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1.
Nature ; 631(8019): 98-105, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38867037

ABSTRACT

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed1,2. Although new particle formation (NPF) mechanisms have been described at specific sites3-6, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes1,7. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO3 probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10-80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.

2.
Proc Natl Acad Sci U S A ; 120(47): e2302126120, 2023 Nov 21.
Article in English | MEDLINE | ID: mdl-37967215

ABSTRACT

Neurotransmitter receptors are increasingly recognized to play important roles in anti-tumor immunity. The expression of the ion channel N-methyl-D-aspartate receptor (NMDAR) on macrophages was reported, but the role of NMDAR on macrophages in the tumor microenvironment (TME) remains unknown. Here, we show that the activation of NMDAR triggered calcium influx and reactive oxygen species production, which fueled immunosuppressive activities in tumor-associated macrophages (TAMs) in the hepatocellular sarcoma and fibrosarcoma tumor settings. NMDAR antagonists, MK-801, memantine, and magnesium, effectively suppressed these processes in TAMs. Single-cell RNA sequencing analysis revealed that blocking NMDAR functionally and metabolically altered TAM phenotypes, such that they could better promote T cell- and Natural killer (NK) cell-mediated anti-tumor immunity. Treatment with NMDAR antagonists in combination with anti-PD-1 antibody led to the elimination of the majority of established preclinical liver tumors. Thus, our study uncovered an unknown role for NMDAR in regulating macrophages in the TME of hepatocellular sarcoma and provided a rationale for targeting NMDAR for tumor immunotherapy.


Subject(s)
Liver Neoplasms , Sarcoma , Humans , Tumor-Associated Macrophages , Neoplastic Processes , Memantine , Tumor Microenvironment
3.
Proc Natl Acad Sci U S A ; 119(43): e2207693119, 2022 10 25.
Article in English | MEDLINE | ID: mdl-36252039

ABSTRACT

Although the onset time of chemical reactions can be manipulated by mechanical, electrical, and optical methods, its chemical control remains highly challenging. Herein, we report a chemical timer approach for manipulating the emission onset time of chemiluminescence (CL) reactions. A mixture of Mn2+, NaHCO3, and a luminol analog with H2O2 produced reactive oxygen species (ROS) radicals and other superoxo species (superoxide containing complex) with high efficiency, accompanied by strong and immediate CL emission. Surprisingly, the addition of thiourea postponed CL emission in a concentration-dependent manner. The delay was attributed to a slow-generation-scavenging mechanism, which was found to be generally applicable not only to various types of CL reagents and ROS radical scavengers but also to popular chromogenic reactions. The precise regulation of CL kinetics was further utilized in dynamic chemical coding with improved coding density and security. This approach provides a powerful platform for engineering chemical reaction kinetics using chemical timers, which is of application potential in bioassays, biosensors, CL microscopic imaging, microchips, array chips, and informatics.


Subject(s)
Luminescence , Luminol , Hydrogen Peroxide , Luminescent Measurements/methods , Reactive Oxygen Species , Superoxides , Thiourea
4.
Anal Chem ; 96(10): 4048-4056, 2024 Mar 12.
Article in English | MEDLINE | ID: mdl-38373182

ABSTRACT

In this work, we developed an alternative calibration method for measuring N2O5 with an iodide adduct mass spectrometer (I-CIMS). In this calibration method, N2O5 is heated and then quantified based on the decrease in the amount of NO due to its reaction with the pyrolysis product (NO3). This alternative calibration method was compared with the commonly used method utilizing NOx analyzers equipped with a photolytic converter, which gauge NO2 reduction as a result of its reaction with O3 to quantify N2O5. It is notable that the two methodologies demonstrate favorable consistency in terms of calibrating N2O5, with a variance of less than 10 %. The alternative calibration method is a more reliable way to quantify N2O5 with CIMS, considering the instability of the NO2 conversion efficiency of photolytic converters in NOx analyzers and the loss of N2O5 in the sampling line. The effects of O3 and relative humidity (RH) on the sensitivity toward N2O5 were further examined. There was minimal perturbation of N2O5 quantification upon exposure to O3 even at high concentrations. The N2O5 sensitivity exhibited a nonlinear dependence on RH as it initially rose and then fell. Besides I(N2O5)-, the collisional interaction between I(H2O)- and N2O5 also forms I(HNO3)-, which may interfere with the accurate quantification of HNO3. As a consequence of the pronounced dependence on humidity, it is advisable to implement humidity correction procedures when conducting measurements of N2O5.

