红壤不同粒径团聚体对草甘膦农药降解动力学的影响

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辛龙川^1,,
吴文雪¹,
薛萐²,
付格娟³,
陈延华⁴,
王学霞⁴,
刘东生⁴,
杨晓梅^{1, 2,,}
1.西北农林科技大学资源环境学院杨凌 712100
2.西北农林科技大学水土保持研究所/黄土高原土壤侵蚀与旱地农业国家重点实验室杨凌 712100
3.西安市环境监测站西安 710100
4.北京市农林科学院植物营养与资源研究所北京 100097
基金项目: 国家自然科学基金项目41877072
陕西省自然科学基金项目2019JQ-639

详细信息

作者简介:辛龙川, 主要研究方向为土壤污染物与微生物互馈作用。E-mail: xinlongchuan@163.com

通讯作者:杨晓梅, 主要研究方向为农田污染物迁移机理与模型模拟、污染物环境风险评估、土壤侵蚀与污染、土壤质量评估与可持续发展。E-mail: xiaomei.yang@nwafu.edu.cn

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出版历程

收稿日期:2020-08-21
录用日期:2021-01-01
刊出日期:2021-05-01

Effects of aggregate size on kinetics of glyphosate degradation in red soil

XIN Longchuan^1,,
WU Wenxue¹,
XUE Sha²,
FU Gejuan³,
CHEN Yanhua⁴,
WANG Xuexia⁴,
LIU Dongsheng⁴,
YANG Xiaomei^{1, 2,,}
1. College of Natural Resources and Environment, Northwest A & F University, Yangling 712100, China
2. Institute of Soil and Water Conservation, Northwest A & F University/The State Key Laboratory of Soil Erosion and Dryland Farming on Loess Plateau, Yangling 712100, China
3. Xi'an Environmental Monitoring Station, Xi'an 710100, China
4. Institute of Plant Nutrition and Resources, Beijing Academy of Agricultural and Forestry Sciences, Beijing 100097, China
Funds: the National Natural Science Foundation of China41877072
the Natural Science Foundation of ShaanxiProvince2019JQ-639

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Corresponding author:YANG Xiaomei, E-mail: xiaomei.yang@nwafu.edu.cn

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摘要
摘要:草甘膦农药的大量喷施，使其在环境特别是土壤中的残留-累积风险日益突出，从团聚体粒径角度研究红壤不同粒径团聚体中草甘膦的降解动力学及其相互作用特征仍鲜有报道。基于此，本研究通过干筛筛分、室内控制培养、液质联用定量分析相结合等探究草甘膦降解残留，并进一步分析团聚体理化性质与草甘膦降解的关系。结果表明：1）不同粒径团聚体中，草甘膦残留量随降解时间不断减小，且粒径之间降解动力学差异不显著。降解半衰期为15.8~20.6 d，粒径最小的团聚体（< 0.25 mm）中草甘膦的降解半衰期最长，为20.6 d。草甘膦在土壤中的主要降解产物氨甲基磷酸（AMPA）的含量随着降解时间的增加而增加，且在第5 d达到峰值，而后不断减小；不同粒径团聚体间AMPA含量差异显著（P < 0.05）。2）相关分析及主成分分析发现，草甘膦残留量与红壤团聚体中速效磷含量呈显著正相关（P < 0.05），而其降解产物AMPA含量与团聚体中酸性磷酸酶活性及N-乙酰氨基-β-葡萄糖苷酶活性呈显著正相关（P < 0.05）。团聚体粒径与草甘膦残留量间没有显著相关性，但与AMPA含量显著正相关（P < 0.05）。此外，草甘膦降解过程中，团聚体中有机质含量及β-葡萄糖苷酶、N-乙酰氨基-β-葡萄糖苷酶、酸性磷酸酶活性与团聚体粒径为显著负相关关系（P < 0.05）。由此表明：红壤不同粒径团聚体影响草甘膦降解速率，粒径最小的团聚体（< 0.25 mm）中草甘膦农药的降解速率最慢，但试验结束时，各粒径红壤团聚体中的草甘膦和AMPA含量均较高，可能会影响土壤健康及生态环境安全；此外，草甘膦降解与土壤磷素密切相关，后续研究需探讨磷亏缺或丰盈条件下，草甘膦农药的土壤环境特征，为后续农田草甘膦环境风险评估提供依据。
关键词:土壤团聚体/
草甘膦/
降解动力学/
土壤磷/
红壤
Abstract:With intensive glyphosate application, its residues and consequent risks of soil health and ecological environment safety have received greater attention. The degradation kinetics of glyphosate in red soil aggregates with different sizes, as well as the interaction between physical and chemical properties of soil aggregates and the degradation of glyphosate, have rarely been studied. Thus, in this study, the degradation characteristics of glyphosate in red soil aggregates with different sizes were observed under laboratory conditions by particle pre-sieving, incubation in a controlled climatic chamber, and residue analysis via liquid chromatography-tandem mass spectrometry. The physical and chemical properties of the soil aggregates, such as contents of organic matter, total phosphorus, and available phosphorus, were tested according to the national approved methods and standards. The relationships between the physical and chemical properties of the aggregates and the degradation of glyphosate were further analyzed and compared in the same observation day. The results showed that 1) the glyphosate content decreased in the different aggregate particles during the observation period, following the single first-order kinetic degradation model. However, no significant differences were observed among different aggregate sizes. The half-life time of glyphosate in the different red soil aggregates ranged from 15.8 to 20.6 d, with a longer half-life time in the smallest aggregates (< 0.25 mm, 20.6 d). The aminomethylphosphonic acid (AMPA) content, the main metabolite of glyphosate, increased immediately and peaked on the 5^th day after glyphosate application, but no differences were found among different aggregates. However, the AMPA content changed and declined significantly in different aggregates after the 5^th observation day (P < 0.05). The contents of organic matter, total nitrogen, total phosphorus, and available phosphorus in different aggregates varied greatly, especially the available phosphorus content, which decreased with glyphosate degradation. 2) Correlation analysis and principal component analysis of glyphosate, aggregate size, and their properties showed that the residual glyphosate was significantly positively correlated with the content of available phosphorus (P < 0.05), and the AMPA content was significantly positively correlated with the activities of acid phosphatase and N-acetylamino-β-glucosidase (P < 0.05). There were no significant relationships between the aggregate size and the residuals of glyphosate, but a significant positive correlation was observed between the aggregate size and the AMPA content (P < 0.05). Furthermore, during the whole period of glyphosate degradation, the organic matter content, acid phosphatase, N-acetylamino-β-glucosidase, and β-glucosidase showed a significant negative relationship with the soil aggregate size (P < 0.05). In conclusion, the characteristics of the red soil aggregates affect the degradation kinetics of glyphosate, as well as the persistence of AMPA, especially the residuals in the smallest aggregates (< 0.25 mm). The contents of glyphosate and AMPA in the red soil aggregates were still high after 30 days, which may affect soil health. Glyphosate degradation was also closely related to phosphorus in the soil. Therefore, the fate of glyphosate under conditions of phosphorus deficiency or abundant soil should be explored to provide detailed information on glyphosate risk assessment in red soil.
Key words:Soil aggregates/
Glyphosate/
Degradation kinetics/
Soil phosphorus/
Red soil

