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扑草净(4,6-双异丙胺基-2-甲硫基-1,3,5-三嗪)是一种低毒、高选择的内吸性除草剂,因杀草谱广、药效长、除藻效果明显等优点被广泛应用于农业生产和水产养殖中[1],在水中溶解度低(25 ℃,48 mg·L−1),半衰期为1~3月,化学性质稳定,难降解,对生态环境的影响已经引起世界各国的关注[2]。2010年扑草净被农业部第1435号公告列入《兽药试行标准废止标准目录》[3],但许多地区仍将其作为水质改良剂大量用于水产养殖中,造成水环境污染,水产品扑草净残留检出甚至超标[4-5]。此外,扑草净是一种环境内分泌干扰物质,经食物链传递进入体内,可导致生物体内分泌系统、生殖器官、神经系统和免疫系统异常等,威胁生物体健康[6-8]。因此,解决扑草净对水环境的污染问题刻不容缓。植物修复是运用植物遏制、降解或提取环境中外源性污染物的技术,具有高效、环保、无公害、成本低的优点[9]。香根草Vetiveria zizanioides又名岩兰草,为禾本科Gramineae香根草属Vetiveria多年生C4草本植物,根系发达,生物量大,适应性广,是较理想的水土保持植物[10]。近年来,香根草在环境修复领域应用广泛,对重金属铁、镍、铬、锰等有较强的富集能力,可有效净化富营养化水体并吸收降解环境中的阿特拉津[11-13]。扑草净是一种三氮苯类除草剂,化学结构与阿特拉津相似。目前,尚未有香根草修复不同质量浓度扑草净污染水体的相关报道。因此,本研究利用温室水培试验,分析不同初始质量浓度扑草净污染下,水体扑草净质量浓度和香根草体内扑草净质量分数的动态变化,为应用香根草修复农药污染水体提供理论基础。
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准确称取103 mg扑草净标准品,溶于100 mL乙腈中,得到1 000.0 mg·L−1扑草净标准储备液;然后用正己烷逐级稀释为标准溶液,测定色谱峰面积。结果表明:扑草净在0~20.0 mg·L−1范围内线性良好,线性回归方程为y=2.303x+1.727,相关系数为0.999。方法的检出限为0.001 mg·L−1。
取空白水样30 mL,植物样品各2.00 g,分别添加 0.5、1.0、1.5 mg·L−1标准溶液,每个加标水平3个重复。测定不同类型样品加标回收率。其中水样加标回收率为(88.76±4.62)%,根系为(98.23±4.04)%,茎叶为(94.38±4.03)%,相对标准偏差为(4.03~4.62)%,表明该方法符合实验要求。
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由图1A可以看出:随培养时间延长,T组水体扑草净质量浓度呈下降趋势。T1、T5处理,培养15 d水体扑草净较5 d分别降低了81.08%、44.39%,T10、T15处理分别降低了48.99%、47.77%。T1处理,培养15 d后水体扑草净质量浓度为0.14 mg·L−1,为培养10和5 d的33.33%和19.92%;T15处理,培养15 d后水体扑草净质量浓度为4.56 mg·L−1,为培养10和5 d的73.43%和52.23%。表明香根草对不同初始质量浓度扑草净污染水体具有一定修复效果。对不同培养时间下的水体扑草净质量浓度与初始质量浓度进行拟合,发现水体扑草净质量浓度与扑草净初始质量浓度呈线性关系,5、10、15 d拟合方程分别为:y5=0.50+0.60x、y10=0.31+0.43x、y15=0.21+0.32x,决定系数分别为0.961、0.965、0.950;培养时间越长,拟合方程斜率越小,说明扑草净初始质量浓度对水体扑草净质量浓度影响较大。
图 1 不同处理下水体扑草净质量浓度(A)、香根草根系(B)、茎叶(C)扑草净质量分数
Figure 1. Prometryn concentration of water (A), roots (B), shoots (C) of V. zizanioides under different treatments
由图1B可知:T组不同处理根系扑草净质量分数均为第5天最大,随培养时间延长,T1、T5处理下香根草根系扑草净质量分数下降,T10、T15处理下先下降后上升。不同处理根系扑草净质量分数培养10 d较5 d分别减少了52.37%、47.87%、59.30%、47.45%,15 d较5 d分别减少了71.29%、79.23%、39.14%、31.17%。推测5 d时其根部吸收扑草净达到最大值,随后向茎叶发生转移,根系继续吸收水培溶液中的扑草净,使得根系扑草净质量分数再次上升。对不同培养时间下的扑草净初始质量浓度与根系扑草净质量分数进行拟合,发现两者呈线性关系,5、10、15 d的拟合方程分别为:y5=0.52+3.84x 、 y10=−0.10+1.86x 、 y15=−2.41+2.65x,决定系数分别为0.952、0.988和0.929,说明不同培养时间下,扑草净初始质量浓度对香根草根系扑草净质量分数影响密切。
由图1C可知:T组不同处理下香根草茎叶中扑草净质量分数在培养5 d时达到峰值,随培养时间延长持续降低;不同处理茎叶中扑草净质量分数培养10 d较5 d分别降低了35.85%、51.80%、39.77%、29.43%,培养15 d时较5 d分别降低了55.09%、70.00%、58.07%、54.30%。对不同培养时间下的扑草净初始质量浓度与茎叶扑草净质量分数进行拟合,发现茎叶扑草净质量分数与扑草净初始质量浓度正相关,斜率随培养时间延长而减小。5、10、15 d的拟合方程分别为:y5=2.37+0.84 x 、y10=0.97+0.59x 、y15=0.70+0.38x ,决定系数分别为0.816、0.954和0.941,说明随着培养时间增加,香根草茎叶扑草净质量分数降低。