5.
Opt Express ; 32(1): 179-187, 2024 Jan 01.
Article in English | MEDLINE | ID: mdl-38175047

ABSTRACT

The Tavis-Cummings model is intensively investigated in quantum optics and has important applications in generation of multi-atom entanglement. Here, we employ a superconducting circuit quantum electrodynamic system to study a modified Tavis-Cummings model with directly-coupled atoms. In our device, three superconducting artificial atoms are arranged in a chain with direct coupling through fixed capacitors and strongly coupled to a transmission line resonator. By performing transmission spectrum measurements, we observe different anticrossing structures when one or two qubits are resonantly coupled to the resonator. In the case of the two-qubit Tavis-Cummings model without qubit-qubit interaction, we observe two dips at the resonance point of the anticrossing. The splitting of these dips is determined by Δ λ=2g12+g32, where g1 and g3 are the coupling strengths between Qubit 1 and the resonator, and Qubit 3 and the resonator, respectively. The direct coupling J12 between the two qubits results in three dressed states in the two-qubit Tavis-Cummings model at the frequency resonance point, leading to three dips in the transmission spectrum. In this case, the distance between the two farthest and asymmetrical dips, arising from the energy level splitting, is larger than in the previous case. The frequency interval between these two dips is determined by the difference in eigenvalues (Δ λ=ε 1+-ε 1-), obtained through numerical calculations. What we believe as novel and intriguing experimental results may potentially advance quantum optics experiments, providing valuable insights for future research.

6.
Environ Sci Technol ; 58(2): 1223-1235, 2024 Jan 16.
Article in English | MEDLINE | ID: mdl-38117938

ABSTRACT

Nanoparticle growth influences atmospheric particles' climatic effects, and it is largely driven by low-volatility organic vapors. However, the magnitude and mechanism of organics' contribution to nanoparticle growth in polluted environments remain unclear because current observations and models cannot capture organics across full volatility ranges or track their formation chemistry. Here, we develop a mechanistic model that characterizes the full volatility spectrum of organic vapors and their contributions to nanoparticle growth by coupling advanced organic oxidation modeling and kinetic gas-particle partitioning. The model is applied to Nanjing, a typical polluted city, and it effectively captures the volatility distribution of low-volatility organics (with saturation vapor concentrations <0.3 µg/m3), thus accurately reproducing growth rates (GRs), with a 4.91% normalized mean bias. Simulations indicate that as particles grow from 4 to 40 nm, the relative fractions of GRs attributable to organics increase from 59 to 86%, with the remaining contribution from H2SO4 and its clusters. Aromatics contribute much to condensable organic vapors (∼37%), especially low-volatility vapors (∼61%), thus contributing the most to GRs (32-46%) as 4-40 nm particles grow. Alkanes also contribute 19-35% of GRs, while biogenic volatile organic compounds contribute minimally (<13%). Our model helps assess the climatic impacts of particles and predict future changes.


Subject(s)
Volatile Organic Compounds , Atmosphere/chemistry , Gases , Alkanes , Oxidation-Reduction , Aerosols
7.
J Appl Clin Med Phys ; : e14352, 2024 May 02.
Article in English | MEDLINE | ID: mdl-38696697

