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1.
Environ Sci Technol ; 58(19): 8380-8392, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38691504

RESUMEN

A comprehensive understanding of the full volatility spectrum of organic oxidation products from the benzene series precursors is important to quantify the air quality and climate effects of secondary organic aerosol (SOA) and new particle formation (NPF). However, current models fail to capture the full volatility spectrum due to the absence of important reaction pathways. Here, we develop a novel unified model framework, the integrated two-dimensional volatility basis set (I2D-VBS), to simulate the full volatility spectrum of products from benzene series precursors by simultaneously representing first-generational oxidation, multigenerational aging, autoxidation, dimerization, nitrate formation, etc. The model successfully reproduces the volatility and O/C distributions of oxygenated organic molecules (OOMs) as well as the concentrations and the O/C of SOA over wide-ranging experimental conditions. In typical urban environments, autoxidation and multigenerational oxidation are the two main pathways for the formation of OOMs and SOA with similar contributions, but autoxidation contributes more to low-volatility products. NOx can reduce about two-thirds of OOMs and SOA, and most of the extremely low-volatility products compared to clean conditions, by suppressing dimerization and autoxidation. The I2D-VBS facilitates a holistic understanding of full volatility product formation, which helps fill the large gap in the predictions of organic NPF, particle growth, and SOA formation.


Asunto(s)
Benceno , Benceno/química , Compuestos Orgánicos/química , Oxidación-Reducción , Aerosoles , Volatilización , Contaminantes Atmosféricos , Modelos Teóricos
2.
Sci Rep ; 14(1): 8805, 2024 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-38627475

RESUMEN

Compressive sensing is favored because it breaks through the constraints of Nyquist sampling law in signal reconstruction. However, the security defects of joint compression encryption and the problem of low quality of reconstructed image restoration need to be solved urgently. In view of this, this paper proposes a compressive sensing image encryption scheme based on optimized orthogonal measurement matrix. Utilizing a combination of DWT and OMP, along with chaos, the proposed scheme achieves high-security image encryption and superior quality in decryption reconstruction. Firstly, the orthogonal optimization method is used to improve the chaotic measurement matrix. Combined with Part Hadamard matrix, the measurement matrix with strong orthogonal characteristics is constructed by Kronecker product. Secondly, the original image is sparsely represented by DWT. Meanwhile, Arnold scrambling is used to disturb the correlation between its adjacent pixels. Following this, the image is compressed and measured in accordance with the principles of compressive sensing and obtain the intermediate image to be encrypted. Finally, the chaotic sequence generated based on 2D-LSCM is used to perform on odd-even interleaved diffusion and row-column permutation at bit-level to obtain the final ciphertext. The experimental results show that this scheme meets the cryptographic requirements of obfuscation, diffusion and avalanche effects, and also has a large key space, which is sufficient to resist brute-force cracking attacks. Based on the sparse and reconstruction algorithm of compressive sensing proposed in this paper, it has better image restoration quality than similar algorithms. Consequently, the compressive sensing image encryption scheme enhances both security and reconstruction quality, presenting promising applications in the evolving landscape of privacy protection for network big data.