由表1可知:相同培养时间下,香根草转移系数均随扑草净初始质量浓度增加而降低。相比T1,培养5 d时T5、T10、T15香根草转移系数分别降低了30.95%、70.24%、71.43%,培养10 d时分别降低了54.46%、66.96%、70.54%,培养15 d时分别降低了32.06%、87.02%、87.79%。相同初始质量浓度处理下,香根草转移系数随培养时间延长呈波动趋势。T1、T5处理,香根草转移系数培养15 d较5 d分别增加55.95%、53.45%,T10、T15处理,香根草转移系数培养15 d较5 d分别降低32.00%、33.33%。表明香根草对水体扑草净的吸收、转移受初始质量浓度、培养时间影响。
表 1 不同处理下香根草转移系数
Table 1. Transfer coefficient of V. zizanioides under different treatments
t/d T1 T5 T10 T15 5 0.84±0.02 Ab 0.58±0.08 Bb 0.25±0.04 Cab 0.24±0.02 Cab 10 1.12±0.14 Aab 0.54±0.04 Bb 0.37±0.06 Ba 0.33±0.06 Ba 15 1.31±0.14 Aa 0.89±0.06 Ba 0.17±0.01 Cb 0.16±0.01 Cb 说明:大写字母表示不同处理间差异显著(P<0.05);小写字母表示不同培养时间下差异显著(P<0.05) -
采用一级反应动力学方程拟合不同培养时间下水体扑草净质量浓度的动态分布规律。水体添加不同质量浓度扑草净后,T组(图2A)和N组(图2B)水体扑草净的降解趋势均符合一级反应动力学方程,拟合度较高,培养时间与水体扑草净质量浓度均呈指数衰减趋势,最后逐渐趋于稳定。结合表2可知:不同初始质量浓度扑草净污染水体中,T组扑草净半衰期为7.42~13.82 d,N组为22.23~33.34 d,种植组较未种植组缩短了14.80~19.78 d;T组降解速率高于N组(P<0.05),表明种植香根草可加速水体中扑草净的降解,使降解半衰期提前。由表3可知:不同初始质量浓度扑草净污染的水体中,水体扑草净去除率T组高于N组(P<0.05);培养15 d,T组水体扑草净去除率为52.27%~85.88%,N组为29.16%~39.55%,去除率提高了22.52%~55.57%(P<0.05),表明香根草对不同初始质量浓度扑草净污染水体均有修复效果,1.0 mg·L−1初始质量浓度处理下,香根草对水体扑草净去除率最高。
图 2 不同处理下水体扑草净质量浓度与培养时间的关系
Figure 2. Relationship between prometryn concentration and cultivation time under different treatments
表 2 不同处理下水体扑草净降解速率和半衰期
Table 2. Degradation rate and half-life of prometryn in water under different treatments
初始质量浓度/
(mg·L−1)T组 N组 降解速率/
d−1半衰期/
d降解速率/
d−1半衰期/
d1.0 0.07 b 9.61 c 0.02 a 29.39 b 5.0 0.05 c 13.82 a 0.02 a 33.34 a 10.0 0.06 bc 10.88 b 0.02 a 29.89 b 15.0 0.09 a 7.42 d 0.03 a 22.23 c 说明:不同小写字母表示差异显著(P<0.05) 表 3 不同处理下水体扑草净去除率
Table 3. Prometryn removal rate in water under different treatments
t/d 初始质量浓度/
(mg·L−1)去除率/% T组 N组 相对去除率 5 1.0 23.28±2.26 g 15.72±4.63 c 3.90±1.41 d 5.0 19.93±0.36 g 16.88±0.62 c 3.05±0.08 d 10.0 22.05±1.63 g 17.11±3.10 c 4.94±1.58 d 15.0 40.38±2.95 e 19.57±1.64 c 20.82±4.59 c 10 1.0 56.44±4.68 c 21.68±4.10 c 40.72±8.53 b 5.0 39.64±0.23 e 21.11±3.12 c 22.76±0.38 c 10.0 45.90±1.37 de 21.77±1.46 c 28.80±1.98 bc 15.0 57.56±1.14 c 29.80±3.22 b 37.99±2.31 b 15 1.0 85.88±6.58 a 30.30±1.03 b 55.57±5.66 a 5.0 52.27±4.06 cd 29.75±2.87 b 22.52±4.48 c 10.0 60.25±1.34 bc 29.16±0.15 b 31.09±1.20 bc 15.0 68.82±5.27 b 39.55±0.99 a 29.27±5.65 bc 说明:不同小写字母表示差异显著(P<0.05) -
