirana pakati peSSD nzira (kusanganisira chete iyo taxa ine hukama-mhinduro) uye EC50 nzira (kusanganisira yese yakasarudzika taxa inocherechedzwa munzvimbo yepakati) uchishandisa iyo EC50 nzira yekuyera hupfumi hwemitero inogona kuongororwa Bonde.Dose mhinduro hukama.
A pesticide risk species (SPEARpesticides) chiratidzo chakaverengerwa kuti chiongorore hukama huri pakati pehutano hwehutano hwevanhu vasina vertebrate uye ΣTUFipronil mu 437 invertebrate-kuunganidza hova.Iyo SPEARpesticides metric inoshandura kuumbwa kwezvisina vertebrates kuita abundance metric ye biological taxonomy ine physiological uye ecological maitiro, nokudaro ichipa kunzwisiswa kumishonga yezvipembenene.Iyo SPEARpesticides chiratidzo haina hanya neakasikwa covariates (49, 50), kunyangwe kuita kwayo kuchakanganiswa nekuparara kwakanyanya kwenzvimbo (51).Iyo yakawanda data inounganidzwa pa-saiti yemutero wega wega inobatanidzwa nehukoshi hwakakosha hwemutero une hukama neASTERICS software yekuongorora mhando yezvisikwa zverwizi (https://gewaeser-bewertung-berechnung.de/index.php/home html).Wobva wapinza iyo data muIndicate (http://systemecology.eu/indicate/) software (version 18.05).Mune iyi software, iyo European trait dhatabhesi uye dhatabhesi ine physiological sensitivity kune mishonga yezvipembenene inoshandiswa kushandura data resaiti yega yega kuita SPEARpesticides chiratidzo.Imwe neimwe yezvidzidzo zvishanu zvedunhu yakashandisa General Additive Model (GAM) ["mgcv" package muR(52)) kuongorora hukama huripo pakati peSPEARpesticides metric neΣTUFipronils [log10(X + 1) conversion] Associated.Kuti uwane rumwe ruzivo nezve SPEARpesticides metrics uye yekuongorora data, ndapota ona Supplementary Materials.
Iyo indekisi yemhando yemvura inowirirana mukuyerera kwega kwega mesoscopic uye iyo yese mesoscopic yekuyedza nguva.Avhareji tembiricha, pH uye conductivity vaiva 13.1 ° C (± 0.27 ° C), 7.8 (± 0.12) uye 54.1 (± 2.1) μS/cm (35), zvichiteerana.Iyo yakayerwa yakanyungudika organic kabhoni mumvura yakachena yerwizi i3.1 mg/L.Mumeso-meso erwizi panoiswa MiniDOT rekodha, iyo okisijeni yakanyungudika iri pedyo nekuzara (avhareji> 8.0 mg/L), zvichiratidza kuti rukova rwakatenderedzwa zvizere.
Kudzora kwemhando uye dhizaini yekusimbisa data pafipronil inopihwa mune inoperekedza data kuburitswa (35).Muchidimbu, mazinga ekudzoreredza erabhoritari matrix spikes uye mesoscopic samples anowanzo ari mukati mezviyero zvinogamuchirika (kudzoreredzwa kwe70% kusvika 130%), zviyero zveIDL zvinosimbisa nzira yehuwandu, uye marabhoritari nemidziyo yezviridzwa zvinowanzo kuchena. izvi zvakazara zvinokurukurwa muwedzero..
Pamusana pekugadzirwa kwehurongwa, iyo yakayerwa yefipronil inowanzove yakaderera pane inotarirwa kukosha (Mufananidzo S2) (nokuti inotora 4 kune mazuva gumi kusvika kune yakadzikama pasi pemamiriro akanaka) (30).Kuenzaniswa nemamwe mafipronil compounds, iyo desulfinyl uye amide inoshandura zvishoma nezvishoma nekufamba kwenguva, uye kusiyanisa kwehutano mukati mekurapa kuduku kudarika kusiyana kwemishonga kunze kwekuderera kwekugadzirisa sulfone uye sulfide.Nguva-yeyero yevhareji yakayerwa yepakati yeboka rega rega rekurapa ndeyotevera: Fipronil, IDL kusvika 9.07μg / L;Desulfinyl, IDL kusvika 2.15μg/L;Amide, IDL kusvika 4.17μg/L;Sulfidi, IDL Kusvika 0.57μg/lita;uye sulfone, IDL i1.13μg/lita (35).Mune mamwe nzizi, isiri-chinangwa fipronil makomisheni akaonekwa, ndiko kuti, makomisheni aive asina kuiswa mune yakasarudzika kurapwa, asi aizivikanwa seanosvibisa zvigadzirwa zvekomboni yekurapa.Iyo mesoscopic membranes inobatwa nefipronil yemubereki ine nhamba yepamusoro-soro yezvinhu zvisiri izvo zvinotapukira zvakaonekwa (kana zvisingashandiswe semusanganiswa wekugadzira, iwo sulfnyl, amide, sulfide uye sulfone);izvi zvinogona kunge zvakakonzerwa nekugadzirwa kweCompound tsvina uye/kana degradation process inoitika panguva yekuchengetera stock solution uye (kana) mukuyedza mesoscopic kwete mhedzisiro yekusvibiswa.Hapana maitiro ekudzikisira kuderedzwa akaonekwa mukurapwa kwefipronil.Zvisizvo-zvinangwa zvinosvibisa zvipembenene zvinonyanya kuonekwa mumuviri nepamusoro-soro yehutano hwehutano, asi kusungirirwa kuduku kudarika kusanganiswa kwezvinhu izvi zvisingatarisirwi (ona chikamu chinotevera chekugadzirisa).Nokudaro, sezvo zvisingatarisirwi zvinosvibisa zvipembenene zvisingawanzoonekwi mune yakaderera fipronil kurapwa, uye nokuti iyo yakaonekwa yakaderera pane iyo inokonzerwa nekugadzirisa mukurapa kwepamusoro, zvinogumiswa kuti izvi zvisingatarisirwi zvinosanganiswa zvine zvishoma pakuongorora.