3.
Sci Total Environ ; 918: 170512, 2024 Mar 25.
Artículo en Inglés | MEDLINE | ID: mdl-38286278

RESUMEN

Wintertime fine particle (PM2.5) pollution remains to be perplexing air quality problems in many parts of China. In this study, PM2.5 compositions and aerosol acidity at different pollution levels at an urban cite in the southwest China's Sichuan Basin were investigated during a sustained winter haze episode. Organic matter was the most abundant component of PM2.5, followed by nitrate, sulfate and ammonium. Shares of organic aerosol in PM2.5 mass decreased with the elevated PM2.5 levels, while the enhancements of sulfate and secondary organic aerosol were much less than that of nitrate and ammonium during heavy pollution with increased ratios of nitrate to sulfate, implying a significant role of nitrate in the haze formation. Results also suggest the nighttime chemistry might contribute substantially to the formation of nitrate under severe pollutions. The daily average aerosol pH showed a decreasing trend with the elevated levels of PM2.5, and this increased aerosl acidity was mainly due to the fast rising secondary inorganic aerosol (SIA) concentration, with the increase in hydronium ion concentration in air (Hair+) surpassing the dilution effect of elevated aerosol liquid water content (LWC). Thermodynamic model calculations revealed that the air environment was NH3-rich with total NHx (NH3 + NH4+) greater than required NHx, and the aerosol pH exponentially declined with the decreasing excess NHx (p < 0.01). This study demonstrated that under air stagnation and NH3-rich environment during winter, the raised relative humidity (RH) would lead to an increase in LWC and thereby facilitate the aqueous chemistry processes with the neutralization capacity of NH3 to form sulfate and nitrate, which would further increase the LWC and lower the pH. This self-amplifying SIA formation might be crucial to the severe PM2.5 pollution and haze events during winter, and therefore cutting both NOx and NH3 emissions would benefit stopping the self-amplification.

4.
Chem Commun (Camb) ; 59(97): 14341-14352, 2023 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-37987689

RESUMEN

The construction of carbon-nitrogen bonds is vital for producing versatile nitrogenous compounds for the chemical and pharmaceutical industries. Among developed synthetic approaches to nitrogenous chemicals, photocatalysis is particularly prominent and has become one of the emerging fields due to its unique advantages of eco-sustainable characteristics, efficient process integration, no need for high-pressure H2, and tunable synthesis methods for developing advanced photocatalytic materials. Here, the review focuses on potential photocatalytic protocols developed for the construction of robust carbon-nitrogen bonds in discrepant activation environments to produce high-value nitrogenous chemicals. The photocatalytic C-N bond construction strategies and involved reaction mechanisms are elucidated.

5.
Environ Sci Process Impacts ; 25(10): 1645-1656, 2023 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-37721367

RESUMEN

Chlorine plays an important role in tropospheric oxidation processes, in both marine and continental environments. Although modeling studies have explored the importance of halogen chemistry, uncertainty remains in associated chemical mechanisms and fundamental kinetics parameters. Prior kinetics measurements of multiphase halogen recycling reactions have been largely performed with dilute, bulk solutions, leaving unexplored more realistic chemical systems which have high solute concentrations and are internally mixed with both halide and organic components. Here, we address the multiphase kinetics of gaseous HOCl using an aerosol flow tube and aerosol mass spectrometer to study its reactions with particulate chloride, using atmospherically relevant particle acidity, solute concentrations, and ionic strength. We also investigate the chemistry that results when biomass burning (BB) aerosol components and chloride are internally mixed. Using pH-buffered deliquesced particles, we show that the rate constant for reaction of dissolved HOCl with H+ and Cl- at high relative humidity (RH) (80-85%) is within a factor of two of the literature value for bulk phase conditions. However, at lower RH values (60-70%) where the particles are considerably more concentrated, the rate constant for chloride loss from the particles is an order of magnitude higher. For pure organic compounds commonly found in biomass burning (BB) aerosol, such as coniferaldehyde, salicylic acid and furfural, an increase in the aerosol chlorine content occurs with HOCl exposure, indicating the formation of organochlorine species. Together, these independent findings explain results for internally mixed aerosol particles with both chloride and BB components present where we observed behavior consistent with both chloride loss and organochlorine formation occurring simultaneously upon HOCl exposure. Our results indicate that chlorine recycling via HOCl uptake by chloride-containing particles will occur in the atmosphere efficiently over a wide range of RH conditions, even when reactive organic compounds are present in the same particles as chloride. Simultaneously, formation of organochlorine compounds, which are commonly toxic, is likely occurring when reactive organic components are present.


