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1.
Proc Natl Acad Sci U S A ; 121(19): e2318652121, 2024 May 07.
Article in English | MEDLINE | ID: mdl-38687781

ABSTRACT

Water oxidation on magnetic catalysts has generated significant interest due to the spin-polarization effect. Recent studies have revealed that the disappearance of magnetic domain wall upon magnetization is responsible for the observed oxygen evolution reaction (OER) enhancement. However, an atomic picture of the reaction pathway remains unclear, i.e., which reaction pathway benefits most from spin-polarization, the adsorbent evolution mechanism, the intermolecular mechanism (I2M), the lattice oxygen-mediated one, or more? Here, using three model catalysts with distinguished atomic chemistries of active sites, we are able to reveal the atomic-level mechanism. We found that spin-polarized OER mainly occurs at interconnected active sites, which favors direct coupling of neighboring ligand oxygens (I2M). Furthermore, our study reveals the crucial role of lattice oxygen participation in spin-polarized OER, significantly facilitating the coupling kinetics of neighboring oxygen radicals at active sites.

2.
Chem Soc Rev ; 53(16): 8123-8136, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39005214

ABSTRACT

Understanding the electronic structure of active sites is crucial in efficient catalyst design. The spin state, spin configurations of d-electrons, has been frequently discussed recently. However, its systematic depiction in electrocatalysis is lacking. In this tutorial review, a comprehensive interpretation of the spin state of metal centers in electrocatalysts and its role in electrocatalysis is provided. This review starts with the basics of spin states, including molecular field theory, crystal field theory, and ligand field theory. It further introduces the differences in low spin, intermediate spin, and high spin, and intrinsic factors affecting the spin state. Popular characterization techniques and modeling approaches that can reveal the spin state, such as X-ray absorption microscopy, electron spin resonance spectroscopy, Mössbauer spectroscopy, and density functional theory (DFT) calculations, are introduced as well with examples from the literature. The examples include the most recent progress in tuning the spin state of metal centers for various reactions, e.g., the oxygen evolution reaction, oxygen reduction reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, nitrogen reduction reaction, nitrate reduction reaction, and urea oxidation reaction. Challenges and potential implications for future research related to the spin state are discussed at the end.

3.
Small ; 20(8): e2305765, 2024 Feb.
Article in English | MEDLINE | ID: mdl-37821399

ABSTRACT

Solid proton electrolytes play a crucial role in various electrochemical energy storage and conversion devices. However, the development of fast proton conducting solid proton electrolytes at ambient conditions remains a significant challenge. In this study, a novel acidified nitrogen self-doped porous carbon material is presented that demonstrates exceptional superprotonic conduction for applications in solid-state proton battery. The material, designated as MSA@ZIF-8-C, is synthesized through the acidification of nitrogen-doped porous carbon, specifically by integrating methanesulfonic acid (MSA) into zeolitic imidazolate framework-derived nitrogen self-doped porous carbons (ZIF-8-C). This study reveals that MSA@ZIF-8-C achieves a record-high proton conductivity beyond 10-2  S cm-1 at ambient condition, along with good long-term stability, positioning it as a cutting-edge alternative solid proton electrolyte to the default aqueous H2 SO4 electrolyte in proton batteries.

4.
Mol Psychiatry ; 28(3): 1027-1045, 2023 03.
Article in English | MEDLINE | ID: mdl-33990773

ABSTRACT

Dopamine (DA) neurons in the ventral tegmental area (VTA) are critical to coping with stress. However, molecular mechanisms regulating their activity and stress-induced depression were not well understood. We found that the receptor tyrosine kinase ErbB4 in VTA was activated in stress-susceptible mice. Deleting ErbB4 in VTA or in DA neurons, or chemical genetic inhibition of ErbB4 kinase activity in VTA suppressed the development of chronic social defeat stress (CSDS)-induced depression-like behaviors. ErbB4 activation required the expression of NRG1 in the laterodorsal tegmentum (LDTg); LDTg-specific deletion of NRG1 inhibited depression-like behaviors. NRG1 and ErbB4 suppressed potassium currents of VTA DA neurons and increased their firing activity. Finally, we showed that acute inhibition of ErbB4 after stress attenuated DA neuron hyperactivity and expression of depression-like behaviors. Together, these observations demonstrate a critical role of NRG1-ErbB4 signaling in regulating depression-like behaviors and identify an unexpected mechanism by which the LDTg-VTA circuit regulates the activity of DA neurons.


