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1.
J Am Chem Soc ; 146(11): 7274-7287, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38377953

RESUMO

The utilization of anionic redox chemistry provides an opportunity to further improve the energy density of Li-ion batteries, particularly for Li-rich layered oxides. However, oxygen-based hosts still suffer from unfavorable structural rearrangement, including the oxygen release and transition metal (TM)-ion migration, in association with the tenuous framework rooted in the ionicity of the TM-O bonding. An intrinsic solution, by using a sulfur-based host with strong TM-S covalency, is proposed here to buffer the lattice distortion upon the highly activating sulfur redox process, and it achieves howling success in stabilizing the host frameworks. Experimental results demonstrate the prolonged preservation of the layered sulfur lattice, especially the honeycomb superlattice, during the Li+ extraction/insertion process in contrast to the large structural degeneration in Li-rich oxides. Moreover, the Li-rich sulfide cathodes exhibited a negligible overpotential of 0.08 V and a voltage drop of 0.13 mV/cycle, while maintaining a substantial reversible capacity upon cycling. These superior electrochemical performances can be unambiguously ascribed to the much shorter trajectories of sulfur in comparison to those of oxygen revealed by molecular dynamics simulations at a large scale (∼30 nm) and a long time scale (∼300 ps) via high-dimensional neural network potentials during the delithiation process. Our findings highlight the importance of stabilizing host frameworks and establish general guidance for designing Li-rich cathodes with durable anionic redox chemistry.

2.
Angew Chem Int Ed Engl ; : e202405620, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38709194

RESUMO

Manganese-based layered oxides are currently of significant interest as cathode materials for sodium-ion batteries due to their low toxicity and high specific capacity. However, the practical applications are impeded by sluggish intrinsic Na+ migration and poor structure stability as a result of Jahn-Teller distortion and complicated phase transition. In this study, a high-entropy strategy is proposed to enhance the high-voltage capacity and cycling stability. The designed P2-Na0.67Mn0.6Cu0.08Ni0.09Fe0.18Ti0.05O2 achieves a deeply desodiation and delivers charging capacity of 158.1 mAh g-1 corresponding to 0.61 Na with a high initial Coulombic efficiency of 98.2 %. The charge compensation is attributed to the cationic and anionic redox reactions conjunctively. Moreover, the crystal structure is effectively stabilized, leading to a slight variation of lattice parameters. This research carries implications for the expedited development of low-cost, high-energy-density cathode materials for sodium-ion batteries.

3.
Angew Chem Int Ed Engl ; 62(44): e202310894, 2023 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-37698488

RESUMO

Li-O2 battery (LOB) is a promising "beyond Li-ion" technology with ultrahigh theoretical energy density (3457 Wh kg-1 ), while currently impeded by the sluggish cathodic kinetics of the reversible gas-solid reaction between O2 and Li2 O2 . Despite many catalysts are developed for accelerating the conversion process, the lack of design guidance for achieving high performance makes catalysts exploring aleatory. The Sabatier principle is an acknowledged theory connecting the scaling relationship with heterogeneous catalytic activity, providing a tradeoff strategy for the topmost performance. Herein, a series of catalysts with wide-distributed d-band centers (i.e., wide range of adsorption strength) are elaborately constructed via high-entropy strategy, enabling an in-depth study of the Sabatier relations in electrocatalysts for LOBs. A volcano-type correlation of d-band center and catalytic activity emerges. Both theoretical and experimental results indicate that a moderate d-band center with appropriate adsorption strength propels the catalysts up to the top. As a demonstration of concept, the LOB using FeCoNiMnPtIr as catalyst provides an exceptional energy conversion efficiency of over 80 %, and works steadily for 2000 h with a high fixed specific capacity of 4000 mAh g-1 . This work certifies the applicability of Sabatier principle as a guidance for designing advanced heterogeneous catalysts assembled in LOBs.

4.
Angew Chem Int Ed Engl ; 62(41): e202310143, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37578683

RESUMO

The moderate reversibility of Zn anodes, as a long-standing challenge in aqueous zinc-ion batteries, promotes the exploration of suitable electrolyte additives continuously. It is crucial to establish the absolute predominance of smooth deposition within multiple interfacial reactions for stable zinc anodes, including suppressing side parasitic reactions and facilitating Zn plating process. Trehalose catches our attention due to the reported mechanisms in sustaining biological stabilization. In this work, the inter-disciplinary application of trehalose is reported in the electrolyte modification for the first time. The pivotal roles of trehalose in suppressed hydrogen evolution and accelerated Zn deposition have been investigated based on the principles of thermodynamics as well as reaction kinetics. The electrodeposit changes from random accumulation of flakes to dense bulk with (002)-plane exposure due to the unlocked crystal-face oriented deposition with trehalose addition. As a result, the highly reversible Zn anode is obtained, exhibiting a high average CE of 99.8 % in the Zn/Cu cell and stable cycling over 1500 h under 9.0 % depth of discharge in the Zn symmetric cell. The designing principles and mechanism analysis in this study could serve as a source of inspiration in exploring novel additives for advanced Zn anodes.

