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1.
Angew Chem Int Ed Engl ; : e202400916, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38767752

RESUMO

Prussian blue analogs (PBAs) as insertion-type cathodes have attracted significant attention in various aqueous batteries to accommodate metal or non-metal ions while suffering from serious dissolution and consequent inferior lifespan. Herein, we reveal that the dissolution of PBAs primarily originates from the locally elevated pH of electrolytes that are caused by proton co-insertion during discharge. To address this issue, a water-locking electrolyte (WLE) has been strategically implemented, which interrupts the generation and Grotthuss diffusion of protons by breaking the well-connected hydrogen bonding network in aqueous electrolytes. As a result, the WLE enables the iron hexacyanoferrate to endure over 1000 cycles at a 1C rate and supports a high-voltage decoupled cell with an average voltage of 1.95 V. These findings provide insights for mitigating dissolution problems in electrode materials, thereby enhancing the viability and performance of aqueous batteries.

2.
Adv Mater ; : e2313388, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38350631

RESUMO

Organic electrode materials (OEMs) have gathered extensive attention for aqueous zinc-ion batteries (AZIBs) due to their structural diversity and molecular designability. However, the reported research mainly focuses on the design of the planar configuration of OEMs and does not take into account the important influence of the spatial structure on the electrochemical properties, which seriously hamper the further performance liberation of OEMs. Herein, this work has designed a series of thioether-linked naphthoquinone-derived isomers with tunable spatial structures and applied them as the cathodes in AZIBs. The incomplete conjugated structure of the elaborately engineered isomers can guarantee the independence of the redox reaction of active groups, which contributes to the full utilization of active sites and high redox reversibility. In addition, the position isomerization of naphthoquinones on the benzene rings changes the zincophilic activity and redox kinetics of the isomers, signifying the importance of spatial structure on the electrochemical performance. As a result, the 2,2'-(1,4-phenylenedithio) bis(1,4-naphthoquinone) (p-PNQ) with the smallest steric hindrance and the most independent redox of active sites exhibits a high specific capacity (279 mAh g-1 ), an outstanding rate capability (167 mAh g-1 at 100 A g-1 ), and a long-term cycling lifetime (over 2800 h at 0.05 A g-1 ).

3.
Angew Chem Int Ed Engl ; 62(35): e202307365, 2023 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-37423888

RESUMO

The slow reaction kinetics and structural instability of organic electrode materials limit the further performance improvement of aqueous zinc-organic batteries. Herein, we have synthesized a Z-folded hydroxyl polymer polytetrafluorohydroquinone (PTFHQ) with inert hydroxyl groups that could be partially oxidized to the active carbonyl groups through the in situ activation process and then undertake the storage/release of Zn2+ . In the activated PTFHQ, the hydroxyl groups and S atoms enlarge the electronegativity region near the electrochemically active carbonyl groups, enhancing their electrochemical activity. Simultaneously, the residual hydroxyl groups could act as hydrophilic groups to enhance the electrolyte wettability while ensuring the stability of the polymer chain in the electrolyte. Also, the Z-folded structure of PTFHQ plays an important role in reversible binding with Zn2+ and fast ion diffusion. All these benefits make the activated PTFHQ exhibit a high specific capacity of 215 mAh g-1 at 0.1 A g-1 , over 3400 stable cycles with a capacity retention of 92 %, and an outstanding rate capability of 196 mAh g-1 at 20 A g-1 .

4.
Am J Cancer Res ; 13(4): 1533-1546, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37168345

RESUMO

Prostate cancer is one of the most lethal malignancies, and androgen deprivation therapy remains the mainstay of treatment for prostate cancer patients. Although androgen deprivation can initially come to remission, the disease often develops into castration-resistant prostate cancer (CRPC), which is still dependent on androgen receptor (AR) signaling and is related to a poor prognosis. Some success against CRPC has been achieved by drugs that target AR signaling, but secondary resistance uninterrupted emerges, and new therapies are urgently needed. In this study, we identified a potent small molecule compound, ZY-444, that suppressed PCa cells proliferation and metastasis, and inhibited tumor growth both in subcutaneous. Transcriptome sequencing analysis showed that TNFAIP3 was significantly elevated in prostate cancer cells after ZY-444 treatment. Further studies through overexpression of TNFAIP3 confirmed that TNFAIP3, as a direct target gene of ZY-444, contributes to the functions of ZY-444. In addition, we demonstrated the effects of TNFAIP3 on prostate cancer cell apoptosis, migration and proliferation to elucidate the mechanism of ZY-444. We found that TNFAIP3 inhibited the TNF signaling pathway, which could inhibit cell migration and proliferation and contribute to apoptosis. Overall, these findings highlighted TNFAIP3 as a tumor suppressor gene in the regulation of the progression and metastatic potential of prostate cancer and that targeting TNFAIP3 by ZY-444 might be a promising strategy for prostate cancer treatment.

