近期，国际环境科学与生态学领域top期刊Chemosphere报道了针对规模化种植的中药材的农药污染状况，该研究全面评估了中药农残的潜在风险及安全性，为建立更全面的风险评估体系和有效的中药质量控制提出了建议。
文章由中国中医科学院中药研究所陈士林团队完成，第一作者是骆璐和董林林副研究员，该团队从503个产区收集了共1771批次种植类中药材，采用液相色谱-串联质谱法(LC/MS-MS)及气相色谱-串联质谱法(GC/MS-MS)对136种农残进行分析。
在分析大样本量中药材有害物质残留量及风险的基础上，通过欧盟药典公式，计算出农药的最大残留限量，为中药材外源性有害物质残留量的标准制定提供依据。采用膳食风险评估(dietary exposureassessment)区分由于暴露量升高而对健康构成的可接受或不可接受风险。应用危害商(HQ)和危害指数(HI)来量化急性、慢性，以及中药农残的累积暴露风险；采用风险安全序数(riskranking score)，通过风险等级评分对农药和中药材的风险等级进行分类和排序。通过将农药毒性、农药摄入量和可检测残留水平的相应分值进行计算，得到农药的风险等级得分(S)和中药材的风险指数(RI)；此外，首次建立了针对中药农残的健康影响评估体系(patienthealth impact assessment)，分别计算致癌和非致癌风险，并最终将中药农残的这些风险与疾病发病概率联系起来。量化了中药材农药残留引起的患者摄入量以及相关癌症和非癌症聚集效应，并将两者合并成患者健康影响得分(IS)，用伤残调整生命年(DALY)表示。
本研究旨在建立中药材多残留物检测目标并确定大样本量的中药材农药残留状况，建立中药材农残系统的检测方法体系和风险评估体系；探讨中药材农残标准制定及控制方法，提出保障中药材质量及有效性的措施。
图1.中药材农残检测及风险评估流程图
结果显示，88.03%(n=1559)的样本中共检出136种农残，联苯菊酯(bifenthrin)检出率最高，为44.62%，其次为二苯胺(diphenylamine，42.41%)和异丙甲草胺(metolachlor，41.50%)。根茎中农残检测率最高(48.56%)，其次是果实和种子(29.83%)，叶和皮质(8.98%)。35种禁用的剧毒农药的检出率为42.97%。禁用农药速灭磷检出率最高(mevinphos，24.20%)，其次是涕灭威(aldicarb，15.00%)和总滴滴涕(total DDT，13.10%)。检出禁用农药的样品中，根茎类占47.44%，果实和种子类占30.62%，叶和皮质类占8.67%。59.01%样本农残超过欧盟标准，速灭磷(mevinphos)超标率最高，为24.20%，其次是异丙氧磷(propetamphos，19.33%)、多菌灵(carbendazim，16.20%)、涕灭威(aldicarb，15.00%)和总滴滴涕(total DDT，13.10%)。
图2. 1771个中药样本中136种农残检测情况及潜在风险最高的药材与农药
Figure 2. Detection of 136 pesticide residue contentsin 1771 HM samples and the top risk-inducing pesticides and HM by threeapproaches of risk assessments. (A) General detection rate,over-limit ratio and detection rate of banned pesticides of 1771samples intotal. (B) Over-limit ratio and banned pesticide detection rate of top 14pesticides (Top ten pesticides by over-limit ratio and top ten by bannedpesticide detection rate were collected together). (C) Times of the highestconcentrations of top ten pesticides detected over the EP limit. (D) Highestrisk assessment scores of top ten pesticides. (Collecting HQa>1and HQc>1 pesticides, and top ten pesticides with highestrisk-ranking score (S=140) and Impact Score (mean ISi,h), tenpesticides were obtained) (E) Number of detected, banned and over-limitpesticides in top 14 herbal medicines (Summarizing top ten HM detected withhighest number of total pesticides, over-limit pesticides and bannedpesticides, 14 HM were obtained. Acanthopanacis Senticosi Radix is short forAcanthopanacis Senticosi Radix et Rhizoma Seu Caulis). (F) Highest riskassessment scores of top 11 herbal medicines. (Collecting HQa>1,HQc>1 HM, and top ten HM with highest risk index (RI) and ImpactScore (mean ISh), 11 risk-inducing herbal medicines appeared overonce thus included here.)
