深圳沿海微塑料污染及纤维老化机制微纳尺度探究

微塑料是一种新兴污染物，在环境中广泛存在，并遭受着各种环境老化作用。近年来，了解微塑料的分布特征和环境效应在全球范围内备受关注。据报道，我国沿海地区普遍存在微塑料污染，在深圳市一些红树林和河口也发现了高浓度的微塑料，然而关于深圳市整个海岸线的微塑料污染特征尚未揭示。微纤维是微塑料最主要且重要的子类别，在海洋、沉积物、污泥、红树林和河流等系统中无处不在。其来源很多，但在新冠疫情影响下口罩成了又一备受关注的潜在微纤维污染源，遗憾的是目前仍缺乏确切证据。一项报告评估了美国人日常食物中的微塑料，发现人体不知不觉从食物中摄入的微塑料绝大多数都是微纤维。然而与已报道的颗粒或片状微塑料相关研究相比，目前关于微纤维的数据严重不足，缺乏对微纤维老化过程和环境效应的关注。因此，本论文从宏观上系统调研了深圳沿海区域的微塑料污染特征和微纤维污染现状，从微观上探究了潜在微纤维污染源口罩在模拟的近岸环境下的物理老化过程，并利用多种微纳尺度技术从多个维度解析了聚丙烯（PP）微纤维在化学老化过程中的演变机制和吸附行为，最后进一步对比剖析了两类最具代表性微纤维聚酰胺（PA）和聚对苯二甲酸乙二醇酯（PET）的老化过程差异。

通过野外调查实验探究了深圳市沿海区域的微塑料污染特征，进行了两次系统性的采样分别收集表层水和沉积物样品。结果表明，深圳沿海区域表层水和沉积物中微塑料平均丰度分别为35.6±22.1 n/L和4955.8±2325.0 n/kg（±SE），透明微塑料是表层水和沉积物的主要成分，分别占59.6%和60.2%。第二次采集的样品受到了台风的干扰，导致表层水中微塑料平均丰度增加了约18%，沉积物中微塑料平均丰度下降了约35%。并且，台风干扰后微纤维在表层水和沉积物中的占比分别达到65.8%和51.9%，占据主导地位。通过溯源分析，以及第二次采集的表层水样中微纤维和紫色微塑料的不均衡增加，可以推断台风的干扰导致了外源微塑料的涌入，这项研究为更全面和动态地了解深圳沿海区域微塑料的污染特征提供了有价值的信息，也证实了微纤维污染严峻。

随后探究了潜在微纤维污染源口罩在模拟的近岸环境下的物理老化变化，定量评估了口罩中微纤维的排放量，发现外科口罩在模拟的水环境中释放出的微纤维数量要高于普通口罩和N95口罩，且口罩中间层最容易产生微纤维。以外科口罩为例，当在模拟条件下物理老化240小时后，推测其微纤维排放量约为10⁴根。并且，在水环境中0.1~1 mm的微纤维占比为74.62~89.58%，在沉积物磨损下其占比为72.41~86.74%。此外，沉积物磨损后口罩纤维表面粗糙度增大，出现明显裂纹和突起，这一现象可能会加速口罩纤维的分解，促进其他污染物的吸附或自身化学物质的释放。

进一步从多个维度探究了PP微纤维在不同方式下的化学老化过程和环境行为，发现氙灯老化和化学氧化过程均改变了PP微纤维的表面形貌、理化性质和聚丙烯链构象，增强了微纤维对Pb²⁺的亲和力，且化学氧化的影响更强，PCA结果也指出PP微纤维在化学氧化和氙灯老化下的老化行为有显著差异。分析PP微纤维老化指标的变化和相关性时还发现，最大吸附量（Q_max）与羰基指数（CI）、氧碳原子比（O/C）和拉曼峰强度比（I_841/808）呈正相关，而与最大质量损失率温度（T_m）和接触角呈负相关。O/C比能精确量化老化程度较低的表面变化，而CI值更适合解释老化程度较高的化学氧化过程。本研究从多个维度解析了微纤维的化学老化过程，并试图将微纤维的老化特征变化与吸附行为关联起来。

最后从微纳米尺度全面解析了两类最具代表性微纤维PA和PET的化学老化过程，结果表明化学老化下PA和PET微纤维表现出显著差异，化学老化过程中PA微纤维表面出现大量裂纹并逐渐恶化为裂缝，而PET微纤维表面没有明显变化。化学老化导致PA微纤维最大失重速率温度（T_m）降低，结晶度增加。同时，α晶型增加，出现Βrill转变致使γ晶型也增加。PA非酰胺部分碳链出现断裂，羰基含量逐渐增加。相反，PET微纤维在化学老化过程中T_m几乎不变，反式构象-CH₂减少，结晶度和羰基含量逐渐降低。此外，还发现羰基指数在评估自身结构含有羰基的这类微塑料的老化程度时有明显的弊端和局限性。本研究为进一步全面评估微纤维的环境行为提供理论支撑。

综上，这些研究的开展对详细了解深圳沿海区域微塑料污染特征，明确近岸环境物理老化在纤维早期老化阶段造成的破坏性影响具有重要意义，同时首次从多个维度关联评估了微纤维的老化过程演变机制和环境影响，为全面评估微纤维的环境效应提供了有效信息和新的视角。

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