工程奈米顆粒一旦釋放到水生環境中，並不會以本來的形式存在，工程奈米顆粒顆粒受同質聚集、異質聚集（heteroaggregation）、溶解或表面改質等過程產生改變，這些改變會顯著影響其環境宿命和風險。然而，目前的分析技術無法在環境條件下同時解析顆粒尺寸、元素組成和聚集狀態。即使適用於環境基質的單顆粒感應耦合電漿質譜儀(spICP-MS)也無法識別環境中最常見的異質聚集顆粒，因為該方法測量的是元素質量而非物理尺寸。因此，在複雜基質中分析工程奈米顆粒的異質聚集仍然是一項重大挑戰。
本論文發展電移動度分析儀結合單顆粒感應耦合電漿質譜儀(ATM-DMA-spICP-MS)的策略，解決了現有技術的侷限性。該方法整合了電移動度分析儀的粒徑分離技術與spICP-MS的單顆粒元素檢測技術，實現了奈米顆粒的二維粒徑分析。本研究同時解決過去ATM-DMA-spICP-MS在定性粒徑上碰到的瓶頸，研究結果顯示，電移動度的粒徑分布相較於標準品在較大粒徑上會有明顯的拖尾現象，此拖尾現象可歸因於水層包裹的奈米顆粒，本研究透過加熱氣膠流使其乾燥，有效消除拖尾。實驗證明，本方法具備優異的粒徑定性能力，能有效區分30 nm和50 nm的金奈米顆粒混合樣本。此外該方法在水樣濃度為4.1 × 105至 107 #/mL (即0.6至14.3 ug Au/L)時展現出良好的線性關係，並能將多顆粒事件降至最低。其方法偵測極限4.1 × 10⁵ #/mL (即0.6 μg Au/L），涵蓋環境中的奈米顆粒的真實濃度。本研究亦首次利用ATM-DMA-spICP-MS 表徵廢水樣本中金、銀奈米顆粒（AuNPs與AgNPs）的異質凝聚現象，證實兩者均會與廢水中固有的膠體或大分子形成異質凝聚體。該方法甚至能在添加外部AgNPs之前，直接檢測出原廢水樣本中固有的銀顆粒，彰顯了其在分析複雜環境基質中異質凝聚奈米顆粒的潛力。
本論文亦深入探討工程奈米顆粒的環境宿命，環境宿命的調查對於預測工程奈米顆粒在水環境中的遷移與轉化（即環境暴露評估）至關重要。為此，環境宿命模型亟需具備環境真實意義的參數以提高預測準確性。本研究首次針對環境真實濃度下的工程奈米顆粒（即氧化鋅奈米顆粒（ZnONPs））溶解情形進行了系統性調查，揭示了其溶解行為與傳統高濃度研究的結果截然不同。因此，採用符合環境真實濃度的條件來評估溶解宿命並推導相關參數顯得尤為重要。本研究在50至200 μg/L的環境相關濃度下，探討了ZnONPs在受都市、農業或海水影響的河水樣本中的溶解狀況。據我們所知，這是目前溶解研究中所使用的最低ZnONP濃度。結果顯示，在50 μg/L的低濃度下，ZnONPs在各類水體中均會完全溶解；而在100 μg/L與200 μg/L的較高濃度下，溶解程度則取決於水化學性質。重要的是，根據本研究的測量數據以及對現有研究（涵蓋海水、高鹼度河水、合成緩衝溶液等）的分析，我們發現初始ZnONP濃度的降低會導致一階溶解速率（1st-order dissolution rate）的增加。因此，在建構高預測性的環境宿命模型時，必須採用或測量基於環境相關濃度下的溶解速率參數。
總體而言，本論文開發了一種能解析複雜基質中同質聚集或異質聚集現象的二維粒徑分析法，並對ZnONPs的溶解過程提供了首次具環境真實意義的評估，進而推動了對工程奈米顆粒的表徵方法研究與環境宿命的理解。溶解研究的結果釐清了濃度與水化學性質如何影響環境真實濃度下ZnONPs的溶解行為。這些貢獻強化了評估水環境中工程奈米顆粒的科學基礎，並為未來的環境宿命建模提供了更可靠的參數。

Engineered nanomaterials (ENMs) undergo aggregation, heteroaggregation, dissolution, and surface modification once released into aquatic environments, and these transformations strongly influence their fate and risks. However, current analytical techniques cannot simultaneously resolve particle size, elemental composition, and aggregation state at environmentally relevant concentrations. Particularly, single-particle ICP-MS lacks the ability to identify heteroaggregates because it measures elemental mass rather than physical size. As a result, transformation-resolved characterization of ENMs in complex matrices remains a major challenge.