Asunto(s)
Cloruros , Cloro , Ácido Hipocloroso , Halógenos , Aerosoles/química , Cinética
6.
Sci Rep ; 13(1): 14721, 2023 Sep 07.
Artículo en Inglés | MEDLINE | ID: mdl-37679414

RESUMEN

This paper proposes a video security transmission enhancement algorithm based on block permutation and dynamic multiplexing sequences encryption based on 4D autonomous hyperchaotic system. Firstly, we employ the block permutation encryption and diffusion confusion encryption module, which is based on dynamic multiplexing chaotic sequences, to encrypt the plaintext and obtain the ciphertext. Subsequently, the hash value of this round's ciphertext is utilized to generate the chaotic key, produced by the multiplexing sequence of this round after mathematical processing. Then, the key is used to generate the chaotic sequence to confuse the N-th of the multiplexed sequence, and the next round of multiplexed sequence is obtained. If the current round of chaotic sequence has been completely confused, the chaotic sequence is re-generated to generate a new multiplex sequence by using the key generated by the current round key and the initial key. Finally, the above steps are repeated for the encryption of each frame of the video. Compared with the traditional permutation coding algorithm, it increases the difficulty of estimation or recognition while ensuring efficiency, and effectively improves the avalanche effect of the algorithm. Through frame by frame ciphertext closed-loop feedback, it has the ability to resist known plaintext attack and selected plaintext attack. The results show that the scheme has high security and significant diffusion characteristics, and can effectively resist various common cryptographic attacks.

7.
Nat Commun ; 14(1): 3347, 2023 Jun 08.
Artículo en Inglés | MEDLINE | ID: mdl-37291087

RESUMEN

The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO2) greatly impacts the formation of highly oxygenated organic molecules (HOM), the key precursors of secondary organic aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on HOM formation from monoterpenes at low NO concentrations (0 - 82 pptv). We demonstrate that such low NO can enhance HOM production by modulating the RO2 loss and favoring the formation of alkoxy radicals that can continue to autoxidize through isomerization. These insights suggest that HOM yields from typical boreal forest emissions can vary between 2.5%-6.5%, and HOM formation will not be completely inhibited even at high NO concentrations. Our findings challenge the notion that NO monotonically reduces HOM yields by extending the knowledge of RO2-NO interactions to the low-NO regime. This represents a major advance towards an accurate assessment of HOM budgets, especially in low-NO environments, which prevails in the pre-industrial atmosphere, pristine areas, and the upper boundary layer.


Asunto(s)
Atmósfera , Óxido Nítrico , Monoterpenos , Oxidación-Reducción , Aerosoles
8.
Nat Commun ; 14(1): 2703, 2023 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-37164951

RESUMEN

Black carbon (BC) plays an important role in the climate system because of its strong warming effect, yet the magnitude of this effect is highly uncertain owing to the complex mixing state of aerosols. Here we build a unified theoretical framework to describe BC's mixing states, linking dynamic processes to BC coating thickness distribution, and show its self-similarity for sites in diverse environments. The size distribution of BC-containing particles is found to follow a universal law and is independent of BC core size. A new mixing state module is established based on this finding and successfully applied in global and regional models, which increases the accuracy of aerosol climate effect estimations. Our theoretical framework links observations with model simulations in both mixing state description and light absorption quantification.

9.
Front Environ Sci Eng ; 17(9): 114, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37125146

RESUMEN

Organic aerosol (OA) is a major component of atmospheric particulate matter (PM) with complex composition and formation processes influenced by various factors. Emission reduction can alter both precursors and oxidants which further affects secondary OA formation. Here we provide an observational analysis of secondary OA (SOA) variation properties in Yangtze River Delta (YRD) of eastern China in response to large scale of emission reduction during Chinese New Year (CNY) holidays from 2015 to 2020, and the COVID-19 pandemic period from January to March, 2020. We found a 17% increase of SOA proportion during the COVID lockdown. The relative enrichment of SOA is also found during multi-year CNY holidays with dramatic reduction of anthropogenic emissions. Two types of oxygenated OA (OOA) influenced by mixed emissions and SOA formation were found to be the dominant components during the lockdown in YRD region. Our results highlight that these emission-reduction-induced changes in organic aerosol need to be considered in the future to optimize air pollution control measures. Electronic Supplementary Material: Supplementary material is available in the online version of this article at 10.1007/s11783-023-1714-0 and is accessible for authorized users.