5.
Langmuir ; 38(45): 13841-13848, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36325981

RESUMO

A heterojunction of Cu2O and Cr-doped SrTiO3 (SrTi1-xCrxO3) was designed for selective photocatalytic isopropanol (IPA) oxidation under visible light irradiation. The photocatalytic oxidation of IPA was measured in a fixed-bed reactor. Cr dopants can increase the light absorption and improve the activity of the catalyst. The formation of the Cu2O/SrTi1-xCrxO3 heterojunction can further broaden the absorption range of lights and dramatically increase the photocatalytic activity for selective oxidation of IPA. The 3% Cu2O/SrTi0.99Cr0.01O3 catalyst can fully convert ∼1000 ppm IPA under illumination in 2 h. The selectivity of acetone is ∼100%. The yield is 83 and 4 times higher than that using SrTiO3 and SrTi0.99Cr0.01O3 as catalysts, respectively. By measuring the ultraviolet-visible absorption spectra and Mott-Schottky plots, we obtained the band structure of the heterojunction, which shows that the conduction and valence bands of Cu2O are higher than those of SrTi1-xCrxO3, therefore facilitating the separation and transfer of photogenerated electrons and holes. In addition, electron paramagnetic resonance spectroscopy and radical trapping tests reveal that the generation of hydroxyl and superoxide leads to photocatalytic oxidation of IPA by the heterojunction photocatalyst.

6.
Biomed Chromatogr ; 33(12): e4677, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31396971

RESUMO

An efficient ultra-performance liquid chromatography with diode-array detector method was established for simultaneous determination of six active components in Roukou Wuwei pills, namely gallic acid, piperine, costundide, dehydrocostus lactone, isoalantolactone and alantolactone. Chromatographic separation of six components was successfully achieved on an Waters BEH C18 column (50 × 2.1 mm, 1.7 µm) with a mobile phase composed of acetonitrile and water using a gradient elution. Gallic acid and piperine were detected at 270 nm and 343 nm, respectively; while costundide, dehydrocostus lactone, isoalantolactone and alantolactone were simultaneously measured at 225 nm. All six calibration curves showed good linearity (R2 ≥ 0.9994) between the peak area of each component and corresponding concentration. Relative standard deviations for inter- and intra-day precisions were <0.45 and 0.77%, respectively. The mean recovery rates ranged from 96.72 to 102.2% with relative standard deviations <2.07%. The developed method was validated in terms of linearity, precision and accuracy and then successfully applied for the quality control of commercial Roukou Wuwei samples.


Assuntos
Cromatografia Líquida de Alta Pressão/métodos , Medicamentos de Ervas Chinesas/análise , Medicamentos de Ervas Chinesas/química , Alcaloides/análise , Benzodioxóis/análise , Ácido Gálico/análise , Lactonas/análise , Limite de Detecção , Modelos Lineares , Piperidinas/análise , Alcamidas Poli-Insaturadas/análise , Reprodutibilidade dos Testes , Sesquiterpenos/análise
7.
Tumour Biol ; 35(7): 6867-77, 2014 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-25051917

RESUMO

The meta-analysis was conducted to evaluate the correlations between common genetic polymorphisms in the IFN-γ gene and susceptibility to breast cancer. The following electronic databases were searched without language restrictions: MEDLINE (1966 ~ 2013), the Cochrane Library Database (issue 12, 2013), EMBASE (1980 ~ 2013), CINAHL (1982 ~ 2013), Web of Science (1945 ~ 2013), and the Chinese Biomedical Database (CBM) (1982 ~ 2013). Meta-analysis was performed with the use of the STATA statistical software. Odds ratios (OR) with their 95 % confidence intervals (95 % CIs) were calculated. Nine clinical case-control studies met all the inclusion criteria and were included in this meta-analysis. A total of 1,182 breast cancer patients and 1,525 healthy controls were involved in this meta-analysis. Three functional polymorphisms were assessed, including rs2069705 C>T, rs2430561 T>A, and CA repeats 2/X. Our meta-analysis results indicated that IFN-γ genetic polymorphisms might be significantly associated with an increased risk of breast cancer (allele model: OR = 1.37, 95 % CI = 1.03 ~ 1.83, P = 0.031; dominant model: OR = 1.55, 95 % CI = 1.01 ~ 2.37, P = 0.046; homozygous model: OR = 2.23, 95 % CI = 1.30 ~ 3.82, P = 0.004; respectively), especially the rs2430561 T>A polymorphism. Subgroup analysis based on ethnicity suggested that genetic polymorphisms in the IFN-γ gene were closely correlated with increased breast cancer risk among Asians (allele model: OR = 1.21, 95 % CI = 1.02 ~ 1.58, P = 0.017; dominant model: OR = 3.44, 95 % CI = 2.07 ~ 5.71, P < 0.001; recessive model: OR = 1.58, 95 % CI = 1.06 ~ 2.37, P = 0.025; homozygous model: OR = 1.83, 95 % CI = 1.19 ~ 2.80, P = 0.006; respectively), but not among Caucasians (all P > 0.05). Our meta-analysis supported the hypothesis that IFN-γ genetic polymorphisms may contribute to an increased risk of breast cancer, especially the rs2430561 T>A polymorphism among Asians.