ABSTRACT

PURPOSE: To design a patient specific quality assurance (PSQA) process for the CyberKnife Synchrony system and quantify its dosimetric accuracy using a motion platform driven by patient tumor traces with rotation. METHODS: The CyberKnife Synchrony system was evaluated using a motion platform (MODUSQA) and a SRS MapCHECK phantom. The platform was programed to move in the superior-inferior (SI) direction based on tumor traces. The detector array housed by the StereoPhan was placed on the platform. Extra rotational angles in pitch (head down, 4.0° ± 0.15° or 1.2° ± 0.1°) were added to the moving phantom to examine robot capability of angle correction during delivery. A total of 15 Synchrony patients were performed SBRT PSQA on the moving phantom. All the results were benchmarked by the PSQA results based on static phantom. RESULTS: For smaller pitch angles, the mean gamma passing rates were 99.75% ± 0.87%, 98.63% ± 2.05%, and 93.11% ± 5.52%, for 3%/1 mm, 2%/1 mm, and 1%/1 mm, respectively. Large discrepancy in the passing rates was observed for different pitch angles due to limited angle correction by the robot. For larger pitch angles, the corresponding mean passing rates were dropped to 93.00% ± 10.91%, 88.05% ± 14.93%, and 80.38% ± 17.40%. When comparing with the static phantom, no significant statistic difference was observed for smaller pitch angles (p = 0.1 for 3%/1 mm), whereas a larger statistic difference was observed for larger pitch angles (p < 0.02 for all criteria). All the gamma passing rates were improved, if applying shift and rotation correction. CONCLUSIONS: The significance of this work is that it is the first study to benchmark PSQA for the CyberKnife Synchrony system using realistically moving phantoms with rotation. With reasonable delivery time, we found it may be feasible to perform PSQA for Synchrony patients with a realistic breathing pattern.

8.
J Clin Ultrasound ; 2024 May 18.
Article in English | MEDLINE | ID: mdl-38761012

ABSTRACT

PURPOSE: This prospective study assessed the value of ultrasonography (US) in the evaluation of hepatosplenic fungal infections (HSFI). METHODS: Thirty-two pediatric participants with confirmed onco-hematological diseases and HSFI were included. Lesions in the liver and/or spleen were detected by US, magnetic resonance imaging (MRI), or computed tomography (CT). RESULTS: Of the participants, 11 (34%) had confirmed HSFI, while 21 (66%) had highly suspected HSFI. The US, CT, MRI, and fungal blood cultures demonstrated positive results in 31, 19, 25, and 7 patients, respectively. US had a significantly higher detection rate than CT, MRI, and fungal blood cultures (p < 0.05). The "bull's eye" phenomenon was a distinctive US feature of HSFI. Follow-up examinations indicated that after a mean of 7.7 (1-15) months, liver and/or spleen lesions disappeared in five patients. The lesion was significantly smaller in 10 patients. Residual calcifications were detected in 15 patients. Two patients died. CONCLUSION: Conclusively, the US may substitute for tissue biopsy, other imaging modalities, or fungal blood culture for the confirmation of HSFI, and may guide better antifungal treatment, thus achieving better outcomes.

9.
Nano Lett ; 23(8): 3540-3548, 2023 Apr 26.
Article in English | MEDLINE | ID: mdl-37026801

ABSTRACT

Surface plasmon resonance-induced charge separation plays key roles in plasmon-related applications, especially in photocatalysis and photovoltaics. Plasmon coupling nanostructures exhibit extraordinary behaviors in hybrid states, phonon scattering, and ultrafast plasmon dephasing, but plasmon-induced charge separation in these materials remains unknown. Here, we design Schottky-free Au nanoparticle (NP)/NiO/Au nanoparticles-on-a-mirror plasmonic photocatalysts to support plasmon-induced interfacial hole transfer, evidenced by surface photovoltage microscopy at the single-particle level. In particular, we observe a nonlinear increase in charge density and photocatalytic performance with an increase in excitation intensity in plasmonic photocatalysts containing hot spots as a result of varying the geometry. Such charge separation increased the internal quantum efficiency by 14 times at 600 nm in catalytic reactions as compared to that of the Au NP/NiO without a coupling effect. These observations provide an improved understanding of charge transfer management and utilization by geometric engineering and interface electronic structure for plasmonic photocatalysis.