10.
Environ Sci Technol ; 57(16): 6609-6615, 2023 04 25.
Artículo en Inglés | MEDLINE | ID: mdl-37040454

RESUMEN

Multiphase oxidation of sulfur dioxide (SO2) by ozone (O3) in alkaline sea salt aerosols is an important source of sulfate aerosols in the marine atmosphere. However, a recently reported low pH of fresh supermicron sea spray aerosols (mainly sea salt) would argue against the importance of this mechanism. Here, we investigated the impact of ionic strength on the kinetics of multiphase oxidation of SO2 by O3 in proxies of aqueous acidified sea salt aerosols with buffered pH of ∼4.0 via well-controlled flow tube experiments. We find that the sulfate formation rate for the O3 oxidation pathway proceeds 7.9 to 233 times faster under high ionic strength conditions of 2-14 mol kg-1 compared to the dilute bulk solutions. The ionic strength effect is likely to sustain the importance of multiphase oxidation of SO2 by O3 in sea salt aerosols in the marine atmosphere. Our results indicate that atmospheric models should consider the ionic strength effects on the multiphase oxidation of SO2 by O3 in sea salt aerosols to improve the predictions of the sulfate formation rate and the sulfate aerosol budget in the marine atmosphere.


Asunto(s)
Contaminantes Atmosféricos , Ozono , Dióxido de Azufre , Sulfatos , Óxidos de Azufre , Atmósfera , Agua , Aerosoles , Concentración Osmolar
11.
Environ Sci Technol ; 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36630690

RESUMEN

Wildfires are a major source of biomass burning aerosol to the atmosphere, with their incidence and intensity expected to increase in a warmer future climate. However, the toxicity evolution of biomass burning organic aerosol (BBOA) during atmospheric aging remains poorly understood. In this study, we report a unique set of chemical and toxicological metrics of BBOA from pine wood smoldering during multiphase aging by gas-phase hydroxyl radicals (OH). Both the fresh and OH-aged BBOA show activity relevant to adverse health outcomes. The results from two acellular assays (DTT and DCFH) show significant oxidative potential (OP) and reactive oxygen species (ROS) formation in OH-aged BBOA. Also, radical concentrations in the aerosol assessed by electron paramagnetic resonance (EPR) spectroscopy increased by 50% following heterogeneous aging. This enhancement was accompanied by a transition from predominantly carbon-centered radicals (85%) in the fresh aerosol to predominantly oxygen-centered radicals (76%) following aging. Both the fresh and aged biomass burning aerosols trigger prominent antioxidant defense during the in vitro exposure, indicating the induction of oxidative stress by BBOA in the atmosphere. By connecting chemical composition and toxicity using an integrated approach, we show that short-term aging initiated by OH radicals can produce biomass burning particles with a higher particle-bound ROS generation capacity, which are therefore a more relevant exposure hazard for residents in large population centers close to wildfire regions than previously studied fresh biomass burning emissions.

12.
Bioresour Technol ; 369: 128390, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36435420

RESUMEN

Thermocatalytic (trans)esterification of oils/lipids to produce biodiesel is generally energy-consuming, reversible, and controlled by the equilibrium law. Herein, a light-induced photothermal process was illustrated to be highly efficient for biodiesel production (96.8 % yield) from microalgae lipids at room temperature enabled by a biomass-based SO3H-functionalized graphene-like heterogeneous catalyst (S-NGL-600), as optimized by response surface methodology. Infrared thermal imaging indicated that interfacial solar heating led to forming a local photothermal catalytic system, reaching 72.2 °C in 2 min. The local light heating was conducive to evaporation and removal of water from acid sites, resulting in local excess of microalgae lipids to facilitate the forward reaction. Notably, the photothermal catalyst was highly recyclable and exhibited a significantly higher conversion rate of microalgae lipids than industrially used catalyst H2SO4. Life cycle assessment suggested energy-saving advantage (0.87 MJ/MJ) and environmental protection (-89.42 CO2eq/MJ) of the photothermal-driven protocol for microalgae biodiesel production.