对扑草净初始质量浓度与香根草不同部位扑草净质量分数及水体扑草净质量浓度、转移系数、去除率作相关性分析。由表4可知:扑草净初始质量浓度与香根草转移系数呈极显著负相关(P<0.01),与香根草茎叶、根系扑草净质量分数呈极显著正相关(P<0.01),与相对去除率相关性不显著(P>0.05),相对去除率与培养时间呈极显著正相关(P<0.01),与转移系数相关性不显著(P>0.05);转移系数与水体扑草净质量浓度、香根草茎叶、根系扑草净质量分数均呈极显著负相关(P<0.01)。
表 4 扑草净初始质量浓度与香根草不同部位扑草净质量分数、相对去除率的相关性
Table 4. Correlation between initial concentration and the concentration of prometryn in V. zizanioides and relative removal rate
项目 初始质量浓度 培养时间 相对去除率 转移系数 水体质量浓度 茎叶质量分数 根系质量分数 初始质量浓度 1 培养时间 0.000 1 相对去除率 −0.033 0.662** 1 转移系数 −0.844** 0.163 0.328 1 水体质量浓度 0.852** −0.396* −0.349* −0.798** 1 茎叶质量分数 0.659** −0.564** −0.441** −0.610** 0.875** 1 根系质量分数 0.850** −0.298 −0.286 −0.803** 0.916** 0.793** 1 说明:*表示显著相关(P<0.05),**表示极显著相关(P<0.01)
Remediation potential of Vetiveria zizanioides on the water polluted with prometryn
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摘要:
目的 探究香根草Vetiveria zizanioides对扑草净污染水体的修复潜力。 方法 采用温室水培模拟实验的方法,研究香根草对水体不同初始质量浓度(1.0、5.0、10.0、15.0 mg·L−1)扑草净的吸收和去除特征。 结果 相同培养时间下,随水体扑草净初始质量浓度增加,香根草茎叶和根系扑草净质量分数显著增加(P<0.05),在第5天达到最大值,之后呈波动下降趋势;随培养时间延长,水体扑草净质量浓度显著降低(P<0.05)。与未种植香根草相比,香根草种植组水体扑草净降解半衰期缩短了14.80~19.78 d,去除率提高了22.52%~55.57%。相关性分析表明:水体扑草净质量浓度与香根草转移系数呈极显著负相关(P<0.01),与相对去除率相关性不显著(P>0.05),与培养时间呈极显著正相关(P<0.01)。 结论 种植香根草可提高水体扑草净降解速率和去除率,香根草可作为扑草净污染水体修复的先锋植物。图2表4参31 Abstract:Objective This study is aimed to explore the remediation potential of Vetiveria zizanioides on prometryn polluted water. Method The characteristics of absorption and removal of prometryn by V. zizanioides with different initial concentrations (1.0, 5.0, 10.0, 15.0 mg·L−1)were studied by hydroponic simulation experiment in greenhouse. Result With the same cultivation time, the increase of initial prometryn concentration brought about a significant increase of prometryn concentration (P<0.05) in the shoots and roots of V. zizanioides, which reached the maximum on the 5th day, and then demonstrated a fluctuating decline. The extension of cultivation time led to a significant decrease in prometryn concentration in water (P< 0.05). Compared with the control without V. zizanioides, the degradation half-life of prometryn in the treatment group with V. zizanioides was shortened by 14.80−19.78 days, and the removal rate was increased by 22.52%−55.57%. The concentration of prometryn in water had a significant negative correlation with the transfer coefficient of V. zizanioides (P<0.01), no significant correlation with relative removal rate (P>0.05), but a significant positive correlation with the cultivation time (P<0.01). Conclusion The planting of V. zizanioides can promote the degradation rate and removal rate of prometryn, therefore, V. zizanioides can be used as a pioneer plant in the remediation of prometryn polluted water. [Ch, 2 fig. 4 tab. 31 ref.] -