Mukuedza kwevezvenhau, benthic macroinvertebrates yainzwa kune fipronil, desulfinyl, sulfone, uye sulfide [Table S1;yepakutanga kuwanda data inopihwa mukuperekedza data vhezheni (35)].Fipronil amide ndeyenhunzi chete Rhithrogena sp.Chepfu (inouraya), EC50 yayo ndeye 2.05μg/L [±10.8(SE)].Dose-mhinduro macurves e15 akasiyana taxa akagadzirwa.Iyi taxa yakaratidza kufa mukati meiyo yakaedzwa yekutarisa renji (Table S1), uye yakanangwa clustered taxa (senge nhunzi) (Figure S3) uye yakapfuma taxa (Figure 1) A dose remhinduro curve rakagadzirwa.Iko kusungirirwa (EC50) yefipronil, desulfinyl, sulfone uye sulfide pane iyo yakasarudzika taxa yeanonyanya kunzwa taxa kubva 0.005-0.364, 0.002-0.252, 0.002-0.061 uye 0.005-0.043μg/L, zvakateerana.Rhithrogena sp.Uye Sweltsa sp.;Mufananidzo S4) yakaderera pane yakanyanya kushivirira taxa (yakadai se Micropsectra / Tanytarsus uye Lepidostoma sp.) (Tafura S1).Zvinoenderana neavhareji EC50 yekomboni yega yega muTable S1, sulfones uye sulfides ndiwo anonyanya kushanda makomisheni, nepo invertebrates kazhinji isinganzwisisike kune desulfinyl (kunze kwekusanganisa amides).Metrics ezvese ecological chimiro, senge taxa kupfuma, yakazara kuwanda, yakazara pentaploid uye yakazara ibwe nhunzi, kusanganisira taxa uye kuwanda kweimwe taxa, izvi hazviwanzo mumeso uye hazvigone kuverengerwa Dhirowa yakaparadzana dosi mhinduro curve.Naizvozvo, izvi zviratidzi zvezvakatipoteredza zvinosanganisira mhinduro dzemitero dzisina kubatanidzwa muSSD.
Taxa kupfuma (larva) ine matatu-level logistic function ye (A) fipronil, (B) desulfinyl, (C) sulfone, uye (D) sulfide concentration.Imwe neimwe poindi yedata inomiririra makonye kubva kune imwechete rukova pakupera kwemazuva makumi matatu ekuedza kwemeso.Taxon kupfuma ndiko kuverenga kwemutero wakasarudzika murukova rwega rwega.Hukoshi yehuremu ndiyo yeavhareji yakayerwa yenguva yakacherechedzwa yerukova yega yega yakayerwa pakupera kwekuedza kwemazuva makumi matatu.Fipronil amide (isina kuratidzwa) haina hukama neakapfuma taxa.Ndokumbira utarise kuti x-axis iri pachiyero chelogarithmic.EC20 uye EC50 ine SE inoshumwa muTafura S1.
Pamusoro pepamusoro pese mashanu efipronil makomisheni, chiyero chekubuda kweUetridae chakaderera.Iko muzana yekumera (EC50) ye sulfide, sulfone, fipronil, amide uye desulfinyl yakaonekwa ichiderera ne50% pazvikamu zve 0.03, 0.06, 0.11, 0.78 uye 0.97μg / L maererano (Mufananidzo 2 uye Mufananidzo S5)Muzvizhinji zvemazuva makumi matatu ekuedzwa, mishonga yose yefipronil, desulfinyl, sulfone uye sulfide yakanonoka, kunze kwemamwe mishonga yakaderera (Mufananidzo 2), uye kuonekwa kwavo kwakadziviswa.Mukurapa kweamide, mvura yakaunganidzwa panguva yekuedza yose yakanga yakakwirira kudarika iyo yekutonga, ine mutsara we 0.286μg / litre.Iyo yepamusoro-soro (4.164μg / litre) panguva yese yekuedza yakadzivisa kusvibiswa, uye chiyero chemvura yekurapa kwepakati chakanga chakafanana neyeboka rinodzora.(mufananidzo 2).
