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        新農(nóng)藥哌蟲(chóng)啶在三種典型土壤中的吸附與淋溶研究*

        2017-02-23 05:50:34慧王杜曉敏李現(xiàn)旭劉
        土壤學(xué)報(bào) 2017年1期
        關(guān)鍵詞:棕壤土壤改良劑淋溶

        謝 慧王 軍?杜曉敏李現(xiàn)旭劉 陽(yáng)

        (1 山東農(nóng)業(yè)大學(xué)資源與環(huán)境學(xué)院,山東省高校農(nóng)業(yè)環(huán)境重點(diǎn)實(shí)驗(yàn)室,山東泰安 271018)

        (2 土肥資源高效利用國(guó)家工程實(shí)驗(yàn)室,山東農(nóng)業(yè)大學(xué)資源與環(huán)境學(xué)院,山東泰安 271018)

        新農(nóng)藥哌蟲(chóng)啶在三種典型土壤中的吸附與淋溶研究*

        謝 慧1,2王 軍1,2?杜曉敏1李現(xiàn)旭1劉 陽(yáng)1

        (1 山東農(nóng)業(yè)大學(xué)資源與環(huán)境學(xué)院,山東省高校農(nóng)業(yè)環(huán)境重點(diǎn)實(shí)驗(yàn)室,山東泰安 271018)

        (2 土肥資源高效利用國(guó)家工程實(shí)驗(yàn)室,山東農(nóng)業(yè)大學(xué)資源與環(huán)境學(xué)院,山東泰安 271018)

        應(yīng)用振蕩平衡法和柱淋洗法研究了哌蟲(chóng)啶在紅壤、棕壤和黑土3種典型土壤中的吸附和淋溶特性,并探討了3種土壤改良劑對(duì)其淋溶的影響。結(jié)果表明:哌蟲(chóng)啶在黑土、紅壤和棕壤中的吸附平衡時(shí)間分別為12、12和9 h,分配系數(shù)Kd分別為23.16、11.24和4.68,吸附常數(shù)Kf分別為22.03、11.69 和5.05,KOC值分別為1 619、2 094和495,吸附自由能值分別為-16.96、-17.59和-14.02 kJ mol-1,F(xiàn)reundlich和線性等溫吸附模型均能較好地描述哌蟲(chóng)啶在土壤中的吸附過(guò)程,其吸附能力順序分別為黑龍江黑土>福建紅壤>山東棕壤。哌蟲(chóng)啶在3種供試土壤中淋溶性存在差異,在棕壤中遷移性最強(qiáng),隨著施藥量的增加,其淋出率也略有提高,但3個(gè)不同水平施藥量差異不顯著。在黑土中遷移性最弱,紅壤和黑土中的哌蟲(chóng)啶殘留量隨著土壤深度的增加逐漸降低。土壤中添加0.5%的活性炭、腐殖酸和草炭能顯著地降低農(nóng)藥哌蟲(chóng)啶在土壤中的淋溶性,減少對(duì)地下水的污染風(fēng)險(xiǎn)。

        新煙堿類殺蟲(chóng)劑;哌蟲(chóng)啶;吸附;淋溶;土壤改良劑

        哌蟲(chóng)啶為國(guó)內(nèi)第一個(gè)新煙堿類殺蟲(chóng)劑創(chuàng)制品種,化學(xué)名稱為:1-((6-氯吡啶-3-基)甲基)-5-丙氧基-7-甲基-8-硝基-1,2,3,5,6,7-六氫咪唑[1,2-a]吡啶,由上海華東理工大學(xué)和江蘇克勝集團(tuán)股份有限公司于2008年聯(lián)合開(kāi)發(fā),主要用于防治同翅目害蟲(chóng)[1]。哌蟲(chóng)啶具有很好的內(nèi)吸傳導(dǎo)功能,是替代吡蟲(chóng)啉和毒死蜱等防治稻、麥等作物的飛虱類害蟲(chóng)新農(nóng)藥[2-3]。在當(dāng)今吡蟲(chóng)啉抗性不斷增長(zhǎng)的情況下,哌蟲(chóng)啶將成為一個(gè)很有發(fā)展前途的新穎殺蟲(chóng)劑[4]?,F(xiàn)有文獻(xiàn)報(bào)道主要集中在噻蟲(chóng)啉和吡蟲(chóng)啉等新煙堿類殺蟲(chóng)劑在土壤中環(huán)境行為的研究[5-6],以及哌蟲(chóng)啶在谷物和土壤中的殘留分析[7-8]和對(duì)植物毒性方面[9]的研究,而對(duì)于哌蟲(chóng)啶在土壤中的吸附和淋溶等環(huán)境行為的研究也具有十分重要的意義。