Subject(s)
Depression , Ventral Tegmental Area , Mice , Animals , Ventral Tegmental Area/metabolism , Dopaminergic Neurons/metabolism , Signal Transduction , Phosphorylation , Receptor, ErbB-4/genetics , Receptor, ErbB-4/metabolism
5.
Br J Nutr ; 131(5): 821-828, 2024 03 14.
Article in English | MEDLINE | ID: mdl-37839856

ABSTRACT

The association between sarcopenia and kidney function remains poorly investigated. We aimed to evaluate the associations between sarcopenia status and kidney function (rapid kidney function decline and chronic kidney disease (CKD)) in middle-aged and older Chinese population. A total of 9375 participants from the China Health and Retirement Longitudinal Study 2011 were included in the cross-sectional analyses. A total of 5864 participants with eGFRcr-cys ≥ 60 ml/min per 1·73 m2 at baseline were included in the longitudinal analyses and were followed up in 2015. Sarcopenia status was defined according to the Asian Working Group for Sarcopenia 2019 criteria. In the cross-sectional analyses, possible sarcopenia and sarcopenia were significantly associated with an increased risk of CKD. During the 4 years of follow-up, 359 (6·12 %) participants experienced rapid decline in kidney function and 126 (2·15 %) participants developed CKD. After multivariable adjustment of baseline eGFRcr-cys level and other risk factors, possible sarcopenia (OR, 1·33; 95 % CI 1·01, 2·12) and sarcopenia (OR, 1·49; 95 % CI 1·05, 2·12) were associated with an increased risk of primary outcome (composite of rapid decline in kidney function (annualised decline in eGFRcr-cys ≥ 5 ml/min per 1·73 m2) and progression to CKD (eGFRcr-cys < 60 ml/min per 1·73 m2). Individuals with low muscle mass or low muscle strength alone also had an increased risk of rapid decline in kidney function and progression to CKD.


Subject(s)
Renal Insufficiency, Chronic , Sarcopenia , Adult , Middle Aged , Humans , Aged , Sarcopenia/epidemiology , Glomerular Filtration Rate/physiology , Longitudinal Studies , Cross-Sectional Studies , Renal Insufficiency, Chronic/epidemiology , Kidney
6.
Inorg Chem ; 63(5): 2640-2646, 2024 Feb 05.
Article in English | MEDLINE | ID: mdl-38252082

ABSTRACT

Organic-inorganic silver halide hybrids show abundant phase transitions and thermochromism. However, it is very rare that silver halides exhibit thermochromism related to thermotropic structure phase transition. Herein, a bromoargentate hybrid, [Pr-dabco]2Ag4Br6 (1) (Pr-dabco+ = 1-propyl-1,4-diazabicyclo-[2.2.2]octan-1-ium), with tetranuclear [Ag4Br6]2- clusters was prepared and characterized by microanalysis, ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy, and thermogravimetric (TG) and differential scanning calorimetry (DSC) techniques. Interestingly, 1 undergoes an irreversible structure phase transition at ∼436 K in the first heating process, which is accompanied by an abrupt color change from colorless to yellow; however, a reversible color change between pale yellow and yellow is observed in the next heating-cooling cycles. Notably, DSC measurement revealed that a reversible phase transition is associated with the change in color between pale yellow and yellow, while the powder X-ray diffraction (PXRD) patterns corresponding to pale yellow and yellow phases are quite similar to each other. These observations demonstrate that thermochromism in the next heating-cooling runs is associated with a reversible structure phase transition, which perhaps concerns the disorder-order transformation of alkyl chains in the cationic ligand [Pr-dabco]+, and relevant to the anharmonic fluctuations of the Ag-Br and Ag-N bonds, a strong electron-phonon coupling effect is seen within the bromoargentate cluster.

