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1.
J Am Chem Soc ; 146(37): 25870-25877, 2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39231938

ABSTRACT

The selective oxidation of methane (CH4) features attractive potentials in both mitigating global warming and producing value-added chemicals. However, due to the short-life and unpaired concentrations of reactive intermediates (such as ·OH, ·CH3, and CO), the selective formation of multicarbon products like ethanol has remained challenging. In this work, we developed a hollow multishelled CeO2@PdO@FeOx nanosphere catalyst with two asymmetric and closely connected interfaces, featuring efficient in-tandem photo-oxidation of CH4 into ethanol with O2 as the oxidant. The outer FeOx surface promotes the photoreduction of the oxazole atoms in O2. In the meantime, the two asymmetric PdO/FeOx and CeO2/PdO catalytic interfaces enable selective photoactivation of CH4 to ·CH3 and then to CO, respectively, and the hollow multishelled structure further facilitates the directional transport and coupling of the as-generated ·CH3 and CO to produce ethanol. Under 100 mW·cm-2 light intensity and ambient conditions, the hollow multishelled CeO2@PdO@FeOx nanosphere photocatalyst exhibited a peak CH4-to-ethanol yield of 728 µmol·g-1·h-1 without photosensitizers or sacrificial agents, almost three times higher than the previous best reports on photocatalytic CH4 oxidation to ethanol, suggesting the attractive potential of the asymmetric multishelled catalytic interfaces.

2.
ChemSusChem ; : e202400683, 2024 May 20.
Article in English | MEDLINE | ID: mdl-38769898

ABSTRACT

The efficient acetate conversion from CO electroreduction is challenging due to the poor selectivity at high reaction rate, which requires the competition with H2 and other C2+ (i. e., ethylene, ethanol, n-propanol) reduction products. Electrolyte engineering is one of the efficient strategies to regulate the reaction microenvironment. In this work, the adding of sulfite (SO3 2-) with high nucleophilicity in KOH electrolytes was demonstrated to enable improving the CO-to-acetate conversion via generating a S-O chemical bond between SO3 2- and oxygenated *C2 intermediates (i. e., *CO-CO, *CO-COH) compared with that in pure KOH system on both synthesized Cu(200)- and normal commercial Cu(111)-facets-exposed metallic Cu catalysts. As a result, the prepared Cu(200)-facets-exposed metallic Cu catalyst with surface ions modification showed an superior Faradaic efficiency of 63.6 % at -0.6 A ⋅ cm-2, and extraordinary absolute value of peak partial current density as high as 1.52 A ⋅ cm-2 with adding SO3 2- in KOH electrolytes, compared to the best reported values in both CO and CO2 electroreduction. Our work suggests an attractive strategy to introduce the oxyanion with high nucleophilicity in electrolytes to regulate the microenvironment for industrial-current-density electrosynthesis of acetate from CO electroreduction.

