Your browser doesn't support javascript.
loading
Show: 20 | 50 | 100
Results 1 - 8 de 8
Filter
Add more filters










Database
Language
Publication year range
1.
Environ Sci Technol ; 58(21): 9091-9101, 2024 May 28.
Article in English | MEDLINE | ID: mdl-38709279

ABSTRACT

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.


Subject(s)
Spectrum Analysis, Raman , Plastics , Nanoparticles , Sodium Chloride/chemistry
2.
J Am Chem Soc ; 146(10): 6580-6590, 2024 Mar 13.
Article in English | MEDLINE | ID: mdl-38427385

ABSTRACT

The multiphase oxidation of sulfur dioxide (SO2) to form sulfate is a complex and important process in the atmosphere. While the conventional photosensitized reaction mainly explored in the bulk medium is reported to be one of the drivers to trigger atmospheric sulfate production, how this scheme functionalizes at the air-water interface (AWI) of aerosol remains an open question. Herein, employing an advanced size-controllable microdroplet-printing device, surface-enhanced Raman scattering (SERS) analysis, nanosecond transient adsorption spectrometer, and molecular level theoretical calculations, we revealed the previously overlooked interfacial role in photosensitized oxidation of SO2 in humic-like substance (HULIS) aerosol, where a 3-4 orders of magnitude increase in sulfate formation rate was speculated in cloud and aerosol relevant-sized particles relative to the conventional bulk-phase medium. The rapid formation of a battery of reactive oxygen species (ROS) comes from the accelerated electron transfer process at the AWI, where the excited triplet state of HULIS (3HULIS*) of the incomplete solvent cage can readily capture electrons from HSO3- in a way that is more efficient than that in the bulk medium fully blocked by water molecules. This phenomenon could be explained by the significantly reduced desolvation energy barrier required for reagents residing in the AWI region with an open solvent shell.

3.
Environ Sci Technol ; 57(50): 21448-21458, 2023 Dec 19.
Article in English | MEDLINE | ID: mdl-38047763

ABSTRACT

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.


Subject(s)
Fluorocarbons , Water Pollutants, Chemical , Water , Caprylates/chemistry , Water Pollutants, Chemical/chemistry
4.
PNAS Nexus ; 2(11): pgad389, 2023 Nov.
Article in English | MEDLINE | ID: mdl-38034096

ABSTRACT

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.

5.
Angew Chem Int Ed Engl ; 62(27): e202304189, 2023 Jul 03.
Article in English | MEDLINE | ID: mdl-37144910

ABSTRACT

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.

6.
Comput Intell Neurosci ; 2022: 7603319, 2022.
Article in English | MEDLINE | ID: mdl-35096047

ABSTRACT

This paper proposes a feature fusion-based improved capsule network (FFiCAPS) to improve the performance of surface electromyogram (sEMG) signal recognition with the purpose of distinguishing hand gestures. Current deep learning models, especially convolution neural networks (CNNs), only take into account the existence of certain features and ignore the correlation among features. To overcome this problem, FFiCAPS adopts the capsule network with a feature fusion method. In order to provide rich information, sEMG signal information and feature data are incorporated together to form new features as input. Improvements made on capsule network are multilayer convolution layer and e-Squash function. The former aggregates feature maps learned by different layers and kernel sizes to extract information in a multiscale and multiangle manner, while the latter grows faster at later stages to strengthen the sensitivity of this model to capsule length changes. Finally, simulation experiments show that the proposed method exceeds other eight methods in overall accuracy under the condition of electrode displacement (86.58%) and among subjects (82.12%), with a notable improvement in recognizing hand open and radial flexion, respectively.


Subject(s)
Gestures , Neural Networks, Computer , Electromyography , Humans , Recognition, Psychology
7.
Bioresour Technol ; 340: 125704, 2021 Nov.
Article in English | MEDLINE | ID: mdl-34375792

ABSTRACT

Nitrous oxide (N2O) emission from wastewater treatment plants (WWTPs) requires urgent mitigation because of its significant contribution to the greenhouse effect. In this study, bioaugmentation was applied in a pilot-scale oxidation ditch with the aerobic denitrifying bacteria strain PCN-1 immobilized on polyurethane biocarriers, which demonstrated effective N2O mitigation. Microbial community analysis suggested that the bioaugmentation facilitated a symbiotic relationship of the bacterial populations between the activated sludge and the biocarriers. The denitrifying bacteria with well-known N2O reducing capabilities predominated on the biocarriers. Correspondingly, the increases of denitrifying genes and NO and N2O reductase provided evidence for the enhanced genetic potential for NO and N2O reduction. Besides, the enriched comammox Nitrospira on the biocarriers is proposed as another significant driver for N2O mitigation by avoiding nitrite accumulation. In addition, the bioaugmentation enhanced the stability and recovery capability of the system in the ammonia overload and aeration failure shock tests.


Subject(s)
Bioreactors , Nitrous Oxide , Ammonia , Bacteria/genetics , Denitrification , Nitrous Oxide/analysis , Sewage
8.
Sci Total Environ ; 798: 149107, 2021 Dec 01.
Article in English | MEDLINE | ID: mdl-34325147

ABSTRACT

Uranium (U) pollution is an environmental hazard caused by the development of the nuclear industry. Microbial reduction of hexavalent uranium (U(VI)) to tetravalent uranium (U(IV)) reduces U solubility and mobility and has been proposed as an effective method to remediate uranium contamination. In this review, U(VI) remediation with respect to U(VI)-reducing bacteria, mechanisms, influencing factors, products, and reoxidation are systematically summarized. Reportedly, some metal- and sulfate-reducing bacteria possess excellent U(VI) reduction capability through mechanisms involving c-type cytochromes, extracellular pili, electron shuttle, or thioredoxin reduction. In situ remediation has been demonstrated as an ideal strategy for large-scale degradation of uranium contaminants than ex situ. However, U(VI) reduction efficiency can be affected by various factors, including pH, temperature, bicarbonate, electron donors, and coexisting metal ions. Furthermore, it is noteworthy that the reduction products could be reoxidized when exposed to oxygen and nitrate, inevitably compromising the remediation effects, especially for non-crystalline U(IV) with weak stability.


Subject(s)
Uranium , Water Pollutants, Radioactive , Bacteria , Biodegradation, Environmental , Nitrates , Oxidation-Reduction , Uranium/analysis
SELECTION OF CITATIONS
SEARCH DETAIL
...