Kuwedzera kubuda kweavhareji yemazuva ese avhareji kubuda kwega kwega kurapwa kubvisa (A) fipronil, (B) desulfinyl, (C) sulfone, (D) sulfide uye (E) amide murukova rwekutonga Avhareji yemazuva ese avhareji kubuda kwe membrane.Kunze kwekutonga (n = 6), n = 1. Kukosha kwehutano ndiyo nguva-yeredhi yevhareji yehutano hwakaonekwa mukuyerera kwega.
Iyo dosi-mhinduro curve inoratidza kuti, pamusoro pekurasikirwa kwetaxonomic, shanduko yezvimiro padanho renharaunda.Kunyanya, mukati meyedzo yekumisikidzwa renji, kuwanda kwe may (Mufananidzo S3) uye taxa kuwanda (Mufananidzo 1) yakaratidza hukama hwakakosha hwedosi-mhinduro nefipronil, desulfinyl, sulfone, uye sulfide.Naizvozvo, takaongorora kuti shanduko dzezvimiro idzi dzinotungamira sei kushanduko mukushanda kwenharaunda nekuyedza iyo inovaka muviri.Kuratidzwa kwemvura invertebrates kune fipronil, desulfinyl, sulfide uye sulfone ine kukanganisa kwakananga kune biomass ye scraper (Mufananidzo 3).Kuti uchengetedze kukanganisa kwakashata kwefipronil pane biomass ye scraper, scraper yakakanganisawo chlorophyll a biomass (Mufananidzo 3).Mhedzisiro yeaya asina kunaka nzira coefficients ndeyekuwedzerwa kweti mu chlorophyll a sezvo kuunganidzwa kwefipronil uye zvinosvibisa kunowedzera.Aya maenzaniso akazara enzira anoratidza kuti kuwedzera kuderera kwefipronil kana fipronil kunotungamirira kuwedzera kwechikamu cheklorophyll a (Mufananidzo 3).Zvinofungidzirwa pachine nguva kuti mhedzisiro yakananga pakati pefipronil kana degradation concentration uye chlorophyll biomass i zero, nekuti fipronil makomisheni mishonga yezvipembenene uye ine yakaderera yakananga huturu kune algae (semuenzaniso, iyo EPA acute isina-vascular plant baseline concentration ndeye 100μg / L. fipronil, disulfoxide group, sulfone uye sulfide; https://epa.gov/pesticide-science-and-assessing-pesticide-risk/aquatic-life-benchmarks-and-ecological-risk), Mibairo yese (mienzaniso inoshanda) inotsigira izvi hypothesis.
Fipronil inogona kuderedza zvakanyanya biomass (direct effect) yemafuro (scraper group is larvae), asi haina zvakananga pane biomass ye chlorophyll a.Nekudaro, iyo yakasimba isina kunanga mhedzisiro yefipronil ndeyekuwedzera biomass yechlorophyll a mukupindura kushoma kwemafuro.Museve unoratidza yakamisikidzwa nzira coefficient, uye minus sign (-) inoratidza gwara rekubatana.* Inoratidza mwero wekukosha.
Iwo matatu SSDs (yepakati layer chete, yepakati layer plus ECOTOX data, uye yepakati layer plus ECOTOX dhata yakagadziridzwa mutsauko wenguva yekuratidzwa) yakagadzira zvakasiyana siyana HC5 kukosha (Tafura S3), asi mhedzisiro yaive mukati meSE renji.Mukusara kwechidzidzo ichi, tichatarisa pane data SSD ine meso universe chete uye yakabatana HC5 kukosha.Kuti uwane tsananguro yakazara yeaya matatu maSSD ongororo, ndapota tarisa kune zvekuwedzera zvinhu (Matafura S2 kusvika S5 uye Figure S6 uye S7).Iyo yakanyanya-yakakodzera data kugovera (yakaderera Akaike ruzivo muyero muyero) yechina fipronil makomisheni (Mufananidzo 4) inoshandiswa chete mumeso-solid SSD mepu ndiyo log-gumbel yefipronil uye sulfone, uye weibull yesulfide Uye desulfurized γ ( Tafura S3).Huwandu hweHC5 hwakawanikwa pakomboni yega yega hunoshumwa muMufananidzo 4 wemeso universe chete, uye muTable S3 kukosha kweHC5 kubva kune ese matatu eSDD data seti anoshumwa.Iyo HC50 kukosha kwefipronil, sulfide, sulfone uye desulfinyl mapoka [22.1±8.78 ng/L (95% CI, 11.4 kusvika 46.2), 16.9±3.38 ng/L (95% CI, 11.2 kusvika 28.0±), 2.66 ng/L (95% CI, 5.44 kusvika 15.8) uye 83.4±32.9 ng/L (95% CI, 36.4 kusvika 163)] Mishonga iyi yakaderera zvakanyanya pane EC50 taxa hupfumi (nhamba yese yemutero wakasiyana) (Tafura S1 ; zvinyorwa zviri patafura yekuwedzera mamicrograms parita).