Key words:
- Vetiveria zizanioides /
- prometryn /
- absorption and removal /
- rhizosphere effect /
- phytoremediation
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表 1 不同处理下香根草转移系数
Table 1. Transfer coefficient of V. zizanioides under different treatments
t/d T1 T5 T10 T15 5 0.84±0.02 Ab 0.58±0.08 Bb 0.25±0.04 Cab 0.24±0.02 Cab 10 1.12±0.14 Aab 0.54±0.04 Bb 0.37±0.06 Ba 0.33±0.06 Ba 15 1.31±0.14 Aa 0.89±0.06 Ba 0.17±0.01 Cb 0.16±0.01 Cb 说明:大写字母表示不同处理间差异显著(P<0.05);小写字母表示不同培养时间下差异显著(P<0.05) 表 2 不同处理下水体扑草净降解速率和半衰期
Table 2. Degradation rate and half-life of prometryn in water under different treatments
初始质量浓度/
(mg·L−1)T组 N组 降解速率/
d−1半衰期/
d降解速率/
d−1半衰期/
d1.0 0.07 b 9.61 c 0.02 a 29.39 b 5.0 0.05 c 13.82 a 0.02 a 33.34 a 10.0 0.06 bc 10.88 b 0.02 a 29.89 b 15.0 0.09 a 7.42 d 0.03 a 22.23 c 说明:不同小写字母表示差异显著(P<0.05) 表 3 不同处理下水体扑草净去除率
Table 3. Prometryn removal rate in water under different treatments
t/d 初始质量浓度/
(mg·L−1)去除率/% T组 N组 相对去除率 5 1.0 23.28±2.26 g 15.72±4.63 c 3.90±1.41 d 5.0 19.93±0.36 g 16.88±0.62 c 3.05±0.08 d 10.0 22.05±1.63 g 17.11±3.10 c 4.94±1.58 d 15.0 40.38±2.95 e 19.57±1.64 c 20.82±4.59 c 10 1.0 56.44±4.68 c 21.68±4.10 c 40.72±8.53 b 5.0 39.64±0.23 e 21.11±3.12 c 22.76±0.38 c 10.0 45.90±1.37 de 21.77±1.46 c 28.80±1.98 bc 15.0 57.56±1.14 c 29.80±3.22 b 37.99±2.31 b 15 1.0 85.88±6.58 a 30.30±1.03 b 55.57±5.66 a 5.0 52.27±4.06 cd 29.75±2.87 b 22.52±4.48 c 10.0 60.25±1.34 bc 29.16±0.15 b 31.09±1.20 bc 15.0 68.82±5.27 b 39.55±0.99 a 29.27±5.65 bc 说明:不同小写字母表示差异显著(P<0.05) 表 4 扑草净初始质量浓度与香根草不同部位扑草净质量分数、相对去除率的相关性
Table 4. Correlation between initial concentration and the concentration of prometryn in V. zizanioides and relative removal rate
项目 初始质量浓度 培养时间 相对去除率 转移系数 水体质量浓度 茎叶质量分数 根系质量分数 初始质量浓度 1 培养时间 0.000 1 相对去除率 −0.033 0.662** 1 转移系数 −0.844** 0.163 0.328 1 水体质量浓度 0.852** −0.396* −0.349* −0.798** 1 茎叶质量分数 0.659** −0.564** −0.441** −0.610** 0.875** 1 根系质量分数 0.850** −0.298 −0.286 −0.803** 0.916** 0.793** 1 说明:*表示显著相关(P<0.05),**表示极显著相关(P<0.01) -
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