7.
Inorg Chem ; 2024 Aug 23.
Article in English | MEDLINE | ID: mdl-39178213

ABSTRACT

Ammonium dinitramide (ADN), as a novel and environmentally friendly oxidizer, has strong hygroscopicity when exposed to high-humidity air, which seriously hinders its application in solid propellants. Modification of oxidizers by cocrystallization is an effective strategy to improve the hygroscopicity of energetic components. In this paper, the theoretical simulation of ADN/CL-20 cocrystals was developed via a directional hydrogen bonding design to establish a cocrystal with improved hygroscopicity. Intermolecular interaction analyses reveal that hydrogen bonds and van der Waals interactions synergistically lead to the formation of cocrystals. The ADN/CL-20 cocrystal was prepared experimentally by the spray drying self-assembly technique, and the corresponding thermal analysis and sensitivity properties were conducted to illustrate the thermal stability and high safety. Furthermore, the critical relative humidity (CRH) measurement was carried out to evaluate the hygroscopicity of the cocrystal, exhibiting a certain degree of antihygroscopic effect with a CRH of 65%. The hydrogen bonds formed between ADN and CL-20 saturate the ammonium ions of ADN, further preventing ADN from absorbing water molecules in the air. The ADN/CL-20 cocrystal has high specific impulse characteristics (Isp: 272.6 s). Accordingly, this work clearly demonstrates that the ADN/CL-20 cocrystal is expected to be used in a solid propellant to make up for the deficiency of the ADN oxidizer.

8.
Org Biomol Chem ; 22(30): 6085-6089, 2024 Jul 31.
Article in English | MEDLINE | ID: mdl-39005048

ABSTRACT

An enantioselective copper-catalyzed 1,2-arylboration reaction of enamines has been developed by employing (R)-xyl-BINAP as a chiral ligand. A number of chiral borate-containing 3,3'-disubstituted isoindolinones were obtained in moderate to good yields and good to excellent enantioselectivities from the reactions of N-(o-iodobenzoyl)enamines and bis(pinacolato)diboron (B2pin2) under mild reaction conditions. Synthetic transformations of the products were conducted to demonstrate the practicality of this reaction.

9.
J Chem Inf Model ; 64(2): 359-377, 2024 01 22.
Article in English | MEDLINE | ID: mdl-38164000

ABSTRACT

p-Sulfonatocalix[n]arenes (SCnA) have demonstrated great potential for drug encapsulation through host-guest complexation to improve solubility, stability, and bioavailability. In this study, the solubilization effect of SCnA (n = 4, 6, 8) on 95 active compounds derived from traditional Chinese medicine (TCM) was investigated. Based on the significant solubilization effect on alkaloids, SC6A/SC8A and 76 alkaloids were selected as the host and guest, respectively, to determine the binding constant by competitive fluorescence titration. LASSO regression was adopted to investigate the mechanism of the complex of SCnA with alkaloids. The binding constant of alkaloids-SC6A and alkaloids-SC8A was related to the alkaloid alkalinity. Also, the electronegativity, polarization, first ionization potential, hydrogen bond potential, the molecular size, and shape of alkaloids are critical properties to determine alkaloids-SC6A binding constant as well as electronegativity, polarization, hydrophobicity, and the molecular size and shape of alkaloids play an important role for the alkaloids-SC8A binding constant.


