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1.
Environ Sci Technol ; 58(21): 9091-9101, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38709279

RESUMO

People of all ages consume salt every day, but is it really just salt? Plastic nanoparticles [nanoplastics (NPs)] pose an increasing environmental threat and have begun to contaminate everyday salt in consumer goods. Herein, we developed a combined surface enhanced Raman scattering (SERS) and stimulated Raman scattering (SRS) approach that can realize the filtration, enrichment, and detection of NPs in commercial salt. The Au-loaded (50 nm) anodic alumina oxide substrate was used as the SERS substrate to explore the potential types of NP contaminants in salts. SRS was used to conduct imaging and quantify the presence of the NPs. SRS detection was successfully established through standard plastics, and NPs were identified through the match of the hydrocarbon group of the nanoparticles. Simultaneously, the NPs were quantified based on the high spatial resolution and rapid imaging of the SRS imaging platform. NPs in sea salts produced in Asia, Australasia, Europe, and the Atlantic were studied. We estimate that, depending on the location, an average person could be ingesting as many as 6 million NPs per year through the consumption of sea salt alone. The potential health hazards associated with NP ingestion should not be underestimated.


Assuntos
Análise Espectral Raman , Plásticos , Nanopartículas , Cloreto de Sódio/química
2.
Environ Sci Technol ; 57(50): 21448-21458, 2023 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-38047763

RESUMO

The efficient elimination of per- and polyfluoroalkyl substances (PFASs) from the environment remains a huge challenge and requires advanced technologies. Herein, we demonstrate that perfluorooctanoic acid (PFOA) photochemical decomposition could be significantly accelerated by simply carrying out this process in microdroplets. The almost complete removal of 100 and 500 µg/L PFOA was observed after 20 min of irradiation in microdroplets, while this was achieved after about 2 h in the corresponding bulk phase counterpart. To better compare the defluorination ratio, 10 mg/L PFOA was used typically, and the defluorination rates in microdroplets were tens of times faster than that in the bulk phase reaction system. The high performances in actual water matrices, universality, and scale-up applicability were demonstrated as well. We revealed in-depth that the great acceleration is due to the abundance of the air-water interface in microdroplets, where the reactants concentration enrichment, ultrahigh interfacial electric field, and partial solvation effects synergistically promoted photoreactions responsible for PFOA decomposition, as evidenced by simulated Raman scattering microscopy imaging, vibrational Stark effect measurement, and DFT calculation. This study provides an effective approach and highlights the important roles of air-water interface of microdroplets in PFASs treatment.


Assuntos
Fluorocarbonos , Poluentes Químicos da Água , Água , Caprilatos/química , Poluentes Químicos da Água/química
3.
Environ Sci Technol ; 57(46): 18203-18214, 2023 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-37399235

RESUMO

The increasing prevalence of nanoplastics in the environment underscores the need for effective detection and monitoring techniques. Current methods mainly focus on microplastics, while accurate identification of nanoplastics is challenging due to their small size and complex composition. In this work, we combined highly reflective substrates and machine learning to accurately identify nanoplastics using Raman spectroscopy. Our approach established Raman spectroscopy data sets of nanoplastics, incorporated peak extraction and retention data processing, and constructed a random forest model that achieved an average accuracy of 98.8% in identifying nanoplastics. We validated our method with tap water spiked samples, achieving over 97% identification accuracy, and demonstrated the applicability of our algorithm to real-world environmental samples through experiments on rainwater, detecting nanoscale polystyrene (PS) and polyvinyl chloride (PVC). Despite the challenges of processing low-quality nanoplastic Raman spectra and complex environmental samples, our study demonstrated the potential of using random forests to identify and distinguish nanoplastics from other environmental particles. Our results suggest that the combination of Raman spectroscopy and machine learning holds promise for developing effective nanoplastic particle detection and monitoring strategies.


Assuntos
Microplásticos , Poluentes Químicos da Água , Plásticos , Análise Espectral Raman , Algoritmos , Aprendizado de Máquina , Poliestirenos , Água
4.
Angew Chem Int Ed Engl ; 62(27): e202304189, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37144910

RESUMO

Solar-driven CO2 reduction reaction (CO2 RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalytic CO2 RR efficiency at the abundant gas-liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk phase reaction. Even in the absence of sacrificial agents, the production rates of HCOOH over WO3 ⋅ 0.33H2 O mediated by microdroplets reaches 2536 µmol h-1 g-1 (vs. 13 µmol h-1 g-1 in bulk phase), which is significantly superior to the previously reported photocatalytic CO2 RR in bulk phase reaction condition. Beyond the efficient delivery of CO2 to photocatalyst surfaces within microdroplets, we reveal that the strong electric field at the gas-liquid interface of microdroplets essentially promotes the separation of photogenerated electron-hole pairs. This study provides a deep understanding of ultrafast reaction kinetics promoted by the gas-liquid interface of microdroplets and a novel way of addressing the low efficiency of photocatalytic CO2 reduction to fuel.

5.
PNAS Nexus ; 2(11): pgad389, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38034096

RESUMO

The origin of life on Earth is an enigmatic and intricate conundrum that has yet to be comprehensively resolved despite recent significant developments within the discipline of archaeology and geology. Chemically, metal-sulfide minerals are speculated to serve as an important medium for giving birth in early life, while yet so far direct evidence to support the hypothesis for the highly efficient conversion of inorganic carbon into praxiological biomolecules remains scarce. In this work, we provide an initial indication that sphalerite, employed as a typical mineral, shows its enormous capability for promoting the conversion of inorganic carbon into elementary biomolecule formic acid (HCOOH) in airborne mineral-bearing aerosol microdroplet, which is over two orders of magnitude higher than that of the corresponding conventional bulk-like aqueous phase medium in the environment (e.g. river, lake, sea, etc.). This significant enhancement was further validated by a wide range of minerals and clays, including CuS, NiS, CoS, CdS, MnS, elemental sulfur, Arizona Test Dust, loess, nontronite, and montmorillonite. We reveal that the abundant interface of unique physical-chemical features instinct for aerosol or cloud microdroplets reduces the reaction energy barrier for the reaction, thus leading to extremely high HCOOH production (2.52 × 1014 kg year-1). This study unfolds unrecognized remarkable contributions of the considered scheme in the accumulation of prebiotic biomolecules in the ancient period of the Earth.

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