10.
Arch Orthop Trauma Surg ; 144(5): 2101-2108, 2024 May.
Article in English | MEDLINE | ID: mdl-38653838

ABSTRACT

INTRODUCTION: According to reports, the modified extra-articular parapatellar approach allows the performance of tibial nailing in the semi-extended position without the concern of joint violation. However, there remains no special study that has provided a detailed assessment of the benefits and risks of this approach for treating distal tibial fractures (DTFs). The aim of this retrospective study was to investigate the clinical and radiological outcomes of patients with DTFs after intramedullary nailing using a lateral parapatellar extra-articular (LPE) approach in comparison to using the suprapatellar (SP) and transpatellar (TP) approaches. METHODS: Data were collected from 99 patients with a minimum follow-up period of 12 months. Comparisons were conducted between the groups regarding the number of intraoperative fluoroscopies, complications, knee pain, knee range of motion (ROM), the Lysholm Knee Scale (LKS), the Olerud-Molander Ankle Score (OMAS) and radiological findings. RESULTS: The demographic characteristics were comparable between the groups. Fewer intraoperative fluoroscopies were performed in the LPE (27.47 ± 4.98) and SP (26.03 ± 5.12) groups than in the TP group (30.20 ± 7.42; P<0.001). When compared with the other two approaches, the LPE approach was associated with less knee pain (P<0.001) and better knee ROM (P<0.001) at one week postoperative. No significant intergroup differences were detected in the incidence of complications, LKS scores (P = 0.687) and OMAS (P = 0.926). Radiological findings demonstrated that postoperative tibial alignment (P = 0.853), the time of bony union and rate of non-union were similar between the groups. CONCLUSION: The LPE approach can serve as a safe and effective option for tibial nailing, as it offers favourable outcomes in knee pain relief and knee ROM in the early postoperative period and is equivalent to the other two approaches in terms of the incidence of complications, fracture healing, functional recovery and postoperative alignment for patients with DTFs.


Subject(s)
Fracture Fixation, Intramedullary , Tibial Fractures , Humans , Fracture Fixation, Intramedullary/methods , Fracture Fixation, Intramedullary/adverse effects , Tibial Fractures/surgery , Tibial Fractures/diagnostic imaging , Retrospective Studies , Male , Female , Middle Aged , Adult , Range of Motion, Articular , Treatment Outcome , Aged , Radiography , Knee Joint/surgery , Knee Joint/diagnostic imaging , Patella/surgery , Patella/injuries , Patella/diagnostic imaging
11.
Angew Chem Int Ed Engl ; : e202408996, 2024 Jun 14.
Article in English | MEDLINE | ID: mdl-38873975

ABSTRACT

Two-dimensional Ti3C2Tx MXene materials, with metal-like conductivities and versatile terminals, have been considered to be promising surface modification materials for Zn-metal-based aqueous batteries (ZABs). However, the oxygen-rich and hybridized terminations caused by conventional methods limit their advantages in inhibiting zinc dendrite growth and reducing corrosion-related side reactions. Herein, -O-depleted, -Cl-terminated Ti3C2Tx was precisely fabricated by the molten salt electrochemical etching of Ti3AlC2, and controlled in-situ terminal replacement from -Cl to unitary -S or -Se was achieved. The as-prepared -O-depleted and unitary-terminal Ti3C2Tx as Zn anode coatings provided excellent hydrophobicity and enriched zinc-ionophilic sites, facilitating Zn2+ horizontal transport for homogeneous deposition and effectively suppressing water-induced side reactions. The as-assembled Ti3C2Sx@Zn symmetric cell achieved a cycle life of up to 4200 h at a current density and areal capacity of 2 mA cm-2 and 1 mAh cm-2, respectively, with an impressive cumulative capacity of up to 7.25 Ah cm-2 at 5 mA cm-2 // 2 mAh cm-2. These findings provide an effective electrochemical strategy for tailoring -O-depleted and unitary Ti3C2Tx surface terminals and advancing the understanding of the role of specific Ti3C2Tx surface chemistry in regulating the plating/stripping behaviors of metal ions.