        農(nóng)藥一旦進(jìn)入土壤,將與土壤接觸發(fā)生吸附-解吸和淋溶作用。農(nóng)藥在土壤中的吸附-解吸被認(rèn)為是農(nóng)藥在土壤中歸宿的主要因素[10],它對(duì)農(nóng)藥在土壤中的化學(xué)、微生物降解、揮發(fā)及其淋溶等行為有著重要的影響[11],也是農(nóng)藥環(huán)境安全性評(píng)價(jià)的重要指標(biāo)。一般認(rèn)為土壤吸附農(nóng)藥的主要作用機(jī)理為:離子交換吸附、配位體交換吸附、范德華力、疏水性結(jié)合、氫鍵結(jié)合和電荷轉(zhuǎn)移[12-13]。農(nóng)藥的施用方式、施用用量及其理化性質(zhì)影響農(nóng)藥在土壤中的移動(dòng),土壤的理化性質(zhì)會(huì)影響哌蟲(chóng)啶異構(gòu)體在土壤中的降解和轉(zhuǎn)移[14-15]。而土壤改良劑能有效地改善土壤理化性狀,已有許多研究集中于改良劑修復(fù)重金屬污染土壤[16-17]。研究表明玉米芯生物炭作為土壤改良劑能提高2,4-D在土壤中的吸附量,降低其在土壤中的遷移性[18];草炭不僅能修復(fù)土壤中重金屬污染[19],還對(duì)油田陳化油泥具有較好的修復(fù)效果,并能提高土壤有機(jī)質(zhì)濃度[20]。本研究選用通氣透水性好、含有氨基酸、腐殖酸和氮磷鉀等多種養(yǎng)分的草炭,具有吸附多種有機(jī)污染物能力的腐殖酸[21-23]和活性炭3種土壤改良劑,研究3種土壤改良劑對(duì)哌蟲(chóng)啶在不同類型土壤中的淋溶性。哌蟲(chóng)啶作為我國(guó)重要的農(nóng)藥創(chuàng)制品種,研究其在土壤中的吸附和淋溶特性,對(duì)預(yù)測(cè)其在土壤中的環(huán)境行為及污染狀況具有重要意義。本研究采用振蕩平衡法和土柱淋溶實(shí)驗(yàn)系統(tǒng)地研究了哌蟲(chóng)啶在3種典型土壤中的吸附行為和遷移規(guī)律及3種土壤改良劑對(duì)哌蟲(chóng)啶在不同類型土壤中的淋溶性影響,為闡明哌蟲(chóng)啶在土壤中的遷移轉(zhuǎn)化規(guī)律,評(píng)價(jià)哌蟲(chóng)啶在土壤環(huán)境中的安全性,促進(jìn)合理施藥與避免對(duì)地下水的污染提供科學(xué)依據(jù)。

        1 材料與方法

        1.1 儀器與試劑

        安捷倫Agilent 1100液相色譜儀(配紫外檢測(cè)器),QHZ-98B全溫度振蕩培養(yǎng)箱(太倉(cāng)市華美生化儀器廠),TG16C/TG16高速離心機(jī)(英泰離心機(jī)),RE-52AA旋轉(zhuǎn)蒸發(fā)儀(上海亞榮生化儀器廠),QSE-12固相萃取儀(北京國(guó)譜科技有限公司)。

        哌蟲(chóng)啶為原藥,由江蘇克勝集團(tuán)提供,純度為93.30%。其余化學(xué)試劑均為分析純。三種改良劑:活性炭(分析純,上海聯(lián)試化工試劑有限公司)、腐殖酸(生化試劑,上海源葉生物科技有限公司)、自制草炭。