Mukuedza kwemeso-scale, kana yaiswa ku (A) fipronil, (B) dessulfinyl fipronil, (C) fipronil sulfone, (D) fipronil sulfide kwemazuva makumi matatu, kunzwisiswa kwemarudzi kunotsanangurwa Ndiyo EC50 kukosha kwetaxon.Mutsara weblue dashed unomiririra 95% CI.Mutsetse wedashi wakachinjika unomiririra HC5.Iko HC5 kukosha (ng / L) yekomboni imwe neimwe ndeyotevera: Fipronil, 4.56 ng / L (95% CI, 2.59 kusvika 10.2);Sulfidi, 3.52 ng/L (1.36 kusvika 9.20);Sulfone, 2.86 ng/ Lita (1.93 kusvika 5.29);uye sulfnyl, 3.55 ng/litre (0.35 kusvika 28.4).Ndokumbira utarise kuti x-axis iri pachiyero chelogarithmic.
Muzvidzidzo zvishanu zvedunhu, Fipronil (vabereki) yakaonekwa mu22% ye444 yemunda sampling points (Table 1).Iyo yekuona nguva ye florfenib, sulfone uye amide yakafanana (18% kusvika 22% yemuenzaniso), iyo yekuona frequency ye sulfide uye desulfinyl yakaderera (11% kusvika 13%), asi zvakasara zvinosvibisa zvigadzirwa zvakanyanya.Vashoma (1% kana pasi) kana vasina kumboonekwa (Tafura 1)..Fipronil inowanzoonekwa kumaodzanyemba kwakadziva kumabvazuva (52% yemasaiti) uye kazhinji kuchamhembe kwakadziva kumadokero (9% yemasaiti), iyo inotaridza kusiyanisa kwekushandiswa kwebenzopyrazole uye njodzi yerukova inogona kuitika munyika yose.Degradants vanowanzo ratidza maitiro ematunhu akafanana, ane yakanyanya kutariswa frequency kumaodzanyemba kwakadziva kumabvazuva uye yakaderera kuchamhembe kwakadziva kumadokero kana mahombekombe California.Iyo yakayerwa yefipronil yaive yepamusoro-soro, ichiteverwa neiyo mubereki compound fipronil (90% muzana ye10.8 uye 6.3 ng/L, zvichiteerana) (Tafura 1) (35).Iyo yakakwirira yefipronil (61.4 ng / L), disulfinyl (10.6 ng / L) uye sulfide (8.0 ng / L) yakatemwa kumaodzanyemba kwakadziva kumabvazuva (mumavhiki mana ekupedzisira emuenzaniso).Iyo yakanyanya kuwanda yesulfone yakatemwa kumadokero.(15.7 ng/L), amide (42.7 ng/L), dessulfinyl flupirnamide (14 ng/L) uye fipronil sulfonate (8.1 ng/L) (35).Florfenide sulfone ndiyo chete musanganiswa wakaonekwa kupfuura HC5 (Table 1).Avhareji ΣTUFipronils pakati pematunhu akasiyana anosiyana zvakanyanya (Tafura 1).Avhareji yenyika ΣTUFipronils ndeye 0.62 (nzvimbo dzese, matunhu ese), uye 71 nzvimbo (16%) ine ΣTUFipronils> 1, zvichiratidza kuti inogona kuva chepfu kune benthic macroinvertebrates.Muzvikamu zvina zvezvishanu zvakadzidzwa (kunze kweMidwest), kune hukama hunokosha pakati peSPEARpesticides neΣTUFipronil, neR2 yakagadziridzwa kubva ku0.07 kumhenderekedzo yeCalifornia kusvika ku0.34 kumaodzanyemba kwakadziva kumabvazuva (Mufananidzo 5).
*Makomponi anoshandiswa mumesoscopic kuyedza.† ΣTUFipronils, iyo yepakati yehuwandu hwehupfu hwemayuniti [akacherechedzwa munda kusungwa kwechina fipronil makomisheni / njodzi yekusangana kwechikamu chimwe nechimwe kubva pachishanu percentile yeSSD-ine hutachiona hwemhando (Mufananidzo 4)] Kwemasamples evhiki nevhiki efipronil, yekupedzisira 4 mavhiki emasampuli emishonga yezvipembenene akaunganidzwa panzvimbo yega yega akaverengerwa.‡ Huwandu hwenzvimbo dzinoyerwa mishonga yezvipembenene.§90th percentile yakavakirwa pahuwandu hwehuwandu hwakaonekwa panzvimbo mukati memavhiki mana ekupedzisira ekuongororwa kwemishonga yezvipembenene.nehuwandu hwemasampuli akaedzwa.¶ Shandisa 95% CI yeHC5 kukosha (Mufananidzo 4 uye Tafura S3, meso chete) kuverenga CI.Dechloroflupinib yakaongororwa mumatunhu ese uye haina kumbobvira yawanikwa.ND, haina kuwanikwa.
Iyo Fipronil toxic unit ndiyo yakayerwa fipronil concentration yakakamurwa nekomboni-chaiyo HC5 kukosha, iyo inotarwa neSSD inowanikwa kubva muyedzo yenhau (ona Mufananidzo 4).Mutsara wakasviba, generalized additive model (GAM).Mutsetse mutsvuku une CI ye95% yeGAM.ΣTUFipronils inoshandurwa kuita log10 (ΣTUFipronils+1).