12.
Anal Chem ; 95(39): 14762-14769, 2023 Oct 03.
Article in English | MEDLINE | ID: mdl-37729474

ABSTRACT

Chemiluminescence (CL) has emerged as a critical tool for the sensing and quantification of various bioanalytes in virtually all clinical fields. However, the rapid nature of many CL reactions raises challenges for typical low-cost optical sensors such as cameras to achieve accurate and sensitive detection. Meanwhile, classic sensors such as photomultiplier tubes are highly sensitive but lack spatial multiplexing capabilities and are generally not suited for point-of-care applications outside a standard laboratory setting. To address this issue, in this paper, a miniaturized and versatile silicon-photomultiplier-based fiber-integrated CL device (SFCD) was designed for sensitive multiplex CL detection. The SFCD comprises a silicon photomultiplier array coupled to an array of high numerical aperture plastic optical fibers to achieve 16-plex detection. The optical fibers ensure efficient light collection while allowing the fixed detector to be mated with diverse sample geometries (e.g., circular or grid), simply by adjusting the fiber configuration. In a head-to-head comparison with a lens-based camera system featuring a cooled detector, the SFCD achieved a 14-fold improved limit of detection in both direct and enzyme-mediated CL reactions. The SFCD also features improved compactness and lower cost, as well as faster temporal resolution compared with camera-based systems while preserving spatial multiplexing and good environmental robustness. Thus, the SFCD has excellent potential for point-of-care biosensing applications.

13.
Small ; 19(52): e2306351, 2023 Dec.
Article in English | MEDLINE | ID: mdl-37635121

ABSTRACT

Ni-rich layered oxide cathode materials demonstrate high energy densities for Li-ion batteries, but the electrochemically driven thermal runaway and mechanical degradation remain their long-standing challenges in practical applications. Herein, it presents a novel ZrV2 O7  (ZVO) coating with negative thermal expansion properties along the secondary particles and primary particle grain boundaries (GBs), to simultaneously enhance the structural and thermal stability of LiNi0.8 Co0.1 Mn0.1 O2 (NCM811). It unveils that, such an architecture can significantly enhance the electronic conductivity, suppress the microcracks of GBs, alleviate the layered to spinel/rock-salt phase transformation, and meanwhile relieve the lattice oxygen loss by increasing the oxygen vacancy formation energy increased (1.43 vs 1.90 eV). Consequently, the ZVO-coated NCM811 material demonstrates a remarkable cyclability with 86.5% capacity retention after 100 cycles, and an outstanding rate performance of 30 C under a high-voltage of 4.6 V, outperforming the state-of-the-art literature. More importantly, the Li+ transportation can be readily blocked at 120 °C by the negative-thermal-expansion ZVO coating, thus avoiding the high-temperature thermal runaway.

14.
Phys Rev Lett ; 131(10): 103602, 2023 Sep 08.
Article in English | MEDLINE | ID: mdl-37739354

ABSTRACT

Optical mirrors determine cavity properties by means of light reflection. Imperfect reflection gives rise to open cavities with photon loss. We study an open cavity made of atom-dimer mirrors with a tunable reflection spectrum. We find that the atomic cavity shows anti-PT symmetry. The anti-PT phase transition controlled by atomic couplings in mirrors indicates the emergence of two degenerate cavity supermodes. Interestingly, a threshold of mirror reflection is identified for realizing strong coherent cavity-atom coupling. This reflection threshold reveals the criterion of atomic mirrors to produce a good cavity. Moreover, cavity quantum electrodynamics with a probe atom shows mirror-tuned properties, including reflection-dependent polaritons formed by the cavity and probe atom. Our Letter presents a non-Hermitian theory of an anti-PT atomic cavity, which may have applications in quantum optics and quantum computation.