        實(shí)驗(yàn)所用棕壤采自山東農(nóng)業(yè)大學(xué)南校實(shí)驗(yàn)田,根據(jù)中國(guó)土壤系統(tǒng)分類命名為普通簡(jiǎn)育濕潤(rùn)淋溶土(Typic-Hapli-Udic Argosols)。紅壤來(lái)自福建省南平武夷山市,根據(jù)中國(guó)土壤系統(tǒng)分類命名為黏化富鋁濕潤(rùn)富鐵土(Argi-Allit-Udic Ferrosols);黑土取自黑龍江省齊齊哈爾市,根據(jù)中國(guó)土壤系統(tǒng)分類命名為黏化濕潤(rùn)均腐土(Argi-Udic Isohumosols)。采取表層土壤(0~20 cm),土壤樣品剔除去其中的石塊、植物枝葉等雜物,自然風(fēng)干,研碎后過(guò)篩備用。土壤的基本理化性質(zhì)如表1。

        1.2 吸附動(dòng)力學(xué)試驗(yàn)

        稱取10.00 g供試土壤(過(guò)60目篩),加入采用0.01 mol L-1CaCl2配制的哌蟲(chóng)啶溶液50 ml,使溶液中哌蟲(chóng)啶濃度為2.0 mg L-1,再加入少量氯化汞作為生物殺滅劑(100 mg L-1)。在振蕩器上充分振蕩,轉(zhuǎn)速為200 r min-1,溫度控制在(25±0.1)℃。吸附時(shí)間設(shè)定 0、0.5、1、3、 5、7、9、12和14 h,同時(shí)設(shè)置3個(gè)重復(fù)和兩個(gè)對(duì)照(加藥不加土,加土不加藥)。振蕩完成后以9 000 r min-1的速度離心10 min,每次振蕩后取2 ml上層清液通過(guò)0.22 μm的水系濾膜過(guò)濾,測(cè)定水相中哌蟲(chóng)啶的濃度。同時(shí)計(jì)算分配系數(shù)Kd:

        表1 供試土壤理化性質(zhì)Table 1 Physical and chemical properties of the 3 tested soils

        式中,Ce為水相中哌蟲(chóng)啶濃度(mg L-1);Cs為土壤中哌蟲(chóng)啶濃度(mg kg-1)。

        哌蟲(chóng)啶在土壤中的吸附濃度Cs,通過(guò)以下公式計(jì)算:

        式中,C0為對(duì)照水相中的農(nóng)藥濃度(mg L-1);Ce為吸附平衡時(shí)水相中的農(nóng)藥濃度(mg L-1);V為水相體積(L);m為所加土壤質(zhì)量(kg)。

        1.3 吸附等溫實(shí)驗(yàn)

        分別設(shè)置5個(gè)哌蟲(chóng)啶濃度處理:0.05、0.1、0.5、2.0和5 mg L-1,于25℃條件下恒溫振蕩由吸附動(dòng)力學(xué)測(cè)定的平衡時(shí)間后,然后以9 000 r min-1的速度離心10 min,上層清液通過(guò)0.22 μm的水系濾膜過(guò)濾,測(cè)定水相中哌蟲(chóng)啶的濃度(Ce)。采用線性模型和Freundlich兩種吸附等溫方程式擬合求得分配系數(shù)Kd與吸附常數(shù)Kf。據(jù)此計(jì)算土壤有機(jī)碳吸附常數(shù)KOC、有機(jī)質(zhì)吸附常數(shù)KOM及土壤對(duì)農(nóng)藥吸附的自由能變化ΔG。

        1.4 土柱淋溶實(shí)驗(yàn)設(shè)計(jì)