Subject(s)
Alkaloids , Medicine, Chinese Traditional , Alkaloids/chemistry
10.
Nutr Metab Cardiovasc Dis ; 34(10): 2257-2265, 2024 Oct.
Article in English | MEDLINE | ID: mdl-38866620

ABSTRACT

BACKGROUND AND AIM: Cardiovascular diseases (CVD) is a major threat to public health, while cardiorespiratory fitness (CRF) is a key predictor of chronic disease. Given this, the purpose of this study was to investigate the relationship between estimated CRF (eCRF) and CVD in middle-aged and elderly Chinese people. METHODS AND RESULTS: The China Health and Retirement Longitudinal Study (CHARLS) with 4761 individuals were included in analysis. Participants were divided into three groups according to eCRF quantile in sex subgroups. Cox proportional hazards regression models were used to explore the correlation of eCRF with CVD (stroke or cardiac events). In total, 4761 participants were included in this cohort study (2500 [52.51%] women). During a 7-year follow-up from 2011 to 2018, 796 CVDs (268 Strokes and 588 cardiac events) were recorded. In multivariable-adjusted analyses, for per 1 SD increase of eCRF, the age-adjusted risk of CVD was reduced by about 18% (HR = 0.82; 95% CI, 0.72-0.93) in men, and was reduced by about 29% (HR = 0.71; 95% CI, 0.62-0.81) in women. Similar associations were also found between eCRF and stroke and cardiac events. Both subgroup and interaction analyses showed that the interaction of age had a statistically significant effect on CVD risk. CONCLUSION: ECRF was inversely associated with CVD risk (stroke or cardiac events) in both men and women. Remarkable sex and age differences exist in the effectiveness of increasing eCRF to reduce the risk of CVD. As a potential, efficient and cost-effective risk prediction tool, eCRF deserves further attention and wide application.


Subject(s)
Cardiorespiratory Fitness , Cardiovascular Diseases , Humans , Female , Male , Middle Aged , China/epidemiology , Longitudinal Studies , Aged , Cardiovascular Diseases/epidemiology , Cardiovascular Diseases/diagnosis , Cardiovascular Diseases/physiopathology , Cardiovascular Diseases/prevention & control , Risk Assessment , Age Factors , Time Factors , Sex Factors , Risk Factors , Prognosis , Protective Factors
11.
BMC Psychiatry ; 24(1): 513, 2024 Jul 18.
Article in English | MEDLINE | ID: mdl-39026187

ABSTRACT

OBJECTIVES: This study examined the relationship of social isolation and loneliness on sarcopenia among Chinese middle-aged and elderly people. METHODS: Social isolation, loneliness, and sarcopenia were measured at baseline. Follow-up measures of new-onset sarcopenia were obtained 4 years later. Then used logistic regression to evaluate the association between social isolation, loneliness and sarcopenia. RESULTS: In cross-sectional analysis, social isolation and loneliness are significantly associated with sarcopenia [OR = 1.88 (95% CI = 1.54-2.28)]. In longitudinal analysis, social isolation and loneliness are significantly associated with sarcopenia [OR = 1.09 (95% CI = 0.71-1.69)]. Social isolation and loneliness have a synergistic effect. Among them, individuals over 60 years old [OR = 2.01 (95% CI = 1.37-2.96)] and those without social support [OR = 2.64 (1.61-4.32), P-for interaction < 0.001] are at higher risk. CONCLUSION: Social isolation and loneliness were significantly associated with sarcopenia, and there was a synergistic effect between social isolation and loneliness.