15.
FASEB J ; 36(8): e22465, 2022 08.
Article in English | MEDLINE | ID: mdl-35867072

ABSTRACT

Anlotinib has been demonstrated to be effective in advanced non-small cell lung cancer (NSCLC) patients. The response stratification of anlotinib remains unclear. In this study, plasma samples from 28 anlotinib-treated NSCLC patients (discovery cohort: 14 responders and 14 non-responders) were subjected to proteomic analysis, and plasma samples from 35 anlotinib-treated NSCLC patients (validation cohort) were subjected to validation analysis. Liquid chromatography-tandem mass spectrometry analysis was performed on samples with different time points, namely baseline (BL), best response (BR), and progression disease (PD). Bioinformatics analysis was performed to screen for the underlying differential proteins. Enzyme-linked immunosorbent assay was performed to detect plasma ARHGDIB, FN1, CDH1, and KNG1 levels respectively. The Kaplan-Meier survival analysis was used for biomarker-based responsive stratification. Our results indicated that differential proteins between responders and non-responders showed that proteomic technology potentially contributes to biomarker screening in plasma samples at BL. Furthermore, our results suggested that the detection of plasma ARHGDIB, FN1, CDH1, and KNG1 levels have potential predictive value for anlotinib response both in the discovery cohort and validation cohort. Collectively, this study offers novel insights into the value of plasma biomarker screening via proteomic examination and suggests that plasma ARHGDIB, FN1, CDH1, and KNG1 levels could be used as biomarkers for anlotinib stratification in NSCLC patients.


Subject(s)
Carcinoma, Non-Small-Cell Lung , Lung Neoplasms , Quinolines , Biomarkers , Carcinoma, Non-Small-Cell Lung/drug therapy , Early Detection of Cancer , Humans , Indoles , Lung Neoplasms/drug therapy , Proteomics , Quinolines/therapeutic use , rho Guanine Nucleotide Dissociation Inhibitor beta
16.
Environ Sci Technol ; 57(21): 8075-8084, 2023 05 30.
Article in English | MEDLINE | ID: mdl-37184340

ABSTRACT

The effects of nitrogen deposition reduction on nutrient loading in freshwaters have been widely studied, especially in remote regions. However, understanding of the ecological effects is still rather limited. Herein, we re-estimated nitrogen deposition, both of wet and dry deposition, in Lake Taihu with monthly monitoring data from 2010 to 2021. Our results showed that the atmospheric deposition of reactive nitrogen (namely NH4+ and NO3-) in Lake Taihu was 4.94-11.49 kton/yr, which equaled 13.9%-27.3% of the riverine loading. Dry deposition of NH4+ and NO3- contributed 53.1% of the bulk deposition in Lake Taihu. Ammonium was the main component of both wet and dry deposition, which may have been due to the strong agriculture-related activities around Lake Taihu. Nitrogen deposition explained 24.9% of the variation in phytoplankton community succession from 2010 to 2021 and was the highest among all the environmental factors. Atmospheric deposition offset the effects of external nitrogen reduction during the early years and delayed the emergence of nitrogen-fixing cyanobacterial dominance in Lake Taihu. Our results implied that a decrease in nitrogen deposition due to a reduction in fertilizer use, especially a decrease in NH4+ deposition, could limit diatoms and promote non-nitrogen-fixing cyanobacterial dominance, followed by nitrogen-fixing taxa. This result was also applied to other shallow eutrophic lakes around the middle and lower reaches of the Yangtze River, where significant reduction of fertilizer use recorded during the last decades.


Subject(s)
Cyanobacteria , Phytoplankton , Lakes , Nitrogen , Fertilizers , Eutrophication
17.
Environ Sci Technol ; 57(16): 6609-6615, 2023 04 25.
Article in English | MEDLINE | ID: mdl-37040454

ABSTRACT

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.


Subject(s)
Air Pollutants , Ozone , Sulfur Dioxide , Sulfates , Sulfur Oxides , Atmosphere , Water , Aerosols , Osmolar Concentration
18.
Environ Sci Technol ; 57(1): 64-75, 2023 01 10.
Article in English | MEDLINE | ID: mdl-36516990