        參照《化學(xué)農(nóng)藥環(huán)境安全評(píng)價(jià)試驗(yàn)準(zhǔn)則》[24]制備淋溶土柱,黑土、紅壤和棕壤容重分別為1.05、1.26和1.48 g cm-3,稱取1 400 g(準(zhǔn)確至0.1 g)過(guò)2 mm篩的土壤,裝于聚乙烯塑料管(內(nèi)徑8 cm、總長(zhǎng)40 cm)中,制成30 cm高的土柱,土壤柱填充完畢后,由下至上利用0.01 mol L-1氯化鈣溶液反滲透法使土柱中水分達(dá)到飽和,趕去土柱中存在的空氣。試驗(yàn)前,利用重力作用,濾去多余水分。在溫度為(18~25 ℃,±2 ℃)避光條件下,按照200 μg(棕壤為100 μg)、250 μg和500 μg 3個(gè)不同水平施藥量將農(nóng)藥哌蟲(chóng)啶均勻拌入10 g 3種不同類型的土壤中,然后讓土壤均勻覆蓋在土柱頂部,靜置24 h使農(nóng)藥與土壤吸附達(dá)到平衡。試驗(yàn)開(kāi)始時(shí),土柱頂部覆蓋0.5 cm厚石英砂,然后模擬降雨,用0.01 mol L-1氯化鈣溶液進(jìn)行淋溶。淋溶時(shí),利用輸液器裝置的調(diào)節(jié)閥控制氯化鈣溶液的流速(30 ml h-1),使相當(dāng)于300 ml降雨量的水在10 h內(nèi)勻速地通過(guò)土壤柱,收集淋出液。淋洗完畢后,將土柱均勻分成0~10、10~20、20~30 cm 3段,首先測(cè)定每段土壤的總質(zhì)量,混勻后分別測(cè)定各段土壤及淋出液中的哌蟲(chóng)啶含量,同時(shí)測(cè)定土壤含水量。每個(gè)處理設(shè)3個(gè)重復(fù)。

        選定250 μg施藥量一個(gè)施藥水平,分別添加0.5%的活性炭、腐殖酸和草炭3種土壤改良劑后按同樣的方法進(jìn)行淋溶實(shí)驗(yàn),每種土壤改良劑設(shè)置3個(gè)平行。

        1.5 哌蟲(chóng)啶的前處理方法和測(cè)定條件

        土壤中哌蟲(chóng)啶的前處理方法已經(jīng)建立,參照文獻(xiàn)[25]方法進(jìn)行。哌蟲(chóng)啶殘留量測(cè)定采用HPLC方法,條件為:色譜柱:C18柱:5 μm,25 cm×4.6 mm;流動(dòng)相:乙腈∶水=40∶60(V/V);流速:1.0 ml min-1;檢測(cè)波長(zhǎng):359 nm;柱溫:30℃;進(jìn)樣:10 μl。

        淋出液中哌蟲(chóng)啶濃度較低,采用SPE濃縮凈化方法。SampliQ C18固相萃取小柱先用5 ml甲醇預(yù)淋小柱,再用5 ml蒸餾水預(yù)淋至干。將淋出液樣品轉(zhuǎn)移至柱中,采用SampliQ C18固相萃取小柱濃縮凈化淋出液,用25 ml乙腈(每次加入5 ml)洗脫樣品,小柱的流速為不超過(guò)1 ml min-1,收集洗脫液,氮?dú)獯蹈?,用乙腈定容?0 ml刻度試管中,經(jīng)0.22 μm有機(jī)相濾膜過(guò)濾后,用HPLC檢測(cè),測(cè)定條件同土壤樣品。

        1.6 數(shù)據(jù)處理和分析

        各處理間的差異性采用SPSS 20.0數(shù)據(jù)統(tǒng)計(jì)軟件進(jìn)行方差分析,利用單因素方差分析(ANOVA)對(duì)各處理總體均數(shù)的差異進(jìn)行顯著性檢驗(yàn);圖采用Sigmaplot 10.0繪制。

        2 結(jié)果與討論

        2.1 哌蟲(chóng)啶在不同類型土壤中的吸附

        哌蟲(chóng)啶在3種土壤中的吸附動(dòng)力學(xué)曲線如圖1所示。采用線性模型和Freundlich等溫吸附方程式對(duì)實(shí)驗(yàn)數(shù)據(jù)進(jìn)行擬合,相關(guān)參數(shù)見(jiàn)表2。

        由圖1可知,哌蟲(chóng)啶在黑土、紅壤和棕壤的吸附平衡時(shí)間分別為12、12和9 h。哌蟲(chóng)啶在黑土、紅壤和棕壤中的分配系數(shù)(Kd)分別為23.16、11.24和4.68(表2),說(shuō)明哌蟲(chóng)啶在黑土介質(zhì)中的土壤-水體系中的分配作用最強(qiáng),在棕壤中最弱。