Assuntos
Neoplasias da Mama/genética , Predisposição Genética para Doença , Interferon gama/genética , Povo Asiático/genética , Neoplasias da Mama/patologia , Estudos de Casos e Controles , Feminino , Estudos de Associação Genética , Humanos , Fatores de Risco , População Branca/genética
8.
ACS Nano ; 18(1): 337-346, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38113246

RESUMO

Layered oxides are widely accepted to be promising cathode candidate materials for K-ion batteries (KIBs) in terms of their rich raw materials and low price, while their further applications are restricted by sluggish kinetics and poor structural stability. Here, the high-entropy design concept is introduced into layered KIB cathodes to address the above issues, and an example of high-entropy layered K0.45Mn0.60Ni0.075Fe0.075Co0.075Ti0.10Cu0.05Mg0.025O2 (HE-KMO) is successfully prepared. Benefiting from the high-entropy oxide with multielement doping, the developed HE-KMO exhibits half-metallic oxide features with a narrow bandgap of 0.19 eV. Increased entropy can also reduce the surface energy of the {010} active facets, resulting in about 2.6 times more exposure of the {010} active facets of HE-KMO than the low-entropy K0.45MnO2 (KMO). Both can effectively improve the kinetics in terms of electron conduction and K+ diffusion. Furthermore, high entropy can inhibit space charge ordering during K+ (de)insertion, and the transition metal-oxygen covalent interaction of HE-KMO is also enhanced, leading to suppressed phase transition of HE-KMO in 1.5-4.2 V and better electrochemical stability of HE-KMO (average capacity drop of 0.20%, 200 cycles) than the low-entropy KMO (average capacity drop of 0.41%, 200 cycles) in the wide voltage window.

9.
Mar Biotechnol (NY) ; 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38861111

RESUMO

Traf6, an adaptor protein, exhibits non-conventional E3 ubiquitin ligase activity and was well studied as an important factor in immune systems and cancerogenesis. In mice, the traf6-null caused a perinatal death, so that the underlying pathophysiology of traf6-defeciency is still largely unclear in animals. Here, in the present study, a traf6 knockout zebrafish line (traf6-/-) was generated and could survive until adulthood, providing a unique opportunity to demonstrate the functions of traf6 gene in animals' organogenesis beyond the mouse model. The body of traf6-/- fish was found to be significantly shorter than that of the wildtype (WT). Likewise, a comparative transcriptome analysis showed that 866 transcripts were significantly altered in the traf6-/- liver, mainly involved in the immune system, metabolic pathways, and progesterone-mediated oocyte maturation. Especially, the mRNA expression of the pancreas duodenum homeobox protein 1 (pdx1), glucose-6-phosphatase (g6pcb), and the vitellogenesis genes (vtgs) were significantly decreased in the traf6-/- liver. Subsequently, the glucose was found to be accumulated in the traf6-/- liver tissues, and the meiotic germ cell was barely detected in traf6-/- testis or ovary. The findings of this study firstly implied the pivotal functions of traf6 gene in the liver and gonads' development in fish species.

10.
Heliyon ; 10(11): e31250, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38828344

RESUMO

This study aimed to ascertain the delayed effects of various exposure temperatures on infectious diarrhea. We performed a Bayesian random-effects network meta-analysis to calculate relative risks (RR) with 95 % confidence intervals (95 % CI). The heterogeneity was analyzed by subgroup analysis. There were 25 cross-sectional studies totaling 6858735 patients included in this analysis, with 12 articles each investigating the effects of both hyperthermia and hypothermia. Results revealed that both high temperature (RRsingle = 1.22, 95%CI:1.04-1.44, RRcum = 2.96, 95%CI:1.60-5.48, P < 0.05) and low temperature (RRsingle = 1.17, 95%CI:1.02-1.37, RRcum = 2.19, 95%CI:1.33-3.64, P < 0.05) significantly increased the risk of infectious diarrhea, while high temperature caused greater. As-sociations with strengthening in bacillary dysentery were found for high temperatures (RRcum = 2.03, 95%CI:1.41-3.01, P < 0.05; RRsingle = 1.17, 95%CI:0.90-1.62, P > 0.05), while the statistical significance of low temperatures in lowering bacterial dysentery had vanished. This investigation examined that high temperature and low temperature were the conditions that posed the greatest risk for infectious diarrhea. This research offers fresh perspectives on preventing infectious diarrhea and will hopefully enlighten future studies on the impact of temperature management on infectious diarrhea.