ABSTRACT

Oxidation of volatile organic compounds (VOCs) forms oxygenated organic molecules (OOMs), which contribute to secondary pollution. Herein, we present measurement results of OOMs using chemical ionization mass spectrometry with nitrate as the reagent ion in Shanghai. Compared to those in forests and laboratory studies, OOMs detected at this urban site were of relatively lower degree of oxygenation. This was attributed to the high NOx concentrations (∼44 ppb), which overall showed a suppression on the propagation reactions. As another result, a large fraction of nitrogenous OOMs (75%) was observed, and this fraction further increased to 84% under a high NO/VOC ratio. By applying a novel framework on OOM categorization and supported by VOC measurements, 50 and 32% OOMs were attributed to aromatic and aliphatic precursors, respectively. Furthermore, aromatic OOMs are more oxygenated (effective oxygen number, nOeff = 4-6) than aliphatic ones (nOeff = 3-4), which can be partly explained by the difference in initiation mechanisms and points to possible discrimination in termination reactions. This study highlights the roles of NOx in OOM formation in urban areas, as well as the formation of nitrogenous products that might show discrimination between aromatic and aliphatic VOCs.


Subject(s)
Air Pollutants , Ozone , Volatile Organic Compounds , Air Pollutants/analysis , Volatile Organic Compounds/analysis , China , Ozone/analysis , Environmental Monitoring , Nitrogen/analysis
19.
Environ Sci Technol ; 57(20): 7764-7776, 2023 05 23.
Article in English | MEDLINE | ID: mdl-37155674

ABSTRACT

Oxygenated organic molecules (OOMs) are critical intermediates linking volatile organic compound oxidation and secondary organic aerosol (SOA) formation. Yet, the understanding of OOM components, formation mechanism, and impacts are still limited, especially for urbanized regions with a cocktail of anthropogenic emissions. Herein, ambient measurements of OOMs were conducted at a regional background site in South China in 2018. The molecular characteristics of OOMs revealed dominant nitrogen-containing products, and the influences of different factors on OOM composition and oxidation state were elucidated. Positive matrix factorization analysis resolved the complex OOM species to factors featured with fingerprint species from different oxidation pathways. A new method was developed to identify the key functional groups of OOMs, which successfully classified the majority species into carbonyls (8%), hydroperoxides (7%), nitrates (17%), peroxyl nitrates (10%), dinitrates (13%), aromatic ring-retaining species (6%), and terpenes (7%). The volatility estimation of OOMs was improved based on their identified functional groups and was used to simulate the aerosol growth process contributed by the condensation of those low-volatile OOMs. The results demonstrate the predominant role of OOMs in contributing sub-100 nm particle growth and SOA formation and highlight the importance of dinitrates and anthropogenic products from multistep oxidation.


Subject(s)
Air Pollutants , Air Pollutants/analysis , Hong Kong , Nitrates , Terpenes , Aerosols/analysis
20.
Article in English | MEDLINE | ID: mdl-37310424

ABSTRACT

Suicidal ideation (SI) is common among people with schizophrenia. However, it has received less attention than suicide attempts (SA), especially in the Chinese population. Alexithymia is a well-established risk factor for SI across different populations. Nevertheless, very few studies evaluated their relationship in schizophrenia patients. We aimed to determine the prevalence and clinical correlates of SI and its relationship with alexithymia in 812 Chinese chronic schizophrenia inpatients. We assessed SI, clinical symptoms, and alexithymia by the Beck Scale for Suicidal Ideation, the Positive and Negative Syndrome Scale (PANSS), and the Toronto Alexithymia Scale, respectively. A multiple logistic regression model was conducted to identify independent correlates of SI. Receiver operating characteristic (ROC) curves and area under the curve (AUC) were performed to determine the ability of our model to distinguish between patients with and without SI. 10% (n = 84) reported current SI. Lifetime SA (OR, 4.68; 95% CI 2.76-7.94, p < 0.001), PANSS depressive factor (OR, 1.24; 95% CI 1.12-1.38, p < 0.001), PANSS positive subscale (OR, 1.055; 95% CI 1.004-1.108, p = 0.035), and difficulty identifying emotions (OR, 1.07; 95% CI 1.03-1.12, p = 0.002) were associated with SI. The AUC value was 0.80, indicating excellent distinguishing capabilities. Timely assessments of these factors may help identify schizophrenia patients who are at risk for SI.

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