        哌蟲(chóng)啶在黑土、紅壤和棕壤中的吸附常數(shù)Kf分別為22.03、11.69和5.05,其吸附能力分別為黑龍江黑土>福建紅壤>山東棕壤。通過(guò)吸附等溫線,可以了解土壤與農(nóng)藥哌蟲(chóng)啶之間的相互作用關(guān)系,以及界面上吸附分子的狀態(tài)。使用最廣泛的吸附等溫線類型為線性模型、Langmuir和Freundlich3種等溫吸附模型,大多數(shù)農(nóng)藥在土壤中的吸附符合Freundlich吸附等溫式,從兩模型對(duì)吸附的擬合參數(shù)r可見(jiàn),F(xiàn)reundlich吸附模型和線性模型均能較好地描述哌蟲(chóng)啶在土壤中的吸附過(guò)程。

        圖1 哌蟲(chóng)啶在3種土壤中的吸附動(dòng)力學(xué)(C0= 2 mg L-1)Fig. 1 Adsorption dynamics of IPP 2 mg L-1in concentration in the three soils

        土壤有機(jī)碳吸附常數(shù)KOC作為評(píng)價(jià)土壤對(duì)有機(jī)物吸附能力的一個(gè)指標(biāo),研究表明,有機(jī)物在土壤中的分配系數(shù)與有機(jī)質(zhì)含量成正相關(guān),有機(jī)質(zhì)對(duì)疏水性有機(jī)物的吸附起著主要的作用。土壤吸附自由能是反映土壤吸附性能的重要參數(shù)。本實(shí)驗(yàn)3種典型土壤對(duì)哌蟲(chóng)啶的有機(jī)碳吸附常數(shù)和吸附自由能如表3。

        哌蟲(chóng)啶在本試驗(yàn)黑土、紅壤和棕壤中的KOC值分別為1 619、2 094和495,根據(jù)《化學(xué)農(nóng)藥環(huán)境安全評(píng)價(jià)試驗(yàn)準(zhǔn)則》,哌蟲(chóng)啶在供試土壤紅壤和黑土中的吸附性較強(qiáng),在棕壤中吸附性較弱。供試土壤對(duì)哌蟲(chóng)啶吸附自由能值分別為-16.96、-17.59 和-14.02 kJ mol-1,哌蟲(chóng)啶在3種土壤中的自由能絕對(duì)值均小于40 kJ mol-1,則可知哌蟲(chóng)啶在這3種土壤中屬于物理性吸附,物理性吸附的平衡速度較快,吸附是可逆過(guò)程。

        研究表明,土壤有機(jī)質(zhì)含量對(duì)農(nóng)藥在土壤中的吸附影響較大,比如噻蟲(chóng)啉[26-27]、噻蟲(chóng)胺[27]、吡蟲(chóng)啉[28]、咪唑乙煙酸[29]、啶蟲(chóng)脒[30]和氟啶胺[31]吸附常數(shù)與土壤有機(jī)質(zhì)含量呈顯著正相關(guān)。但土壤的理化性質(zhì)對(duì)烯啶蟲(chóng)胺在土壤中吸附的影響極小,這是由于烯啶蟲(chóng)胺的水溶性極強(qiáng)(水溶解度達(dá)840 g L-1,20℃),農(nóng)藥的水溶性成為影響其吸附性的主導(dǎo)因素[32]。而土壤對(duì)阿維菌素的吸附特性和土壤黏粒相關(guān)[33]。農(nóng)藥在土壤中的吸附影響因素主要是由農(nóng)藥理化性質(zhì)和土壤有機(jī)質(zhì)含量決定的,而土壤pH、黏粒含量及其鐵鋁氧化物含量也影響農(nóng)藥在土壤中的吸附和遷移,農(nóng)藥在土壤中的行為是所有理化性質(zhì)綜合作用的結(jié)果。而哌蟲(chóng)啶易溶于有機(jī)溶劑乙腈和土壤中的二氯甲烷,在水中溶解度較小(0.61 g L-1,20℃),哌蟲(chóng)啶的理化性質(zhì)決定了其在土壤中的吸附和土壤有機(jī)質(zhì)含量及土壤黏粒具有較強(qiáng)的相關(guān)性,土壤有機(jī)質(zhì)含量和黏粒含量最高的黑土吸附能力最強(qiáng),黏粒含量較高的紅壤土吸附能力次之,山東棕壤雖然有機(jī)質(zhì)含量高于紅壤,但黏粒含量最低,其對(duì)哌蟲(chóng)啶的吸附能力最弱。