Subject(s)
Loneliness , Sarcopenia , Social Isolation , Humans , Loneliness/psychology , Social Isolation/psychology , Sarcopenia/psychology , Male , Female , China/epidemiology , Aged , Cross-Sectional Studies , Middle Aged , Longitudinal Studies , Social Support
12.
BMC Geriatr ; 24(1): 225, 2024 Mar 04.
Article in English | MEDLINE | ID: mdl-38439007

ABSTRACT

OBJECTIVE: The aim of present study was to evaluate the combined effect of hypertension and activities of daily living (ADL)/instrumental activities of daily living (IADL) with the risk of CVD, stroke and cardiac events. METHODS: A total of 14,083 participants aged 45 years or older from the China Health and Retirement longitudinal study were included in current study. Participants were divided into 4 groups according to hypertension and ADL/IADL status. Cox proportional hazards regression model was used to explore the associations between hypertension, ADL/IADL and new-onset CVD, stroke and cardiac events. RESULTS: During the 7-year follow-up, a total of 2,324 respondents experienced CVD (including 783 stroke and 1,740 cardiac events). Individuals with limitations in ADL alone, or with hypertension alone, or with both limitations in ADL and hypertension were associated with increased risk of CVD, with the adjusted hazard ratios (95% confidence intervals) were 1.17(1.00-1.35), 1.36(1.24-1.49) and 1.44(1.23-1.68), respectively. Those with limitations in ADL and hypertension also had higher risk of stroke (hazard ratios = 1.64; 1.26-2.14) and cardiac events (hazard ratios = 1.37; 1.14-1.64). Similarly, individuals with both limitations in IADL and hypertension were associated with increased risk of CVD (hazard ratios = 1.34; 1.15-1.57), stroke (hazard ratios = 1.50; 1.17-1.95) and cardiac events (hazard ratios = 1.27; 1.06-1.53). CONCLUSION: Hypertension and limitations in ADL/IADL jointly increased the risk of CVD, stroke and cardiac events.


Subject(s)
Cardiovascular Diseases , Hypertension , Stroke , Humans , Cardiovascular Diseases/diagnosis , Cardiovascular Diseases/epidemiology , Activities of Daily Living , Longitudinal Studies , Hypertension/diagnosis , Hypertension/epidemiology , Stroke/diagnosis , Stroke/epidemiology
13.
Proc Natl Acad Sci U S A ; 118(16)2021 04 20.
Article in English | MEDLINE | ID: mdl-33850017

ABSTRACT

Epilepsy, a common neurological disorder, is featured with recurrent seizures. Its underlying pathological mechanisms remain elusive. Here, we provide evidence for loss of neogenin (NEO1), a coreceptor for multiple ligands, including netrins and bone morphological proteins, in the development of epilepsy. NEO1 is reduced in hippocampi from patients with epilepsy based on transcriptome and proteomic analyses. Neo1 knocking out (KO) in mouse brains displays elevated epileptiform spikes and seizure susceptibility. These phenotypes were undetectable in mice, with selectively depleted NEO1 in excitatory (NeuroD6-Cre+) or inhibitory (parvalbumin+) neurons, but present in mice with specific hippocampal astrocytic Neo1 KO. Additionally, neurons in hippocampal dentate gyrus, a vulnerable region in epilepsy, in mice with astrocyte-specific Neo1 KO show reductions in inhibitory synaptic vesicles and the frequency of miniature inhibitory postsynaptic current(mIPSC), but increase of the duration of miniature excitatory postsynaptic current and tonic NMDA receptor currents, suggesting impairments in both GABAergic transmission and extracellular glutamate clearance. Further proteomic and cell biological analyses of cell-surface proteins identified GLAST, a glutamate-aspartate transporter that is marked reduced in Neo1 KO astrocytes and the hippocampus. NEO1 interacts with GLAST and promotes GLAST surface distribution in astrocytes. Expressing NEO1 or GLAST in Neo1 KO astrocytes in the hippocampus abolishes the epileptic phenotype. Taken together, these results uncover an unrecognized pathway of NEO1-GLAST in hippocampal GFAP+ astrocytes, which is critical for GLAST surface distribution and function, and GABAergic transmission, unveiling NEO1 as a valuable therapeutic target to protect the brain from epilepsy.