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图1红壤不同粒径团聚体中草甘膦(A)和氨甲基磷酸(AMPA, B)的残留量变化
Figure1.Glyphosate (A) and aminomethylphosphonic acid (AMPA, B) residues in red soil aggregates with different sizes

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图2喷施草甘膦后不同时间红壤不同粒径团聚体中β-葡萄糖苷酶(BG)、N-乙酰氨基-β-葡萄糖苷酶(NAG)、酸性磷酸酶(ACP)活性变化及其变化率
Figure2.β-glucosidase (BG), N-acetylamino-β-glucosidase (NAG), acid phosphatase (ACP) activities and their change rates in red soil aggregates with different sizes at different days after application of glyphosat

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图3各粒径团聚体主成分得分(a)以及草甘膦残留量与团聚体性质的主成分分析(b)
Gly: 草甘膦残留量; OM: 有机质含量; AP: 速效磷含量; BG: β-葡萄糖苷酶活性; NAG: N-乙酰氨基-β-葡萄糖苷酶活性; ACP: 酸性磷酸酶活性。
Figure3.Principal component scores of aggregate sizes (a) and principal component analysis of glyphosate residue and aggregate properties (b)
Gly: glyphosate residue; OM: organic matter content; AP: available phosphorus content; BG: β-glucosidase activity; NAG: N-acetylamino-β-glucosidase activity; ACP: acid phosphatase activity.

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表1试验用红壤不同粒径团聚体的基本性质
Table1.Properties of aggregates with different sizes of the tested red soil

土壤性质Soil property	粒径Size (mm)
土壤性质Soil property	< 2 (X)	1~2 (Ⅱ)	0.25~1 (Ⅲ)	< 0.25 (Ⅳ)
pH	5.29±0.02	5.03±0.01	4.91±0.00	4.89±0.00
有机质Organic matter (g?kg^?1)	16.56±0.48	15.43±0.08	16.97±0.14	16.60±0.42
全氮Total nitrogen (g?kg^?1)	0.99±0.01	1.02±0.01	1.21±0.01	1.20±0.03
全磷Total phosphorus (g?kg^?1)	0.70±0.00	0.76±0.03	0.76±0.01	0.76±0.00
速效磷Available phosphorus (g?kg^?1)	0.14±0.00	0.14±0.00	0.14±0.00	0.14±0.00

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表2红壤不同粒径团聚体中草甘膦降解动力学方程
Table2.Glyphosate degradation kinetic equations in red soil aggregates with different sizes

团聚体粒径Aggregate size (mm)	动力学方程Kinetics equation	半衰期Half-life (d)	R²
< 2	C_t=13.56e^?0.037^t	18.5±3.5	0.73
1~2	C_t=14.41e^?0.044^t	15.8±2.8	0.73
0.25~1	C_t=14.14e^?0.039^t	17.7±3.6	0.62
< 0.25	C_t=13.50e^?0.034^t	20.6±4.0	0.65