        表2 哌蟲(chóng)啶在3種土壤中的吸附模型參數(shù)Table 2 Parameters of the adsorption models for IPP in the three soils(25℃)

        表3 哌蟲(chóng)啶在3種土壤中的有機(jī)碳吸附常數(shù)和吸附自由能Table 3 KOCand ΔG of IPP in the three soils

        2.2 施藥量對(duì)哌蟲(chóng)啶在不同類型土壤中淋溶遷移的影響

        施藥量對(duì)哌蟲(chóng)啶在棕壤、紅壤和黑土中淋溶遷移的影響如表4。

        由表4可知,哌蟲(chóng)啶在棕壤中隨著施藥量的增加,其淋出率也略有提高,但3個(gè)不同水平施藥量差異不顯著;隨著土壤深度的增加,農(nóng)藥殘留量逐漸降低,說(shuō)明哌蟲(chóng)啶在棕壤中具有一定的移動(dòng)性,但遷移性不強(qiáng)。施藥量對(duì)哌蟲(chóng)啶在紅壤和黑土中的淋出率影響也不大,在所測(cè)試的3個(gè)施藥量下,僅有200 μg和500 μg施藥處理在紅壤中的淋出率差異顯著(p<0.05),而黑土中的淋出率雖然隨著施藥量的增加略有變化,但差異不顯著。紅壤和黑土中的哌蟲(chóng)啶殘留量隨著土壤深度的增加也逐漸降低,但降低幅度不大,說(shuō)明哌蟲(chóng)啶在紅壤和黑土中吸附性較強(qiáng),移動(dòng)性較弱。

        表4 施藥量對(duì)哌蟲(chóng)啶在3種土壤中淋溶遷移的影響Table 4 Effects of dosage on leaching of paichongding in the three soils

        哌蟲(chóng)啶在3種供試土壤中淋溶性存在差異。其中在棕壤中易發(fā)生垂直方向的遷移,其淋出液中哌蟲(chóng)啶含量高于其他兩種土壤;在黑土中垂直方向的遷移能力最弱,其淋出液中哌蟲(chóng)啶含量低于其他兩種土壤。棕壤、紅壤和黑土中淋出液中哌蟲(chóng)啶所占總量的百分比分別為:16.69%~16.86%、11.55%~13.52%、8.98%~9.35%。說(shuō)明哌蟲(chóng)啶在棕壤中吸附性最弱,遷移性最強(qiáng);在黑土中吸附性最強(qiáng),遷移性最弱,本研究結(jié)果與前面吸附性研究結(jié)論一致。

        Kurwadkar等[6]研究了3種新煙堿類殺蟲(chóng)劑在葡萄園土壤中的淋溶性,研究結(jié)果表明其淋溶性強(qiáng)弱和農(nóng)藥的水溶性有很強(qiáng)的相關(guān)性,吡蟲(chóng)啉、噻蟲(chóng)嗪和呋蟲(chóng)胺在水中溶解度分別為610、4 100和39 830 mg L-1,而淋溶性強(qiáng)弱為吡蟲(chóng)啉<噻蟲(chóng)嗪<呋蟲(chóng)胺,即土壤類型相同的條件下,水溶性越強(qiáng),淋溶性越強(qiáng),而哌蟲(chóng)啶在水中溶解度為610 mg L-1(20℃),與吡蟲(chóng)啉相近,屬于水溶性較差的農(nóng)藥,它在土壤中的淋溶性亦較小。本研究結(jié)論和文獻(xiàn)報(bào)道結(jié)果相符。雖然吡蟲(chóng)啉和哌蟲(chóng)啶均屬于新煙堿類農(nóng)藥,但是吡蟲(chóng)啉在土壤中的吸附主要是有機(jī)質(zhì)的作用,不是土壤黏粒的作用[34-35],哌蟲(chóng)啶在土壤中的吸附則和土壤黏粒含量具有較好的相關(guān)性。