根据膳食风险评估结果，10种中药材的急性风险为不可接受风险(HIa>1),包括山楂(HIa=12.09),花椒 (HIa=11.54), 枸杞子 (HIa=1.86), 和苦地丁 (HIa=1.48)等。23种中药材的慢性风险为不可接受风险(HIc>1)，包括山楂(HIc=6.62)，肉豆蔻(HIc=3.51)，和花椒(HIc=3.38)等。山楂和花椒的急慢性风险(HQa和HQc)及急慢性累积风险(HIa和HIc)最高，而禁用农药呋喃丹(carbofuran)和甲氧基硫磷(mevinphos)在膳食暴露风险评估中风险商最高。此外，果实和种子类药材显示出最高的膳食暴露风险。在风险安全序数评估中，山楂、枸杞子、金银花和蒲公英中检测到的3-羟基呋喃丹(Carbofuran-3-hydroxy)和对溴磷(letophos)的风险等级得分(S=140)最高。而中药材山楂的风险指数最高(RI=1925)，其次是石斛(RI=1315)和防风(RI=1144)。此外，根据Spearman相关系数(Spearmancorrelation coefficients),农药残留(p=0.783)对风险排序的贡献最大，其次是农药毒性(p=0.691),相关性最小的是中药材摄入量(p=0.370)。
根据健康影响评估结果，中药材薏苡仁(minISh=3945.40DALY·person-1, mean ISh=3972.07DALY·person-1)和川明参(ISh=4287.78DALY·person-1)调整伤残年数最高，而薏苡仁中o,p'-滴滴涕(o,p'-DDT)(Isi,h=2729.58DALY·person-1),及川明参中的o,p'-滴滴涕(o,p'-DDT)(meanIsi,h=2837.91DALY·person-1, max ISi,h=3682.78 DALY·person-1)风险最高。
综合三种风险评估方法，总滴滴涕(totalDDTs)、呋喃丹(carbofuran)，和速灭磷(mevinphos)被确认为中药材中是最具风险隐患的杀虫剂。其除具有肾毒性和肝毒性外，还具有致癌、遗传毒性、生殖和发育效应。而以山楂为代表的果实类中药材的农残问题需要特别关注。
图3 风险最高的11种药材中的7种农药的健康影响值及其可能造成的健康损害（ISi,h热图）
Figure 3. Heatmapof Impact Scores (mean ISi,h) of top seven risk-inducing (banned)pesticides in 11 HM and their possible connections with health impacts.Collecting HQa>1 and HQc>1 pesticides, and top tenpesticides with highest risk-ranking score (S=140) and Impact Score (mean ISi,h),ten pesticides were obtained. Since p,p'-DDT, leptophos, and methomyl were notdetected in the 11 HM included thus not shown here, totally seven bannedpesticides were summarized above. Collecting HQa>1and HQc>1HM, and top ten HM with highest risk index (RI) and Impact Score (mean ISh),11 risk-inducing herbal medicines appeared over once thus included here. Thepossible health impacts of seven pesticides were derived from PesticideProperties Data Base (PPDB)22, European Food Safety Authority(EFSA), United States Environmental Protection Agency (USEPA), Agency for ToxicSubstances and Disease Registry (ATSDR), Toxicology Data Network from U.S.National Library of Medicine (TOXNET), and Beyond Pesticides. Data showingpositive, possible, mixed and ambiguous results are considered a possibleconnection, while no data and negative results considered unrelated.
外源性有害残留物超标影响中药质量与信誉，阻碍中医药走向世界。然而农药残留可以通过科学、合理的途径及方法解决。通过对农药残留进行限量规定，保障药材的安全性及有效性，实现中药资源可持续发展，推进中药产业的现代化和国际化。时空尺度大规模中药材农残检测及风险评估，可为中药材外源性有害残留物标准制定提供数据支撑，为中药材规范化种植和质量监管提供依据。
文章发表于Chemosphere (Luo L, Dong L, Huang Q,et al. Detection and risk assessments of multi-pesticides in 1771 cultivatedherbal medicines by LC/MS-MS and GC/MS-MS.Chemosphere.2020,7,https://doi.org/10.1016/j.chemosphere.2020.127477)
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