Mhedzisiro yakashata yefipronil pane dzisiri-chinangwa mhuka dzemumvura dzakanyorwa zvakanaka (15, 21, 24, 25, 32, 33), asi ichi ndicho chidzidzo chekutanga umo inonzwisisika munzvimbo inodzorwa yerabhoritari.Nharaunda dzemutero dzakaratidzirwa kune fipronil makomisheni, uye mhedzisiro yacho yakawedzera pachiyero chekondinendi.Mhedzisiro yemazuva makumi matatu ekuedza kwemesocosmic inogona kuburitsa 15 discrete mapoka ezvipembenene zvemumvura (Table S1) ine isina kutaurwa kusungwa mumabhuku, pakati peiyo zvipembenene zvemumvura mudhatabhesi rehupfu zvinomiririrwa (53, 54).Taxa-specific dose-response curves (yakadai seEC50) inoratidzwa mukuchinja kwenharaunda (sekupfuma kwetaxa uye inogona kubhururuka kurasikirwa kwakawanda) uye kuchinja kwekushanda (zvakadai sekudya kunovaka muviri uye kuchinja kwechitarisiko).Mhedzisiro yemesoscopic universe yakawedzerwa kumunda.Mune ina yenzvimbo shanu dzekutsvagisa muUnited States, iyo fipronil yakayerwa yemunda yaive yakabatana nekuderera kweiyo ecosystem yemvura mumvura inoyerera.
Iyo HC5 kukosha kwe95% yezvipenyu zviri mukati memembrane kuyedza ine mhedzisiro yekudzivirira, zvichiratidza kuti nharaunda dzese dzemumvura dzemumvura dzinonzwa zvakanyanya kune fipronil makomisheni kupfuura zvaimbonzwisiswa.Iyo yakawanikwa HC5 kukosha (florfenib, 4.56 ng/liter; desulfoxirane, 3.55 ng/liter; sulfone, 2.86 ng/liter; sulfide, 3.52 ng/litre) yakapetwa (florfenib) kusvika katatu Kupfuura order of magnitude (desulfinyl) ) pazasi pezvino EPA isingaperi invertebrate benchmark [fipronil, 11 ng/liter;desulfinyl, 10,310 ng/litre;sulfone, 37 ng/litre;uye sulfide, ye110 ng/litre (8)].Mesoscopic miedzo yakaratidza mapoka akawanda anonzwisisa fipronil panzvimbo yeaya anoratidzwa neEPA chronic invertebrate benchmark (4 mapoka anonyanya kufunga fipronil, 13 pairs of desulfinyl, 11 pairs of sulfone uye 13 pairs) Sulfide sensitivity) (Mufananidzo 4 uye tafura) S1).Izvi zvinoratidza kuti mabenchmarks haakwanise kuchengetedza akati wandei anoonekwa munyika yepakati, ayo akapararira munzvimbo dzemumvura.Musiyano uripo pakati pezvatichawana uye bhenji yemazuva ano inonyanya kukonzerwa nekushaikwa kwefipronil toxicity test data inoshanda kune huwandu hwezvipembenene zvemumvura taxa, kunyanya kana nguva yekuratidzira ichipfuura mazuva mana uye fipronil inoshatisa.Munguva yemazuva makumi matatu ekuedza kwemesocosmic, zvipembenene zvakawanda munharaunda ye invertebrate zvainyanya kunzwisiswa fipronil kupfuura yakajairika test organism Aztec (crustacean), kunyange mushure mekugadzirisa Aztec Iyo EC50 yeTeike inoita kuti ive yakafanana mushure mekushandura kwakanyanya.(Kazhinji maawa 96) kusvika kunguva isingaperi yekuratidzwa (Mufananidzo S7).Kubvumirana kurinani kwakasvikwa pakati peyepakati membrane kuyedza uye chidzidzo chakashumwa muECOTOX uchishandisa yakajairwa test organism Chironomus dilutus (chipembenene).Hazvishamisi kuti zvipembenene zvemumvura zvinonyanya kunetseka nemishonga yezvipembenene.Pasina kugadzirisa nguva yekuratidzwa, iyo meso-scale kuyedza uye yakazara data yeECOTOX dhatabhesi yakaratidza kuti yakawanda taxa yakaonekwa ichinyanya kunzwisiswa nefipronil makomisheni pane yakadirwa Clostridium (Mufananidzo S6).Zvisinei, nekugadzirisa nguva yekutarisana, Dilution Clostridium ndiyo inonyanya kuoma kune fipronil (mubereki) uye sulfide, kunyange zvazvo isinganzwisisi sulfone (Mufananidzo S7).Mhedzisiro iyi inoratidza kukosha kwekusanganisa marudzi akawanda ezvipukanana zvemumvura (kusanganisira tumbuyu twakawanda) kugadzira mijenya chaiyo inogona kudzivirira zvipukanana zvemumvura.