Asunto(s)
Microalgas , Animales , Biocombustibles , Aceites , Esterificación , Biomasa , Estadios del Ciclo de Vida
13.
Dalton Trans ; 51(43): 16668-16680, 2022 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-36278834

RESUMEN

trans-Anethole (trans-AN) is widely applied in food, daily necessities, and pharmaceuticals and is typically available from inefficient natural oil extraction or complex organic transformations over mineral acid or noble metals. Here, a green and sustainable route was developed to stereoselectively produce trans-AN (ca. 90% selectivity) over an organic polymeric phosphonate-hafnium catalyst (PAS-Hf) through the cascade transfer hydrogenation and dehydration of biomass-based 4'-methoxypropiophenone (4-MOPP), with an environmental impact factor (E-factor) of 47.73. The porous structure and the enhanced hydrophobicity of the spherical catalyst PAS-Hf ensured the formation of more accessible and stable Lewis (Hf4+) and Brønsted (SO3H) acid active sites, which could be used for rapid conversion of biomass-based 4-MOPP to AN (100% conversion, 97.2% yield) in 0.5-2 h (TOF: 9.3 h-1). Density functional theory (DFT) calculations elucidated that the addition of PAS-Hf could remarkably facilitate the overall conversion process by decreasing the reaction energy barrier (151.33 to 48.27 kJ mol-1) of the rate-determining step. The good thermal stability and heterogeneity of the bifunctional catalyst were responsible for its constant activity during at least five consecutive cycles. The synergistic/relay catalysis of Lewis acid-base and Brønsted acid species could be extended to more than ten kinds of aldehydes and ketones. This acid-base multi-catalytic protocol has considerable potential in cascade biomass conversion via heterogeneous catalysis without any base additive.


Asunto(s)
Derivados de Alilbenceno , Catálisis , Anisoles , Bases de Lewis , Interacciones Hidrofóbicas e Hidrofílicas
14.
Environ Res ; 209: 112751, 2022 06.
Artículo en Inglés | MEDLINE | ID: mdl-35077717

RESUMEN

Secondary organic aerosols (SOA) constitute a large fraction of atmospheric aerosols, yet our knowledge of the formation and aging processes of SOA in megacities of China is still limited. In this work, the formation and aging processes of SOA in winter in Beijing was investigated using a high-resolution aerosol mass spectrometer (AMS) and an oxidation flow reactor (OFR). Our results showed that the OA enhancement from OH aging peaked at ∼3.9 equivalent days with an average enhancement of 0.9 (±0.3) µg m-3. Positive matrix factorization analysis of AMS-OFR data identified three primary OA (POA) and two SOA factors. While the concentrations of POA factors decreased as a function of photochemical age, the two SOA factors showed clear enhancements by 2.5 and 4.3 µg m-3 at ∼3.9 and ∼2.6 days of equivalent photochemical age, respectively. The average contribution of SOA to the total OA was 47% in ambient air and 87% in OFR-oxidized ambient air. The elevated oxygen-to-carbon (O/C) ratio from 0.49 to 0.77-0.82 and the decreased hydrogen-to-carbon (H/C) from 1.37 to ∼1.1 highlighted the formation of more oxidized SOA during photochemical aging in winter in Beijing. The ubiquitous SOA enhancement as a function of OA levels indicated the significant formation potential of SOA in winter, and it varied differently among different episodes. In particular, we observed a maximum SOA enhancement of 38.6 µg m-3 during a biomass burning event. This result demonstrates that photochemical oxidation of ubiquitous biomass burning emissions can be a large source of SOA in winter in North China Plain.