Subject(s)
Astrocytes/metabolism , Hippocampus/metabolism , Membrane Proteins/metabolism , Animals , Astrocytes/physiology , Biological Transport/physiology , Epilepsy/physiopathology , Epilepsy/prevention & control , Excitatory Amino Acid Transporter 1/metabolism , Excitatory Amino Acid Transporter 2/metabolism , Female , Glutamic Acid/metabolism , Male , Membrane Proteins/physiology , Mice , Mice, Inbred C57BL , Mice, Knockout , Neurons/metabolism , Seizures/metabolism , Signal Transduction , Synaptic Potentials/physiology
14.
Chem Biodivers ; 21(6): e202400408, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38441384

ABSTRACT

To develop novel bacterial biofilm inhibiting agents, a series of 1,3,4-thiadiazole derivatives containing sulfonylpiperazine structures were designed, synthesized, and characterized using 1H nuclear magnetic resonance (1H NMR), 13C nuclear magnetic resonance (13C NMR), and high-resolution mass spectrometry. Meanwhile, their biological activities were evaluated, and the ensuing structure-activity relationships were discussed. The bioassay results showed the substantial antimicrobial efficacy exhibited by most of the compounds. Among them, compound A24 demonstrated a strong efficacy with an EC50 value of 7.8 µg/mL in vitro against the Xanthomonas oryzae pv. oryzicola (Xoc) pathogen, surpassing commercial agents thiodiazole copper (31.8 µg/mL) and bismerthiazol (43.3 µg/mL). Mechanistic investigations into its anti-Xoc properties revealed that compound A24 operates by increasing the permeability of bacterial cell membranes, inhibiting biofilm formation and cell motility, and inducing morphological changes in bacterial cells. Importantly, in vivo tests showed its excellent protective and curative effects on rice bacterial leaf streak. Besides, molecular docking showed that the hydrophobic effect and hydrogen-bond interactions are key factors between the binding of A24 and AvrRxo1-ORF1. Therefore, these results suggest the utilization of 1,3,4-thiadiazole derivatives containing sulfonylpiperazine structures as a bacterial biofilm inhibiting agent, warranting further exploration in the realm of agrochemical development.


Subject(s)
Anti-Bacterial Agents , Biofilms , Microbial Sensitivity Tests , Molecular Docking Simulation , Thiadiazoles , Xanthomonas , Thiadiazoles/chemistry , Thiadiazoles/pharmacology , Thiadiazoles/chemical synthesis , Structure-Activity Relationship , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemical synthesis , Anti-Bacterial Agents/chemistry , Xanthomonas/drug effects , Biofilms/drug effects , Piperazines/pharmacology , Piperazines/chemistry , Piperazines/chemical synthesis , Molecular Structure , Oryza/microbiology
15.
Nano Lett ; 23(9): 3678-3686, 2023 05 10.
Article in English | MEDLINE | ID: mdl-37052638

ABSTRACT

Identification of cancer metastatic sites is of importance for adjusting therapeutic interventions and treatment choice. However, identifying the location of metastatic lesions with easy accessibility and high safety is challenging. Here we demonstrate that cancer metastatic sites can be accurately detected by a triple targeting nanoprobe. Through coencapsulating molecular beacons probing a cancer biomarker (CXCR4 mRNA), a lung metastatic biomarker (CTSC mRNA), and a bone metastatic biomarker (JAG1 mRNA), the nanoprobe decorated by SYL3C conjugated hyaluronic acid and ICAM-1 specific aptamer conjugated hyaluronic acid can target diverse phenotyped circulating tumor cells (CTCs) during epithelial-mesenchymal and mesenchymal-epithelial transitions in whole blood for sensitive probing. The detection of CTCs from cancer patients shows that the nanoprobe can provide accurate information to distinguish different cancer metastasis statuses including nonmetastasis, lung metastasis, and bone metastasis. This study proposes an efficient screening tool for identifying the location of distant metastatic lesions via facile blood biopsy.


