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The presence of poly‐ and perfluoroalkyl substances (PFAS) in the environment is associated with adverse health effects but measuring PFAS is challenging due to the associated high cost and technical complexities of the analysis. Here, the reactivity of atomically precise metal‐oxo clusters is reported and the foundation for their use is provided as fluorescent nanosensors for PFAS detection. The material comprises crystalline, water soluble, hexanuclear cerium‐oxo clusters [Ce6(µ3‐O)4(µ3‐OH)4]12+decorated with glycine molecules (Ce‐Gly) characterized by fluorescence emission at 353 nm. The Ce‐Gly fluorescence is found sensitive to long chain carboxylated PFAS of CF3–(CF2)more » « less
n –, where n ≥ 6, such as perfluorooctanoic, perfluorononanoic and perfluorodecanoic acids. This unique reactivity leads to a change in the emission spectra in a concentration dependent manner, enabling PFAS detection through ligand exchange and aggregation‐induced emission (AIE) enhancement. No significant cross‐reactivity from potentially co‐existing species, including sulfonated PFAS, octanoic and dodecanoic acids, humic acid, and inorganic ions is observed. With an optimal concentration of 3.3 µg mL−1Ce‐Gly, the method demonstrated detection limits of 0.24 ppb for PFOA and 0.4 ppb for PFNA. These findings highlight the potential of fluorescence‐based detection strategies utilizing nanoscale probes such as Ce‐Gly as fluorescent probes and nanosensors for PFAS.Free, publicly-accessible full text available September 1, 2025 -
Free, publicly-accessible full text available June 1, 2025
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Cerium oxide nanoparticles (CeNPs) are versatile materials with unique and unusual properties that vary depending on their surface chemistry, size, shape, coating, oxidation states, crystallinity, dopant, structural and surface defects. This review details advances made over the past twenty years in the development of CeNPs and ceria-based nanostructures, the structural determinants affecting their activity, and translation of these distinct features into applications. The two-oxidation states of nanosized CeNPs (Ce3+/Ce4+) coexisting at the nanoscale level, facilitate formation of oxygen vacancies and defect states which confer extremely high reactivity and oxygen buffering capacity, and the ability to act as catalysts for oxidation and reduction reactions. However, the method of synthesis, surface functionalization, surface coating and defects are important factors in determining their properties. This review highlights the key properties of CeNPs, their synthesis, interactions and reaction pathways, and provides examples of emerging applications. Due to their unique properties, CeNPs have become quintessential candidates for catalysis, chemical mechanical planarization (CMP), sensing, biomedical applications and environmental remediation, with tremendous potential to create novel products and translational innovations in a wide range of industries. This review highlights the timely relevance and the transformative potential of these materials in addressing societal challenges and driving technological advancements across these fields.more » « less
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Traditionally, FPGA programming has been done via a hardware description language (HDL). An HDL provides fine-grained control over reconfigurable hardware but with limited productivity due to a steep learning curve and tedious design cycle. Thus, high-level synthesis (HLS) approaches have been a significant boon to productivity, and in recent years, OpenCL has emerged as a vendor-agnostic HLS language that offers the added benefit of interoperation with other OpenCL platforms (e.g., CPU, GPU, DSP) and existing OpenCL software. However, OpenCL's productivity can also suffer from tedious boilerplate code and the need to manually coordinate the host (i.e., CPU) and device (i.e., FPGA or other device). So, we present MetaCL, a compiler-assisted interface that takes OpenCL kernel functions as input and automatically generates OpenCL host-side code as output. MetaCL produces more efficient and readable host-side code, ensures portability, and introduces minimal additional runtime overhead compared to unassisted OpenCL development.more » « less
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Abstract The presence of contaminants of emerging concerns (CECs) such as pharmaceuticals and personal care products, endocrine disrupting compounds (EDCs), per/poly‐fluorinated substances (PFAS), pesticides, and nanomaterials poses significant challenges to the environment and human health. This review discusses the current status of electrochemical sensing methods and their potential as low‐cost analytical platforms for the detection and characterization of emerging contaminants. Recent developments in advanced materials and fabrication techniques such as electrophoretic deposition, layer‐by‐layer deposition, roll‐to‐roll and 3D printing techniques, and the scalable manufacturing of low‐cost portable electrochemical devices are discussed. Examples of detection mechanisms, electrode modification procedures, device configuration, and their performance along with recent developments in fundamental electrochemistry, particularly nanoimpact methods, are provided to demonstrate the capabilities of these methods for the environmental monitoring of CECs. Finally, a critical discussion of future research needs, detection challenges, and opportunities is provided to demonstrate how electrochemistry can be used to advance field monitoring of these chemicals. These methods can be used as complementary or alternative methods to the currently used laboratory‐based analytical instrumentation to facilitate large‐scale studies and manage risks associated with the presence of CECs in the environment and other matrices.
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Abstract Nanoelectrochemistry allows for the investigation of the interaction of per‐ and polyfluoroalkyl substances (PFASs) with silver nanoparticles (AgNPs) and the elucidation of the binding behaviour of PFASs to nanoscale surfaces with high sensitivity. Mechanistic studies supported by single particle collision electrochemistry (SPCE), spectroscopic and density functional theory (DFT) calculations indicate the capability of polyfluorooctane sulfonic acid (PFOS), a representative PFAS, to selectively bind and induce aggregation of AgNPs. Single‐particle measurements provide identification of the “discrete” AgNPs agglomeration (e.g. 2–3 NPs) formed through the inter‐particles F−F interactions and the selective replacement of the citrate stabilizer by the sulfonate of the PFOS. Such interactions are characteristic only for long chain PFAS (‐SO3−) providing a means to selectively identify these substances down to ppt levels. Measuring and understanding the interactions of PFAS at nanoscale surfaces are crucial for designing ultrasensitive methods for detection and for modelling and predicting their interaction in the environment.
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Abstract Nanoelectrochemistry allows for the investigation of the interaction of per‐ and polyfluoroalkyl substances (PFASs) with silver nanoparticles (AgNPs) and the elucidation of the binding behaviour of PFASs to nanoscale surfaces with high sensitivity. Mechanistic studies supported by single particle collision electrochemistry (SPCE), spectroscopic and density functional theory (DFT) calculations indicate the capability of polyfluorooctane sulfonic acid (PFOS), a representative PFAS, to selectively bind and induce aggregation of AgNPs. Single‐particle measurements provide identification of the “discrete” AgNPs agglomeration (e.g. 2–3 NPs) formed through the inter‐particles F−F interactions and the selective replacement of the citrate stabilizer by the sulfonate of the PFOS. Such interactions are characteristic only for long chain PFAS (‐SO3−) providing a means to selectively identify these substances down to ppt levels. Measuring and understanding the interactions of PFAS at nanoscale surfaces are crucial for designing ultrasensitive methods for detection and for modelling and predicting their interaction in the environment.