Asunto(s)
Contaminantes Atmosféricos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Beijing , China
15.
Environ Pollut ; 292(Pt A): 118266, 2022 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-34610414

RESUMEN

Cooking is an important source of organic aerosols (OA), particularly in urban areas, but it has not been explicitly included in current emission inventories in China. This study estimated the organic aerosol emissions from cooking during winter over the Pearl River Delta (PRD) region, China. Using the retrieved hourly cooking organic aerosol (COA) concentrations at two sites in Hong Kong and Guangzhou, population density, and daily per capita COA emissions, we determined the spatial and temporal distribution of COA emissions over the PRD region based on two approaches by treating COA as non-volatile (NVCOA) and semi-volatile (SVCOA), respectively. By using the estimated COA emissions and the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) model, we reproduced the diurnal cycles of COA concentrations at the PolyU site in Hong Kong and Panyu site in Guangzhou. We also resolved the different patterns of COA between weekdays and weekends. The mean COA concentration during wintertime over the urban areas of the PRD region was 0.7 µg m-3 and 0.9 µg m-3 for the NVCOA and SVCOA cases, respectively, contributing 5.1% and 6.9% to the urban OA concentrations. The total COA emissions in winter over the PRD region were estimated to be 3.5 × 108 g month-1 and 3.8 × 108 g month-1 for the NVCOA and SVCOA cases, respectively, adding 34.8% and 37.8% to the total primary organic aerosol emissions. Considering COA emissions in the model increased the mean regional OA concentrations by 4.6% and 7.4% for the NVCOA and SVCOA cases, respectively. Our study therefore highlights the importance of cooking activities to OA concentrations in winter over the PRD region.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , China , Culinaria , Monitoreo del Ambiente , Material Particulado/análisis
16.
IEEE Trans Pattern Anal Mach Intell ; 44(10): 6327-6344, 2022 10.
Artículo en Inglés | MEDLINE | ID: mdl-34106844

RESUMEN

In this paper, we propose a pose grammar to tackle the problem of 3D human pose estimation from a monocular RGB image. Our model takes estimated 2D pose as the input and learns a generalized 2D-3D mapping function to leverage into 3D pose. The proposed model consists of a base network which efficiently captures pose-aligned features and a hierarchy of Bi-directional RNNs (BRNNs) on the top to explicitly incorporate a set of knowledge regarding human body configuration (i.e., kinematics, symmetry, motor coordination). The proposed model thus enforces high-level constraints over human poses. In learning, we develop a data augmentation algorithm to further improve model robustness against appearance variations and cross-view generalization ability. We validate our method on public 3D human pose benchmarks and propose a new evaluation protocol working on cross-view setting to verify the generalization capability of different methods. We empirically observe that most state-of-the-art methods encounter difficulty under such setting while our method can well handle such challenges.


Asunto(s)
Algoritmos , Postura , Fenómenos Biomecánicos , Humanos
17.
Nat Chem ; 13(12): 1173-1177, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34594012

RESUMEN

Although the multiphase chemistry of SO2 in aerosol particles is of great importance to air quality under polluted haze conditions, a fundamental understanding of the pertinent mechanisms and kinetics is lacking. In particular, there is considerable debate on the importance of NO2 in the oxidation of SO2 in aerosol particles. Here experiments with atmospherically relevant deliquesced particles at buffered pH values of 4-5 show that the effective rate constant for the reaction of NO2 with SO32- ((1.4 ± 0.5) × 1010 M-1 s-1) is more than three orders of magnitude larger than the value in dilute solutions. An interfacial reaction at the surface of aerosol particles probably drives the very fast kinetics. Our results indicate that oxidation of SO2 by NO2 at aerosol surfaces may be an important source of sulfate aerosols under polluted haze conditions.