Subject(s)
Neoplastic Cells, Circulating , Humans , Hyaluronic Acid , Biomarkers, Tumor/genetics , Biopsy , RNA, Messenger/genetics , Neoplasm Metastasis
16.
Int J Mol Sci ; 25(14)2024 Jul 10.
Article in English | MEDLINE | ID: mdl-39062806

ABSTRACT

Histone arginine residue methylation is crucial for individual development and gene regulation. However, the dynamics of histone arginine methylation in response to cellular stress remains largely unexplored. In addition, the interplay and regulatory mechanisms between this and other histone modifications are important scientific questions that require further investigation. This study aimed to investigate the changes in histone arginine methylation in response to DNA damage. We report a global decrease in histone H3R26 symmetric dimethylation (H3R26me2s) and hypoacetylation at the H3K27 site in response to DNA damage. Notably, H3R26me2s exhibits a distribution pattern similar to that of H3K27ac across the genome, both of which are antagonistic to H3K27me3. Additionally, histone deacetylase 1 (HDAC1) may be recruited to the H3R26me2s demethylation region to mediate H3K27 deacetylation. These findings suggest crosstalk between H3R26me2s and H3K27ac in regulating gene expression.


Subject(s)
Arginine , Histone Deacetylase 1 , Histones , Histones/metabolism , Arginine/metabolism , Methylation , Humans , Histone Deacetylase 1/metabolism , Histone Deacetylase 1/genetics , DNA Damage , Acetylation , Protein Processing, Post-Translational , Stress, Physiological/genetics
17.
Molecules ; 29(14)2024 Jul 22.
Article in English | MEDLINE | ID: mdl-39065002

ABSTRACT

The metal-free porphyrins protonation has gained interest over five decades because its structure modification and hardly monoacid intermediate isolation. Here, upon the hydrogen atom abstraction processes, one step diproptonated H3STTP(BF4)2 (STTP = 5,10,15,20-tetraphenyl-21-thiaporphyrin) (3) and stepwise protonated HS2TTPSbCl6 (5) and diprotonated H2S2TTP(BF4)2 (6) (S2TTP = 5,10,15,20-tetraphenyl-21,23-thiaporphyrin) compounds were obtained using HSTTP and S2TTP with oxidants. The closed-shell protonated compounds were fully characterized using XRD, UV-vis, IR and NMR spectra. In addition, the reduced 19π compounds [K(2,2,2)]HSTTP (2) and [K(2,2,2)]S2TTP (7) were synthesized by the ligands with reductant KC8 in THF solution. These two open-shell compounds were characterized with UV-vis, IR and EPR spectroscopies. The semiempirical ZINDO/S method was employed to analyze the HOMO/LUMO gap lever and identify the electronic transitions of the UV-vis spectra of the closed- and open-shell porphyrin compounds.

18.
Psychogeriatrics ; 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39228150

ABSTRACT

BACKGROUND: This study aims to examine the association of depressive trajectories with disability-free-survival (DFS). METHODS: This prospective cohort study used data from the China Health and Retirement Longitudinal Study, 2011-2015. Depressive symptoms were assessed using the Centre for Epidemiology Studies Depression Scale-10. Disability was assessed using activities of daily living (ADLs) and instrumental ADLs. Trajectories of depressive symptoms were identified and classified by latent mixture modelling. Logistic regression models were used to examine the association between depressive trajectories and DFS. RESULTS: A total of 8373 participants aged 45 years and older were included. We identified four distinct trajectories of depressive symptoms: 'no depressive symptoms', 'decreasing depressive symptoms', 'increasing depressive symptoms', and 'persistent depressive symptoms'. Compared to participants in the no depressive symptom trajectory, those in the decreasing depressive symptoms, increasing depressive symptoms and persistent depressive symptoms trajectories had an increased risk of disability or mortality, with multiple-adjusted hazard ratios (95% confidence intervals) of 1.75 (1.45-2.12), 2.05 (1.77-2.38) and 3.50 (2.77-4.42). CONCLUSION: Our study shows that among middle-aged and older Chinese adults, individuals with a trajectory of depressive symptoms are at increased risk of disability or mortality. Our findings underscore the importance of early prevention, identification and intervention of depression in clinical care to promote healthy ageing.