This dissertation addresses these limitations by developing and validating an atomizer differential mobility analysis coupled with single-particle ICP-MS (ATM-DMA–spICP-MS) method. The method integrates mobility diameter separation with particle-specific elemental detection, enabling two-dimensional nanoparticle size analysis. With this method, the tailing of electrical mobility size distribution observed in earlier studies using ATM-DMA-ICP-MS was resolved. It is shown that the size distribution tailing can be attributed to the water-shelled NPs that could be dehydrated by heating the aerosol flow, effectively eliminating the tailing. Our method exhibited a good sizing performance and can resolve mixed bimodal 30 nm and 50 nm AuNPs. The nano DMA-spICP-MS method can reliably analyze 7.8 × 105 to 1.9 × 107 # of 50 nm AuNPs (or 4.1 × 105 to 107 # NPs/mL equivalent to 0.6 to 14.3 μg Au/L) introduced with a linear response and minimized multiple particle events. The LOD for counting was 7.8 × 105 # AuNPs introduced (equivalent to 4.1 × 105 #/mL and 0.6 μg Au/L) that is relevant to environmental NP concentrations. DMA-spICP-MS was used for the first time to characterize heteroaggregated AuNPs and AgNPs in a wastewater sample, in which both NPs were shown to form heteroaggregates with colloids and/or macromolecules inherent in wastewater. DMA-spICP-MS was able to directly detect Ag particles inherent in the original wastewater even before adding external AgNPs, manifesting its potential to characterize heteroaggregated NPs in complex environmental matrices.
In addition, understanding the environmental fate processes of ENMs is essential in the prediction of their environmental fate and transport in the aqueous environment (i.e., environmental exposure of ENMs). To this end, the availability of environmentally realistic fate parameters is warranted in the predictivity of the fate models. This work provides the first systematic investigation of ZnONP dissolution at environmentally realistic concentrations, revealing dissolution behaviors that contrast sharply with those reported in traditional high concentration studies. Using environmentally relevant conditions to evaluate the fate processes and derive related parameters is therefore important. In this study, we have investigated ZnONP dissolution in two freshwater samples (river and lake) and a seawater-influenced river sample using environmentally relevant ZnONP concentrations of 50-200 μg/L. To our knowledge, these are the lowest concentrations of ZnONPs used among existing dissolution studies. We demonstrate the complete dissolution of ZnONPs at a low concentration of 50 μg/L independent of the water matrices involved, while at higher concentrations of 100 μg/L and 200 μg/L, the dissolution levels were dependent on the water chemistry. Importantly, we found a correlation of decreased initial ZnONP concentrations with increased 1st-order dissolution rate coefficients based on our measurements and those from existing studies where a range of water chemistry (e.g., seawater, high alkalinity river water, synthetic buffer solutions) was used. It is essential to measure or adopt ZnONP dissolution rate coefficients from studies using relevant ZnONP concentrations for use in building highly predictive environmental fate models. While this work focuses on ZnONPs, it is also important for future work to examine the concentration-dependent dissolution behavior for other dissolvable ENMs such as silver and copper nanoparticles.
Overall, this dissertation advances the characterization and environmental understanding of ENMs by validating a two-dimensional nanoparticle size analysis method capable of resolving aggregation and heteroaggregation in complex matrices, and by providing the first environmentally realistic assessment of ZnONP dissolution. The dissolution results clarify how concentration and water chemistry affect dissolution behavior of ZnONPs under realistic exposure levels. These contributions strengthen the scientific basis for evaluating fate of ENMs in aqueous environment and provide more reliable parameters for future environmental fate modeling.

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