        2.3 土壤改良劑對(duì)哌蟲(chóng)啶在不同類型土壤中的淋溶性影響

        加入土壤改良劑后,哌蟲(chóng)啶在棕壤、紅壤和黑土中的淋溶遷移結(jié)果如表5。

        由表5可知,3種類型土壤中添加土壤改良劑均能顯著地影響哌蟲(chóng)啶的遷移性。在土壤中添加活性炭后不僅顯著地降低了哌蟲(chóng)啶在土壤中的遷移性和淋出量,而且降低了土壤中可提取態(tài)殘留,土壤中可提取態(tài)殘留在3種土壤中分別降低了34.8%、36.79%和16.93%;紅壤和黑土中均未檢出淋出量,而棕壤中淋出量較未加活性炭的土壤也顯著降低了74.6%。棕壤中添加0.5%的腐殖酸和草炭后,哌蟲(chóng)啶的淋出量分別減少了25.1%和17.1%,紅壤添加腐殖酸和草炭后,哌蟲(chóng)啶的淋出量分別減少了29.7%和23.3%,而黑土中添加相同量的腐殖酸和草炭后,哌蟲(chóng)啶的淋出量分別減少了42.1%和27.6%。

        表5 土壤改良劑對(duì)哌蟲(chóng)啶在3種土壤中淋溶遷移的影響Table 5 Effects of soil amendments on leaching of paichongding in the three soils

        土壤改良劑不僅影響土壤肥力和土壤的理化性質(zhì),而且還影響污染物在土壤中的環(huán)境化學(xué)行為,文獻(xiàn)表明添加土壤改良劑能延阻污染物在土壤中的淋溶遷移[36-40],本研究結(jié)果表明土壤中添加0.5%的活性炭、腐殖酸和草炭均能顯著地降低農(nóng)藥哌蟲(chóng)啶在土壤中的淋溶性,減少對(duì)地下水的污染風(fēng)險(xiǎn)。

        3 結(jié) 論

        應(yīng)用振蕩平衡法研究了新煙堿類殺蟲(chóng)劑哌蟲(chóng)啶在紅壤、棕壤和黑土中吸附特性。哌蟲(chóng)啶在黑土、紅壤和棕壤中的吸附能力為黑龍江黑土>福建紅壤>山東棕壤。Freundlich和線性等溫吸附模型均能較好地描述哌蟲(chóng)啶在土壤中的吸附過(guò)程。哌蟲(chóng)啶的理化性質(zhì)決定了其在土壤中的吸附和土壤有機(jī)質(zhì)含量及其土壤黏粒具有較強(qiáng)的相關(guān)性。哌蟲(chóng)啶在3種供試土壤中淋溶性存在差異,在棕壤中遷移性最強(qiáng),隨著施藥量的增加,其淋出率也略有提高,但3個(gè)不同水平施藥量差異不顯著;在黑土中吸附性最強(qiáng),遷移性最弱,紅壤和黑土中的哌蟲(chóng)啶殘留量隨著土壤深度的增加也逐漸降低,但降低幅度不大。土壤中添加0.5%的活性炭、腐殖酸和草炭能顯著地降低農(nóng)藥哌蟲(chóng)啶在土壤中的淋溶性,減少對(duì)地下水的污染風(fēng)險(xiǎn)。

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        Adsorption and Leaching of Paichongding a New Pesticide in Three Typical Soils

        XIE Hui1,2WANG Jun1,2?DU Xiaomin1LI Xianxu1LIU Yang1
        (1 College of Resources and Environment,Shandong Agricultural University,Key Laboratory of Agricultural Environment in Universities of Shandong,Tai’an,Shandong 271018,China)
        (2 National Engineering Laboratory for Efficient Utilization of Soil and Fertilizer Resources;College of Resources and Environment,Shandong Agricultural University,Tai’an,Shandong 271018,China)