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表3喷施草甘膦后不同时间红壤不同粒径团聚体的性质
Table3.Soil properties of red soil aggregates with different sizes at different days after application of glyphosat?g?kg^?1

土壤性质Soil property	团聚体粒径Aggregate size (mm)	喷施后天数Days after application (d)
土壤性质Soil property	团聚体粒径Aggregate size (mm)	0	1	3	5	7	14	30
有机质Organic matter	< 2	16.73±0.52b	17.05±0.56b	16.92±0.28b	16.89±0.24b	17.30±0.59b	17.27±0.45b	16.88±0.94ab
	1~2	16.30±0.16b	15.84±0.43b	16.27±0.38b	16.33±0.21b	16.31±0.37b	16.28±0.36b	15.20±0.57c
	0.25~1	17.56±0.40ab	16.62±0.16ab	16.37±0.80b	17.34±0.18b	16.31±0.81b	17.16±0.59b	16.38±0.40b
	< 0.25	18.55±0.17a	18.25±0.59a	18.04±0.76a	19.41±0.50a	18.62±0.66a	18.09±0.62a	17.58±0.69ac
全氮Totalnitrogen	< 2	1.05±0.13b	1.00±0.09b	1.00±0.08b	1.06±0.05b	1.15±0.04ab	0.97±0.05b	1.08±0.03b
	1~2	0.92±0.02b	0.93±0.05b	1.14±0.05a	1.11±0.03ab	1.20±0.06b	1.01±0.05b	1.04±0.07b
	0.25~1	0.95±0.02b	0.93±0.08b	1.09±0.03ab	1.10±0.05ab	1.06±0.10b	1.08±0.04ab	1.10±0.04b
	< 0.25	1.01±0.05a	1.21±0.08a	1.18±0.05a	1.19±0.10a	1.13±0.02ab	1.12±0.02a	1.11±0.03a
全磷Total phosphorus	< 2	0.77±0.02a	0.78±0.01a	0.76±0.01a	0.73±0.01a	0.78±0.02a	0.74±0.02a	0.75±0.03a
	1~2	0.77±0.03a	0.77±0.03a	0.75±0.02a	0.76±0.01a	0.77±0.02a	0.78±0.02a	0.74±0.02a
	0.25~1	0.75±0.01a	0.78±0.01a	0.78±0.02a	0.76±0.01a	0.76±0.01a	0.79±0.01a	0.74±0.02a
	< 0.25	0.76±0.02a	0.76±0.02a	0.74±0.02a	0.77±0.00a	0.75±0.02a	0.76±0.02a	0.70±0.00a
速效磷Availablephosphorus	< 2	0.14±0.01a	0.15±0.00a	0.13±0.00a	0.12±0.00a	0.14±0.01a	0.13±0.01a	0.13±0.01a
	1~2	0.14±0.00a	0.15±0.00a	0.13±0.01a	0.12±0.00a	0.14±0.00a	0.13±0.01a	0.13±0.01a
	0.25~1	0.14±0.01a	0.14±0.00a	0.13±0.00a	0.13±0.00a	0.13±0.01a	0.14±0.00a	0.13±0.00a
	< 0.25	0.15±0.00a	0.13±0.00a	0.13±0.00a	0.12±0.00a	0.14±0.01a	0.14±0.01a	0.13±0.01a
不同小写字母表示同一指标同一时间不同粒径间差异在P < 0.05水平显著。Different lowercase letters indicate significant differences among different aggregate sizes for the same index at the same time at P < 0.05 level.

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表4团聚体粒径与草甘膦及氨甲基磷酸(AMPA)含量的相关性分析
Table4.Correlation analysis among aggregate properties with glyphosate and aminomethylphosphonic acid (AMPA) contents

相关性Correlation	团聚体粒径Aggregate size	草甘膦Glyphosate	氨甲基磷酸AMPA	有机质Organic matter	速效磷Available phosphorus	BG活性BG activity	NAG活性NAG activity
草甘膦Glyphosate	0.020
氨甲基磷酸AMPA	0.131^*	?0.443^**
有机质Organic matter	?0.268^*	?0.140	?0.028
速效磷Available phosphorus	?0.018	0.412^**	?0.523^**	?0.068
BG活性BG activity	?0.357^**	0.009	0.173	0.366^**	?0.369^**
NAG活性NAG activity	?0.231^*	?0.205	0.335^**	0.281^*	?0.463^**	0.695^**
BG: β-葡萄糖苷酶; NAG: N-乙酰氨基-β-葡萄糖苷酶; ACP: 酸性磷酸酶。和分别表示显著性水平为P < 0.05和P < 0.01。BG: β-glucosidase; NAG: N-acetylamino-β-glucosidase; ACP: acid phosphatase. and ** indicate significant correlation at P < 0.05 and P < 0.01 levels, respectively.

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