Exposure assessment constitutes a fundamental component of the risk assessment of engineered nanomaterials (ENMs). Given the considerable challenges in performing direct and quantitative measurements of ENMs in complex environmental systems, environmental fate models (EFMs) have become essential tools for estimating their environmental distribution. This study reviews the development and application of EFMs in surface waters and categorizes existing models into three principal types: material flow analysis models (MFAMs), multimedia compartment models (MCMs), and spatial river/watershed models (SRWMs). MFAMs are employed to estimate ENM releases and provide input concentrations for EFMs, while MCMs represent intermedia transfer processes under spatially and temporally averaged conditions. In contrast, SRWMs resolve hydrological and morphological variability in rivers and watersheds with higher spatial and temporal detail. As the foundation of EFMs, we also review the existing and emerging ENM fate processes and their inclusion in recent EFMs. The review is concluded by identifying the opportunities and challenges in using EFMs for ENMs.
To enhance predictive capability of exposure modeling for ENMs, this research introduces an integrated modeling framework that links a form-specific probabilistic MFAMs (P-MFAMs) with a highly spatiotemporally resolved river model. The approach was applied to zinc oxide nanoparticles (ZnONP) in the Yanshuei River, southern Taiwan, incorporating local release characteristics, tidal influence, and experimentally derived dissolution rate coefficients. The form-specific P-MFAMs indicated that pristine ZnONP accounted for 89% of releases due to limited wastewater treatment coverage. Dissolution was identified as the dominant fate process of ZnONP, whereas heteroaggregation played a relatively minor role. The occurrence of free ZnONP was infrequent and mainly confined to discharge zones, with the maximum steady-state concentration reaching 0.9 μg/L. In contrast, dissolved Zn ions represented the primary transformation product, with concentrations accumulating downstream to approximately 7 μg/L. Sensitivity analysis revealed that dissolution strongly influenced outcomes at dissolution rates above 3 d⁻¹, while heteroaggregation became relevant only when the dissolution rate was extremely low (≤0.1 d⁻¹). Tidal influences also exerted a marked effect on Zn species distribution: over a two-month simulation period, high tides increased Zn species accumulation up to threefold in river sections receiving substantial inputs, whereas low tides facilitated the drain of Zn plumes.
These findings highlight the necessity of integrating the realistic local ENM release, including the ENM forms as the output of probabilistic MFAMs with spatiotemporal fate models to support higher-tier exposure assessments of ENMs.

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