        【Objecivet】Paichongding,a neonicotinoid type of insecticide recently developed in China,is easily absorbed by plant and transferred inside the plant. Now it is used mainly for controlling insects of homoptera and expected to have a bright future as a promising new pesticide. Once pesticides enter into the soil,they readily get adsorbed,desorbed and leached in the soil. Their sorption and desorption are the main factors influencing fate of the pesticides in the soil,and seriously affecting their behaviors,like chemical and microbial degradation,volatilization and leaching,and moreover,it is an important index in pesticide environmental safety assessment. The study on its adsorption and leaching characteristics is of important significance to prediction of its environmental behavior and pollution in the soil. 【Method】In order to provide a scientific basis for the study of environmental behavior,migration and transformation,of paichongding in the soil,the batch oscillating equilibration method and column leaching method were adopted to explore adsorption and leaching characteristics of paichongding in three typical soils,that is brown soil from Tai’an,red soil from Fujian and black soil from Northeast China,and effects of three soil amendments on leaching of the substance in the soils. Residue of the pesticide in the soil was determined with SPE-HPLC. As in the leachate,the concentration of paichongding was low,the solution underwent concentration and purification with SPE before determination of residue of paichongding in the leachate with HPLC. 【Result】Results show that the adsorption equilibrium time of paichongding was 12 h,9 h and 12 h in the red soil,brown soil and black soil,respectively,by absorption dynamics. The Freundlich model and the Linear isothermal adsorption model can well be used to describe the adsorption processes of paichongding in soil. Of the pesticide,distribution coefficient,Kd,was 23.16,11.24 and 4.68,and adsorption constant was 22.03,11.69 and 5.05 in the black soil,red soil and brown soil,respectively. Among the three soils,black soil was the highest in paichongding adsorption capacity and brown soil was the lowest. The adsorption isotherms of paichongding in three different soils fitted fairly the Freundlich model and Linear model at 25℃,with Koc being 1 619,2 094 and 495,respectively,and the absolute values of free energy in all the three soils were less than 40 kJ mol-1,so the adsorption of paichongding in these soils belonged to physical adsorption. Leaching of paichongding varied in the three soils. In the brown soil,paichongding migration rate was the highest,and slightly increased with rising dosage of the pesticide,and the variation with dosage was not significant;In the red soil and black soil,dosage did not have much effect on leaching rate of the pesticide,either,and Only a slight difference in leaching rate was found in the red soil between treatments applied with 200 μg and 500 μg of paichongding. One-way ANOVA analysis of the black soil shows that the effect of dosage was not significant. In the leachate from the brown soil,red soil and black soil,paichongding residue accounted for 16.69%~16.86%,11.55%~13.52% and 8.98%~9.35% of the total applied,respectively. As the black soil was the highest in adsorption capacity,pesticide in the soil was the lowest in mobility. Residue of paichongding in the red soil and black soil decreased with soil depth,but by a little margin. Once activated carbon was added into the soils,it reduced not only migration and leaching rate of paichongding significantly,but also extractable residue by 34.8%,36.79% and 16.93%,respectively,in the brown soil,red soil and black soil;No residue was detected in the leachates from the red soil and black soil,while 76.4% less residue was found in the leachate from the brown soil in the treatments amended with activated carbon. The addition of 0.5% humic acid and peat,separately,reduced the leaching rate of the pesticide by 25.1% and 17.1%,respectively,in the brown soil,by 29.7%% and 23.3%,respectively,in the red soil,and by 42.1% and 27.6 %,respectively,in the black soil. 【Conclusion】 In brief,the amendment of 0.5% activated carbon,humic acid and peat into the paichongding-contaminated soils can significantly reduce leaching rate of the substance,and hence its risk of polluting the groundwater.

        Neonicotinoid insecticides;Paichongding;Adsorption;Leaching;Soil amendment

        X131.3

        A

        10.11766/trxb201604200104

        (責(zé)任編輯:盧 萍)

        * 國(guó)家自然科學(xué)基金項(xiàng)目(41671321)、國(guó)家重點(diǎn)研發(fā)計(jì)劃項(xiàng)目(2016YFD0800304)和山東農(nóng)業(yè)大學(xué)青年創(chuàng)新基金(23816)資助 Supported by the National Natural Science Foundation of China(No. 41671321),the National Key Research and Development Project of China(No. 2016YFD0800304),and the Science and Technology Innovation Foundation for Youth of Shandong Agricultural University(No. 23816)

        ? 通訊作者 Corresponding author,E-mail:jwang@sdau.edu.cn

        謝 慧(1973—),女,山東濟(jì)寧人,博士,講師,主要從事農(nóng)藥殘留與環(huán)境毒理方面的研究。E-mail:huixie@sdau.edu.cn

        2016-04-20;

        2016-10-08;優(yōu)先數(shù)字出版日期(www.cnki.net):2016-11-14

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