Iyo SSD nzira inogona kuchengetedza isingawanzo kana kusanzwa mutero ine EC50 isingagone kutsanangurwa, senge Cinygmula sp., Isoperla fulva uye Brachycentrus americanus.Iyo EC50 tsika dze taxa kuwanda uye inogona kubhururuka yakawanda inoratidza shanduko mukuumbwa kwenharaunda inoenderana neHC50 kukosha kweSSD yefipronil, sulfone uye sulfide.Iyo protocol inotsigira zano rinotevera: Iyo SSD nzira inoshandiswa kutora zvikumbaridzo inogona kuchengetedza nharaunda yese, kusanganisira isingawanzo kana kusanzwa mutero munharaunda.Mukumbaridzo wezvipenyu zvemumvura zvakatemerwa kubva kumaSDD zvichibva pamitero mishoma kana kusanzwa mutero unogona kunge usina kukwana mukuchengetedza zvipenyu zvemumvura.Iyi ndiyo nyaya ye desulfinyl (Mufananidzo S6B).Nekuda kwekushaikwa kwe data muECOTOX dhatabhesi, iyo EPA isingaperi invertebrate baseline concentration ndeye 10,310 ng/L, iyo ine mirairo ina yehukuru hwakakwirira kupfuura 3.55 ng/L yeHC5.Mhedzisiro yeakasiyana taxon mhinduro seti inogadzirwa mumesoscopic kuyedza.Kushaikwa kwedhata rehuchetura kunonyanya kunetsa kune zvinoshatisa makomisheni (Figure S6), izvo zvinogona kutsanangura kuti nei iripo yemvura biological benchmarks ye sulfone uye sulfide ingaita 15 kusvika 30 nguva isinganyanyi kunzwa pane iyo SSD HC5 kukosha kwakavakirwa paChina Universe.Mukana weiyo yepakati membrane nzira ndeyekuti akawanda EC50 maitiro anogona kutariswa mune imwechete kuyedza, iyo inokwana kuumba yakazara SSD (semuenzaniso, desulfinyl; Mufananidzo 4B uye Figures S6B uye S7B), uye ine yakakosha kukanganisa. pamutero wechisikigo weiyo yakachengetedzwa ecosystem Mhinduro zhinji.
Zviyedzo zveMesoscopic zvinoratidza kuti fipronil uye zvigadzirwa zvayo zvekudzikisira zvinogona kuve nemhedzisiro yakaipa uye isina kunanga yakashata pakuita kwenharaunda.Muchiyedzo chemesoscopic, ese mashanu efipronil makomisheni akaonekwa achikanganisa kubuda kwezvipembenene.Migumisiro yekufananidza pakati pepamusoro uye yakaderera zvakanyanya (kudzivisa uye kukurudzirwa kwekubuda kwega kana kuchinja munguva yekubuda) inopindirana nemigumisiro yakambotaurwa yekuongorora kwemeso uchishandisa insecticide bifenthrin (29).Kubuda kwevanhu vakuru kunopa mabasa anokosha ezvakatipoteredza uye zvinogona kuchinjwa nezvinosvibisa zvakadai sefipronil (55, 56).Kubuda panguva imwe chete hakungokoshese kubereka kwezvipembenene uye kuenderera mberi kwehuwandu, asiwo nekupihwa kwezvipembenene zvakura, izvo zvinogona kushandiswa sechikafu chemhuka dzemvura uye dzepasi (56).Kudzivirira kubuda kwemhodzi kunogona kukanganisa kuchinjana kwechikafu pakati pezvipenyu zvemumvura uye zvipenyu zvemumvura, uye kuparadzira mhedzisiro yezvinosvibisa mumvura munzvimbo dzepasi (55, 56).Kuderera kwehuwandu hwezvipembenene (zvipembenene zvinodya algae) zvakaonekwa mukuedza kwemeso-scale zvakaguma nekuderera kwekushandiswa kwealgae, izvo zvakakonzera kuwedzera kwechlorophyll a (Mufananidzo 3).Iyi trophic cascade inoshandura iyo kabhoni uye nitrogen inoyerera mune yemvura chikafu webhu, yakafanana neongororo yakaongorora mhedzisiro yepyrethroid bifenthrin munharaunda dzebenthic (29).Nokudaro, phenylpyrazoles, yakadai sefipronil uye zvigadzirwa zvayo zvinosvibisa, pyrethroids, uye zvichida mamwe marudzi emishonga inouraya zvipembenene, inogona kukurudzira nenzira isina kunanga kuwedzera kwealgal biomass uye kukanganisa kwekabhoni nenitrogen muhova duku.Zvimwe zvinokanganisa zvinogona kuwedzera kusvika pakuparadzwa kwekabhoni nenitrogen kutenderera pakati pezvipenyu zvemumvura nepasi.