3.
Front Pharmacol ; 13: 986199, 2022.
Article in English | MEDLINE | ID: mdl-36408259

ABSTRACT

Objective: T cells represent a predominant cell type in autoimmune disease. However, their exact roles are not fully clear in systemic sclerosis (SSc). This study aimed to mainly investigate the alteration in the absolute numbers of T-lymphocyte subsets and the serum levels of cytokines in SSc patients. Methods: A total of 76 patients with SSc and 76 age- and sex-matched healthy controls (HCs) were enrolled. The levels of circulating T cell subsets and serum cytokines were measured by flow cytometry. T cell subsets or serum cytokines correlations with disease activity and organ involvement were analyzed. Results: The absolute numbers of Th2 and Treg cells in SSc patients were lower than those in HCs (p < 0.05), resulting in the ratios of Th1/Th2 [25.01 (12.24, 38.61) vs. 11.64 (6.38, 20.34)] and Th17/Treg [0.42 (0.17, 0.66) vs. 0.17 (0.13, 0.29)] were increased significantly (p < 0.001). The absolute numbers of total T, Th, and Treg cells were negatively correlated with CRP (r = -0.406, p = 0.002; r = -0.263, p < 0.05; r = -0.367 p < 0.01). The serum levels of IL-2, SIL-2R, IL-6, IL-10, INF-γ, and TNF-α were significantly higher than those in HCs (p < 0.001). Increasing IL-2 in the wake of the augment of ESR (r = 0.671, p = 0.004), so did IL-6 (r = 0.378, p < 0.05). The ratio of Th17/Treg in SSc-ILD patients had lower levels than that in other patients [0.35 (0.14, 0.53) vs. 0.64 (0.26, 0.93) p = 0.028]; Treg cells were lessened in patients with Raynaud's phenomenon relative to controls [3.00 (2.41, 4.28) vs. 3.55 (2.86, 4.53) p < 0.05]. The levels of IL-2, IL-10 and INF-γ [3.32 (1.05,11.73) vs. 2.32 (0.44,6.45), p = 0.045], [8.08 (3.63, 355,77) vs. 4.89 (0.78, 21.44), p = 0.02], [6.31 (2.66, 44.03) vs. 4.03 (0.22, 16.96), p = 0.009] were elevated in patients with arthralgia, while the level of Th17 was decreased [0.62 (0.20,2.16) vs. 1.26 (0.22,10.93), p = 0.026]. ROC curve analysis yielded an optimal cut-off IL-2, IL-10, and INF-γ levels of 2.67, 5.93, and 5.32 pg/ml for the presence of arthralgia. Conclusion: We exhibited abnormalities in T subsets and the production of their cytokines in SSc, as compared with those in HCs. This may allow the pathogenesis of SSc and the development of novel therapeutic interventions aimed at targeting these cells and the cytokines they produce.

4.
Rev Environ Health ; 37(2): 267-279, 2022 Jun 27.
Article in English | MEDLINE | ID: mdl-34049423

ABSTRACT

Previous studies have confirmed that poor living conditions can lead to a wide range of health problems. However, in the context of the COVID-19 pandemic, vulnerable groups in unstable housing are more susceptible to disease. This study aims to systematically examine the housing and health problems of vulnerable groups using a bibliometric approach to explore how housing causes health problems, types of health illnesses, and coping strategies. It is found that the poor housing mechanism, persistent inequalities, and poor housing environments have a significant impact on the health of vulnerable groups. Therefore, the government must make concerted efforts across all sectors to ensure that the housing and health care needs of vulnerable groups are improved, and that housing security standards and related policies are improved; targeted safety plans are formulated with community as the carrier, taking into account the characteristics of vulnerable groups; and new information technology is widely used to provide medical convenience for vulnerable groups. It is hoped that the research in this paper can arouse social attention to the health of vulnerable groups and improve their health from the perspective of housing, so as to point out the direction for solving the housing health problems of vulnerable groups in the future.


Subject(s)
COVID-19 , Housing , Bibliometrics , COVID-19/epidemiology , Humans , Pandemics
5.
Front Psychol ; 12: 795142, 2021.
Article in English | MEDLINE | ID: mdl-35095680

ABSTRACT

The continuous increase of carbon emissions is a serious challenge all over the world, and many countries are striving to solve this problem. Since 2020, a widespread lockdown in the country to prevent the spread of COVID-19 escalated, severely restricting the movement of people and unnecessary economic activities, which unexpectedly reduced carbon emissions. This paper aims to analyze the carbon emissions data of 30 provinces in the 2020 and provide references for reducing emissions with epidemic lockdown measures. Based on the method of time series visualization, we transform the time series data into complex networks to find out the hidden information in these data. We found that the lockdown would bring about a short-term decrease in carbon emissions, and most provinces have a short time point of impact, which is closely related to the level of economic development and industrial structure. The current results provide some insights into the evolution of carbon emissions under COVID-19 blockade measures and valuable insights into energy conservation and response to the energy crisis in the post-epidemic era.

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