5.
Adv Mater ; 35(22): e2301088, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37036047

RESUMO

Organic materials have attracted much attention in aqueous zinc-ion batteries (AZIBs) due to their sustainability and structure-designable, but their further development is hindered by the high solubility, poor conductivity, and low utilization of active groups, resulting in poor cycling stability, terrible rate capability, and low capacity. In order to solve these three major obstacles, a novel organic host, benzo[b]naphtho[2',3':5,6][1,4]dithiino[2,3-i]thianthrene-5,7,9,14,16,18-hexone (BNDTH), with abundant electroactive groups and stable extended π-conjugated structure is synthesized and composited with reduced graphene oxide (RGO) through a solvent exchange composition method to act as the cathode material for AZIBs. The well-designed BNDTH/RGO composite exhibits a high capacity of 296 mAh g-1 (nearly a full utilization of the active groups), superior rate capability of 120 mAh g-1 , and a long lifetime of 58 000 cycles with a capacity retention of 65% at 10 A g-1 . Such excellent performance can be attributed to the ingenious structural design of the active molecule, as well as the unique solvent exchange composition strategy that enables effective dispersion of excess charge on the active molecule during discharge/charge process. This work provides important insights for the rational design of organic cathode materials and has significant guidance for realizing ideal high performance in AZIBs.

6.
J Cell Physiol ; 237(12): 4580-4590, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36317691

RESUMO

Polo like kinase 1 (PLK1) is a protein kinase involved in regulating the spindle assembly and cell cycle control in mammalian oocytes. SUMOylation, one way of post-translational modification, regulates oocyte meiosis by controlling several substrates. However, the relation between PLK1 and SUMOylation in oocytes is still unknown. In this study, we investigated that whether PLK1 was modified by SUMOylation in oocytes and its potential relationship with age-related meiotic abnormalities. We showed that PLK1 had colocalization and protein interaction with Small Ubiquitin-Like Modifier (SUMO)-1 and SUMO-2/3 in mouse oocytes, indicating that PLK1 could be modified by SUMO-1 and SUMO-2/3. Overexpression of PLK1 SUMOylation site mutants PLK1K178R and PLK1K191R caused the increase of the abnormal spindle rate of oocytes and the decline of the first polar body extrusion rate with the abnormal localization of PLK1, suggesting that the SUMOylation modification of PLK1 is essential for normal meiosis in oocytes. Compared with young mice, the expression of PLK1 protein increased and the expression of SUMO-1 and SUMO-2/3 protein decreased in the oocytes of aged mice, indicating that the SUMOylation of PLK1 might be related to the mouse aging. Therefore, our data suggested that PLK1 could be SUMOylated by SUMO-1 and SUMO-2/3 in mouse oocytes and SUMOylation of PLK1 regulated the meiosis progression of oocytes which was related with aging.


Assuntos
Proteínas de Ciclo Celular , Meiose , Oócitos , Proteínas Serina-Treonina Quinases , Sumoilação , Animais , Camundongos , Proteínas de Ciclo Celular/metabolismo , Oócitos/metabolismo , Fuso Acromático/metabolismo , Proteínas Serina-Treonina Quinases/metabolismo , Proteínas Proto-Oncogênicas/metabolismo , Fatores Etários , Quinase 1 Polo-Like
7.
Angew Chem Int Ed Engl ; 60(51): 26806-26812, 2021 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-34582084

RESUMO

The performance of electrode material is correlated with the choice of electrolyte, however, how the solvation has significant impact on electrochemical behavior is underdeveloped. Herein, N-heteropentacenequinone (TAPQ) is investigated to reveal the solvation effect on the performance of sodium-ion batteries in different electrolyte environment. TAPQ cycled in diglyme-based electrolyte exhibits superior electrochemical performance, but experiences a rapid capacity fading in carbonate-based electrolyte. The function of solvation effect is mainly embodied in two aspects: one is the stabilization of anion intermediate via the compatibility of electrode and electrolyte, the other is the interfacial electrochemical characteristics influenced by solvation sheath structure. By revealing the failure mechanism, this work presents an avenue for better understanding electrochemical behavior and enhancing performance from the angle of solvation effect.