Ruzivo rwakawanikwa kubva muyedzo yemembrane yepakati rwakatibvumira kuti tiongorore kukosha kwezvakatipoteredza zvefipronil mukomboni wakayerwa muzvidzidzo zvakakura zvakaitwa mumatunhu mashanu eUnited States.Mune 444 nzizi diki, 17% yeavhareji yekusangana kweimwe kana kupfuura fipronil komisheni (avhareji pamusoro pemavhiki e4) yakapfuura kukosha kweHC5 yakawanikwa kubva mukuedzwa kwenhau.Shandisa iyo SSD kubva pameso-scale kuyedza kushandura yakayerwa fipronil mukomboni concentration kuita toxicity-inoenderana index, kureva, huwandu hwehuturu hwezvikamu (ΣTUFipronils).Kukosha kwe1 kunoratidza huturu kana kuwanda kwekuratidzwa kwefipronil komputa inodarika iyo inozivikanwa dziviriro Mhando dzinokosha 95%.Ukama hwakakosha pakati pe ΣTUFipronil muzvikamu zvina zvezvishanu uye SPEARpesticides chiratidzo che invertebrate munharaunda hutano hunoratidza kuti fipronil inogona kukanganisa nharaunda dze benthic invertebrate munzizi munzvimbo dzakawanda dzeUnited States.Iyi mhedzisiro inotsigira hypothesis yeWolfram et al.(3) Ngozi yezvipembenene zve phenpyrazole kumvura yepamusoro muUnited States hainyatsonzwisiswi nokuti kukanganisa kwezvipembenene zvemvura kunoitika pasi pechikumbaridzo chezvino chekutonga.
Hova zhinji dzine fipronil zviri pamusoro pechepfu dziri munzvimbo ine maguta ekumaodzanyemba kwakadziva kumabvazuva (https://webapps.usgs.gov/rsqa/#!/region/SESQA).Kuongororwa kwekare kwenzvimbo yacho hakuna kungogumisa kuti fipronil ndiyo inonyanya kunetseka inobata invertebrate community structure murukova, asiwo iyo yakaderera yakanyunguduka okisijeni, yakawedzera kudya kunovaka muviri, kuyerera kwekuchinja, kuparara kwenzvimbo, uye zvimwe zvinouraya zvipembenene uye Chikamu chinosvibisa chinhu chakakosha. tsime rekushushikana (57).Uyu musanganiswa wezvinonetsa unopindirana ne "urban river syndrome", inova iyo kuparara kwenzizi ecosystems inowanzoonekwa maererano nekushandiswa kwenzvimbo yemaguta (58, 59).Zviratidzo zvekushandiswa kwevhu mumadhorobha mudunhu reSoutheast zviri kukura uye zvinotarisirwa kuwedzera sezvo huwandu hwenzvimbo iyi huri kukura.Mhedzisiro yekuvandudzwa kwemaguta mune ramangwana uye mishonga yekuuraya zvipembenene pakufamba kwemaguta inotarisirwa kuwedzera (4).Kana kuguta kwemaguta uye kushandiswa kwefipronil kuchiramba kuchikura, kushandiswa kwemushonga uyu mumaguta kunogona kuwedzera kukanganisa nharaunda dzinoyerera.Kunyangwe iyo meta-kuongorora ichigumisa kuti kushandiswa kwemishonga yekurima kunotyisidzira mafambiro epasi rose (2, 60), isu tinofungidzira kuti ongororo idzi dzinorerutsa kukanganiswa kwepasi rose kwemishonga yekuuraya zvipembenene nekusabatanidza kushandiswa kwemaguta.
Zvinetso zvakasiyana-siyana, kusanganisira mishonga yezvipembenene, zvinogona kukanganisa macroinvertebrate nharaunda munzvimbo dzakasimukira dzemvura (mumaguta, yekurima uye yakasanganiswa kushandiswa kwevhu) uye inogona kunge ine chekuita nekushandiswa kwenyika (58, 59, 61).Kunyangwe chidzidzo ichi chakashandisa chiratidzo cheSPEARpesticides uye zvisikwa zvemumvura-zvakananga fipronil toxicity maitiro kuti kuderedze kukanganisa kwezvinhu zvinovhiringidza, kuita kwechiratidzo cheSPEARpesticides kunogona kukanganiswa nekuparara kwenzvimbo, uye fipronil inogona kuenzaniswa nedzimwe Pesticide ine hukama (4, 17, 51, 57).Zvisinei, maitiro akawanda ekudzvinyirira akagadzirwa achishandisa zviyero zvemumunda kubva kuzvidzidzo zviviri zvekutanga zvenharaunda (Midwestern neSoutheastern) zvakaratidza kuti mishonga yezvipembenene inokosha kumusoro kwepamusoro kwemamiriro emunharaunda macroinvertebrate munzizi dzinoyerera.Mune aya mamodheru, akakosha anotsanangura akasiyana anosanganisira mishonga yezvipembenene (kunyanya bifenthrin), chikafu uye hunhu hwekugara muhova zhinji dzekurima muMidwest, uye mishonga yezvipembenene (kunyanya fipronil) mumaguta mazhinji kumaodzanyemba kwakadziva kumabvazuva.Kuchinja kweokisijeni, zvinovaka muviri uye kuyerera (61, 62).Nokudaro, kunyange zvazvo zvidzidzo zvemunharaunda zvichiedza kugadzirisa kukanganisa kwevasina-pesticide stressors pane zviratidzo zvekupindura uye kugadzirisa zviratidzo zvekufungidzira kutsanangura kukanganisa kwefipronil, migumisiro yemunda yeongororo iyi inotsigira maonero efipronil.) Inofanirwa kutorwa seimwe yeanonyanya kupesvedzera manyuko ekumanikidzwa munzizi dzeAmerica, kunyanya kumaodzanyemba kwakadziva kumabvazuva kweUnited States.