18.
Sci Total Environ ; 794: 148638, 2021 Nov 10.
Artículo en Inglés | MEDLINE | ID: mdl-34217089

RESUMEN

Cooking is an important source of primary organic aerosol (POA) in urban areas, and it may also generate abundant non-methane organic gases (NMOGs), which form oxidized organic aerosol (OOA) after atmospheric oxidation. Edible fats play an important role in a balanced diet and are part of various types of cooking. We conducted laboratory studies to examine the primary emissions of POA and NMOGs and OOA formation using an oxidation flow reactor (OFR) for three animal fats (i.e., lard, beef and chicken fats) heated at two different temperatures (160 and 180 °C). Positive matrix factorization (PMF) revealed that OOA formed together with POA loss after photochemical aging, suggesting the conversion of some POA to OOA. The maximum OOA production rates (PRs) from heated animal fats, occurring under OH exposures (OHexp) of 8.3-15 × 1010 molecules cm-3 s, ranged from 8.9 to 24.7 µg min-1, 1.6-14.5 times as high as initial POA emission rates (ERs). NMOG emissions from heated animal fats were dominated by aldehydes, which contributed 14-71% of the observed OOA. We estimated that cooking-related OOA could contribute to as high as ~10% of total organic aerosol (OA) in an urban area in Hong Kong, where cooking OA (COA) dominated the POA. This study provides insights into the potential contribution of cooking to urban OOA, which might be especially pronounced when cooking contributions dominate the primary emissions.


Asunto(s)
Contaminantes Atmosféricos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Animales , Culinaria , Calor , Oxidación-Reducción , Material Particulado/análisis
19.
ACS Appl Mater Interfaces ; 13(14): 16355-16363, 2021 Apr 14.
Artículo en Inglés | MEDLINE | ID: mdl-33797219

RESUMEN

Urea electrolysis has prospects for urea-containing wastewater purification and hydrogen (H2) production, but the shortage of cost-effective catalysts restricts its development. In this work, the tomentum-like FeNi3-MoO2 heterojunction nanosheets array self-supported on nickel foam (NF) as bifunctional catalyst is prepared by facile hydrothermal and annealing method. Only 1.29 V and -50.8 mV is required to obtain ±10 mA cm-2 for urea oxidation and hydrogen evolution reaction (UOR and HER), respectively, showing great bifunctional catalytic activity. For overall urea electrolysis, it only needs 1.37 V to reach 10 mA cm-2 and can last at 100 mA cm-2 for 70 h without obvious activity attenuation, showing outstanding durability. Coupling interface constructions of FeNi3-MoO2 heterostructures, novel morphology with a mesoporous and self-supporting structure could be the reason for this good performance. This work thus proposes a promising catalyst for boosting UOR and HER to realize efficient overall urea electrolysis.

20.
Environ Sci Technol ; 55(8): 4227-4242, 2021 04 20.
Artículo en Inglés | MEDLINE | ID: mdl-33760581

RESUMEN

Atmospheric oxidation of sulfur dioxide (SO2) forms sulfate-containing aerosol particles that impact air quality, climate, and human and ecosystem health. It is well-known that in-cloud oxidation of SO2 frequently dominates over gas-phase oxidation on regional and global scales. Multiphase oxidation involving aerosol particles, fog, and cloud droplets has been generally thought to scale with liquid water content (LWC) so multiphase oxidation would be negligible for aerosol particles due to their low aerosol LWC. However, recent field evidence, particularly from East Asia, shows that fast sulfate formation prevails in cloud-free environments that are characterized by high aerosol loadings. By assuming that the kinetics of cloud water chemistry prevails for aerosol particles, most atmospheric models do not capture this phenomenon. Therefore, the field of aerosol SO2 multiphase chemistry has blossomed in the past decade, with many oxidation processes proposed to bridge the difference between modeled and observed sulfate mass loadings. This review summarizes recent advances in the fundamental understanding of the aerosol multiphase oxidation of SO2, with a focus on environmental conditions that affect the oxidation rate, experimental challenges, mechanisms and kinetics results for individual reaction pathways, and future research directions. Compared to dilute cloud water conditions, this paper highlights the differences that arise at the molecular level with the extremely high solute strengths present in aerosol particles.


Asunto(s)
Contaminantes Atmosféricos , Dióxido de Azufre , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Ecosistema , Asia Oriental , Humanos , Sulfatos/análisis
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