8.
Huan Jing Ke Xue ; 37(7): 2714-2720, 2016 Jul 08.
Artigo em Chinês | MEDLINE | ID: mdl-29964483

RESUMO

Evaluating the response of soil microbial respiration to extreme precipitation event is significant for a better understanding about the influence of the change of precipitation regime on soil carbon cycling under global warming. A simulated experiment of extreme precipitations was conducted during the rainy season (July-September 2015) in the Changwu State Key Agro-Ecological Station, Shaanxi, China. The treatments consisted of three total precipitations in rainy season (600 mm, 300 mm, and 150 mm) and two precipitation regimes (10 mm, 150 mm; P10, P150). Soil microbial respiration varied differently in the same single rainfall event among three precipitations. The variation coefficient of soil microbial respiration under 600 mm total precipitation was 36% (P150) and 33% (P10), and 28% and 22% under 300 mm total precipitation, 43% and 29% under 150 mm total precipitation. Under 600 mm total precipitation, the cumulative soil microbial respiration under P150 was 20% less than that under P10; however, the cumulative soil respiration of P150 under 150 mm total precipitation was 22% more than that under P10; and there was no significant difference between P10 and P150 under 300 mm total precipitation. Therefore, the duration in soil water stress must be considered to estimate soil microbial respirations under extreme precipitations.


Assuntos
Clima Desértico , Chuva , Microbiologia do Solo , Ciclo do Carbono , China , Solo
9.
Huan Jing Ke Xue ; 37(9): 3616-3624, 2016 Sep 08.
Artigo em Chinês | MEDLINE | ID: mdl-29964800

RESUMO

The CO2 flux from soil is an important component of global carbon cycle, and a small variation of soil CO2 flux can prominently influence atmospheric CO2 concentration and soil organic carbon stock. Soil erosion significantly influences soil CO2 emission. However, the process of soil CO2 flux during soil erosion and soil deposition remains uncertain. At the present study, a simulated experiment on soil erosion and deposition was conducted at Changwu State Key Agro-Ecological Station, Shaanxi, China. From July to September in 2014 and 2015, soil CO2 flux was periodically measured using an automated CO2 flux system LI-8100 (LI-COR, Lincoln, NE, USA) and soil temperature and moisture were collected by series data collection system of soil temperature and soil moisture (EM50, DECAGON, USA). The measurement frequency of soil CO2 flux was once a week during 09:00 and 11:00. Soil temperature and soil moisture of 10 cm topsoil were measured continuously (at an interval of 30 minutes) during the experiment. At the same time, runoff and sediment were collected as well in each rain event, and then SOC content in sediment was measured. The results showed that soil CO2 flux between erosion and deposition sites had a significant difference (P<0.05), and soil CO2 flux at deposition site [mean value 1.38 µmol·(m2·s)-1] was 31% higher than that of soil CO2 flux at deposition site [1.05 µmol·(m2·s)-1], while temperature sensitivity at deposition site (Q10:8.14) was 3 times as high as that at erosion site (2.34). Soil moisture at deposition site was 19% higher than that at erosion site (P<0.05). Soil temperature was slightly higher at erosion site. The average SOC content (7.26 g·kg-1) increased by 6% in the sediment compared with the initial SOC content (6.83 g·kg-1). Soil moisture and SOC redistribution across erosion and deposition sites were influencing factors for soil CO2 flux under erosional environment. In conclusion, soil CO2 flux showed a significant variation at erosion site and deposition site. Changes in soil moisture and SOC contributed much to the difference in soil CO2 flux across erosion and deposition sites.

10.
Huan Jing Ke Xue ; 36(5): 1802-9, 2015 May.
Artigo em Chinês | MEDLINE | ID: mdl-26314133

RESUMO

Understanding the effects of nitrogen fertilization on soil respiration rate and its temperature sensitivity (Q10) is of critical importance to predict the variability of soil respiration in cropland. A field experiment was established in a rain-fed spring maize cropland (Zea mays L. ) in the State Key Agro-Ecological Experimental Station in the Loess Plateau in Changwu County, Shaanxi Province, China. The experiment comprised of two treatments: no N-fertilizer application ( CK) and N-fertilizer application with 160 kg N · hm(-2) (N). Soil respiration rate, soil temperature, soil moisture, yields, aboveground biomass and root biomass were measured in two continuous spring maize growing seasons from April 2013 to September 2014. The cumulative soil CO2 emissions were increased by 35% in 2013 and 54% in 2014 in N treatment as compared to CK treatment. Though nitrogen fertilization significantly increased the cumulative soil CO2 emissions (P < 0.05), it did decrease evidently the temperature sensitivity of soil respiration (P < 0.05) . The Q10 values in N treatment were decreased by 27% and 17% compared with CK treatment in 2013 and 2014, respectively. Nitrogen fertilization significantly increased the maize yields, aboveground biomass and root biomass (P < 0.05). Root biomasses in N treatment were 32% and 123% greater than those in CK treatment of 2013 and 2014, respectively. Nitrogen fertilization had no marked influence on soil temperature or moisture. Root biomass was a critical biotical factor for variation of soil respiration under nitrogen fertilization.


Assuntos
Clima Desértico , Fertilizantes , Nitrogênio/química , Solo/química , Temperatura , Biomassa , China , Raízes de Plantas/crescimento & desenvolvimento , Estações do Ano , Zea mays/crescimento & desenvolvimento
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