Kuitika kwekuparara kwemishonga yezvipembenene munharaunda hakuwanzonyorwa, asi kutyisidzira kune zvipenyu zvemvura kunogona kukuvadza kudarika muviri wemubereki.Panyaya yefipronil, zvidzidzo zvemumunda uye ma-meso-scale zviyedzo zvakaratidza kuti zvigadzirwa zvekudzikisira zvakajairwa semuviri wemubereki mumasampled hova uye zvine muchetura wakafanana kana wepamusoro (Tafura 1).Muyedzo yemembrane yepakati, fluorobenzonitrile sulfone ndiyo yainyanya huturu hwezvigadzirwa zvekuparadza zvipembenene zvakadzidzwa, uye yakanga ine muchetura kupfuura musanganiswa wevabereki, uye yakaonekwawo pafrequency yakafanana neyemukomboni yemubereki.Kana chete mishonga yezvipembenene yevabereki ikayerwa, zvinogona kuitika muchetura zvinogona kusaonekwa, uye kushaikwa kweruzivo rwehupfu panguva yekuderedzwa kwezvipembenene zvinoreva kuti kuitika kwavo nemhedzisiro yavo inogona kufuratirwa.Semuenzaniso, nekuda kwekushaikwa kweruzivo pamusoro pehupfu hwezvigadzirwa zvinoshatisa, ongororo yakazara yemishonga yezvipembenene muSwiss streams yakaitwa, kusanganisira 134 zvigadzirwa zvekuparadza zvipembenene, uye chete musanganiswa wevabereki ndiwo waionekwa semusanganiswa wemubereki mukuongorora kwayo njodzi ye ecotoxicological.
Mhedzisiro yeiyi ecological njodzi yekuongorora inoratidza kuti fipronil makomisheni ane mhedzisiro yakaipa pahutano hwerwizi, saka zvinogona kutaurwa zvine musoro kuti mhedzisiro inogona kucherechedzwa chero kupi uko fipronil makomisheni anopfuura chiyero cheHC5.Mhedzisiro yezviyedzo zvemesoscopic yakazvimirira pane nzvimbo, zvichiratidza kuti kusungirirwa kwefipronil uye zvigadzirwa zvayo zvekushatisa mune yakawanda stream taxa yakadzikira zvakanyanya pane yakamborekodhwa.Isu tinotenda kuti kuwanikwa uku kungangowedzerwa kune protobiota mune pristine hova chero kupi.Migumisiro yekuedza kwemeso-scale yakashandiswa kune zvidzidzo zvemunda zvakakura (444 nzizi diki dzinoumbwa nemaguta, ekurima, uye kushandiswa kwevhu kwakasanganiswa kumatunhu makuru mashanu muUnited States), uye zvakaonekwa kuti kuungana kwehova dzakawanda. uko fipronil yakaonekwa inotarisirwa kuve Iyo inokonzeresa chepfu inoratidza kuti mhedzisiro iyi inogona kuwedzera kune dzimwe nyika uko fipronil inoshandiswa.Maererano nemishumo, nhamba yevanhu vanoshandisa Fipronil iri kuwedzera muJapan, UK uye US (7).Fipronil iripo munenge makondinendi ese, kusanganisira Australia, South America neAfrica (https://coherentmarketinsights.com/market-insight/fipronil-market-2208).Mhedzisiro yeongororo yemeso-to-munda yakapihwa pano inoratidza kuti kushandiswa kwefipronil kunogona kuve nekukosha kwezvakatipoteredza pasi rose.
Zvekuwedzera zvechinyorwa chino, ndapota ona http://advances.sciencemag.org/cgi/content/full/6/43/eabc1299/DC1
Ichi chinyorwa chekuwana chakavhurika chakagoverwa pasi pemitemo yeCreative Commons Attribution-Non-Commercial License, iyo inobvumira kushandiswa, kugovera uye kubereka mune chero svikiro, chero bedzi kushandiswa kwekupedzisira kusiri kwekutsvaga kwekutengesa uye chirevo ndechekuti basa rekutanga rakarurama.Reference.
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Janet L. Miller, Travis S. Schmidt, Peter C. Van Metre, Barbara Mahler ( Barbara J. Mahler, Mark W. Sandstrom, Lisa H. Nowell, Daren M. Carlisle, Patrick W. Moran
Zvidzidzo zvakaratidza kuti mishonga inouraya zvipembenene iyo inowanzoonekwa muhova dzeAmerica ine muchetura kupfuura zvaimbofungwa.
Janet L. Miller, Travis S. Schmidt, Peter C. Van Metre, Barbara Mahler ( Barbara J. Mahler, Mark W. Sandstrom, Lisa H. Nowell, Daren M. Carlisle, Patrick W. Moran
Zvidzidzo zvakaratidza kuti mishonga inouraya zvipembenene iyo inowanzoonekwa muhova dzeAmerica ine muchetura kupfuura zvaimbofungwa.
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