19.
Zhongguo Yi Xue Ke Xue Yuan Xue Bao ; 46(1): 25-32, 2024 Feb.
Article in Zh | MEDLINE | ID: mdl-38433627

ABSTRACT

Objective To analyze the trends of disease burden of cervical cancer,uterine cancer,and ovarian cancer among Chinese women from 1990 to 2019,and to provide a basis for formulating precise prevention and control measures in China. Methods The global disease burden data in 2019 were used to describe the changes in indicators such as incidence,mortality,years of life lost due to premature mortality(YLL),years lived with disability(YLD),and disability-adjusted life year(DALY) of cervical,uterine,and ovarian cancers in China from 1990 to 2019.Furthermore,the Bayesian age-period-cohort model was adopted to predict the incidence and mortality of the cancers from 2020 to 2030. Results From 1990 to 2019,the incidence rates and mortality of cervical,uterine,and ovarian cancers in Chinese women showed an upward trend,and the age-standardized incidence rate of ovarian cancer increased the most(0.78%).In 2019,the incidence of cervical cancer and uterine cancer concentrated in the women of 55-59 years old,and ovarian cancer mainly occurred in the women of 70-74 years old.The DALY,YLL,and YLD of cervical,uterine,and ovarian cancers all presented varying degrees of growth at all ages.The Bayesian age-period-cohort model predicted that from 2020 to 2030,the incidence and mortality of cervical cancer in China showed a decreasing trend,while those of uterine cancer and ovarian cancer showed an increasing trend.There was no significant change in the age with high incidence of the three cancers. Conclusions From 1990 to 2019,the overall disease burden of cervical,uterine,and ovarian cancers in China increased,while the disease burden of cervical cancer decreased after 2020.It is recommended that the efforts should be doubled for the prevention and control of cervical,uterine,and ovarian cancers.


Subject(s)
Ovarian Neoplasms , Uterine Cervical Neoplasms , Female , Humans , Middle Aged , Aged , Uterine Cervical Neoplasms/epidemiology , Bayes Theorem , Ovarian Neoplasms/epidemiology , Cost of Illness , Genitalia , China/epidemiology
20.
Angew Chem Int Ed Engl ; 63(24): e202405676, 2024 Jun 10.
Article in English | MEDLINE | ID: mdl-38606914

ABSTRACT

Metal-organic framework (MOF) membranes with rich functionality and tunable pore system are promising for precise molecular separation; however, it remains a challenge to develop defect-free high-connectivity MOF membrane with high water stability owing to uncontrollable nucleation and growth rate during fabrication process. Herein, we report on a confined-coordination induced intergrowth strategy to fabricate lattice-defect-free Zr-MOF membrane towards precise molecular separation. The confined-coordination space properties (size and shape) and environment (water or DMF) were regulated to slow down the coordination reaction rate via controlling the counter-diffusion of MOF precursors (metal cluster and ligand), thereby inter-growing MOF crystals into integrated membrane. The resulting Zr-MOF membrane with angstrom-sized lattice apertures exhibits excellent separation performance both for gas separation and water desalination process. It was achieved H2 permeance of ~1200 GPU and H2/CO2 selectivity of ~67; water permeance of ~8 L ⋅ m-2 ⋅ h-1 ⋅ bar-1 and MgCl2 rejection of ~95 %, which are one to two orders of magnitude higher than those of state-of-the-art membranes. The molecular transport mechanism related to size-sieving effect and transition energy barrier differential of molecules and ions was revealed by density functional theory calculations. Our work provides a facile approach and fundamental insights towards developing precise molecular sieving membranes.

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