11.
Heliyon ; 10(8): e28801, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38638993

RESUMO

Objective: To investigate the association between air pollutants and the incidence of tuberculosis (TB) through a systematic review and meta-analysis, and to provide directions for future research and prevention of TB. Methods: A search was conducted for all literature related to the incidence of TB and air pollution in the database. We screened the retrieved articles and proceeded statistical analyses using random effects models to investigate the relationships between five air pollutants (PM2.5, PM10, SO2, NO2 and O3) and the incidence of TB. Results: The initial search identified 100 pieces of literature and 9 studies met the screening criteria after the screening. The single-day lagged risk ratio (RR) and 95% Confidence Intervals (CIs) for the combined effects estimates are as follows: PM2.5: 1.059 (0.966, 1.160); PM10: 1.000 (0.996, 1.004); SO2: 0.980 (0.954, 1.007); NO2: 1.011 (0.994, 1.027); O3: 0.994 (0.980,1.008). The cumulative lagged results for these five pollutants are listed like this: PM2.5: 1.095 (0.983, 1.219); PM10: 1.035 (1.006, 1.066); SO2: 0.964 (0.830, 1.121); NO2: 1.037 (1.010, 1.065); O3: 0.982 (0.954, 1.010). Conclusion: The single-day lag effects of PM2.5, PM10, SO2, NO2, and O3 are not statistically significantly relevant for the occurrence of TB. However, the cumulative lag results show that both PM10 and NO2 contribute to the prevalence of TB, while the statistical relationship between the cumulative lag effects of PM2.5, SO2, and O3 and the onset of TB remains unknown.

12.
Sci Rep ; 13(1): 7440, 2023 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-37156811

RESUMO

Quantifying temporal and spatial changes in reactive nitrogen (Nr) losses from a watershed and exploring its main drivers are the key to watershed water quality improvements. Huge Nr losses continue to threaten the safety of the water environment in the Taihu Lake Basin (TLB). Here, the InVEST and GeoDetector models were combined to estimate Nr losses in the TLB from 1990 to 2020 and explore driving forces. Different scenarios for Nr losses were compared, showing that Nr loss peaked at 181.66 × 103 t in 2000. The key factors affecting Nr loss are land use, followed by elevation, soil, and slope factors, and their mean q-values were 0.82, 0.52, 0.51, and 0.48, respectively. The scenario analysis revealed that Nr losses increased under the business-as-usual and economic development scenarios, while ecological conservation, increased nutrient use efficiency, and reduced nutrient application all contribute to a reduction in Nr losses. The findings provide a scientific reference for Nr loss control and future planning in the TLB.

13.
Gene ; 887: 147729, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37619650

RESUMO

Rad51 is a recA-like recombinase that plays a crucial role in repairing DNA double-strand breaks through homologous recombination during mitosis and meiosis in mammals and other organisms. However, its role in reptiles remains largely unclear. In this study, we aimed to investigate the physiological role of the rad51 gene in reptiles, particularly in Pelodiscus sinensis. Firstly, the cDNA of rad51 gene was cloned and analyzed in P. sinensis. The cloned cDNA contained an open reading frame (ORF) of 1020 bp and encodeed a peptide of 339 amino acids. The multiple alignments and phylogenetic tree analysis of Rad51 showed that P. sinensis shares the high identity with Chelonia mydas (97.95%) and Mus musculus (95.89%). Secondly, reverse transcription-polymerase chain reaction (RT-PCR) and real-time quantitative polymerase chain reaction (RT-qPCR) analysis showed that rad51 mRNA was highly expressed in both ovary and testis, while being weak in the somatic tissues examined in this study. Furthermore, chemical in situ hybridization (CISH) was performed to examine the expression profile of rad51 mRNA in germ cells at different stages. In the testis, rad51 mRNA expression was found to be stronger in the germ cells at early stages, specifically in spermatogonia and spermatocytes, but it was undetectable in spermatids. In the ovary, rad51 mRNA exhibited a uniform distribution in the cytoplasm of oocytes at early stages. The signal intensity of rad51 mRNA was highest in primary oocytes and gradually declined during oogenesis as the oocytes developed. These results suggest that rad51 plays a vital role in the development of germ cells, particularly during the early stages of gametogenesis in P. sinensis. The dynamic expression pattern of rad51 mRNA provides insights into the mechanisms underlying germ cell development and differentiation into gametes in turtles, even in reptiles.


Assuntos
Tartarugas , Animais , Feminino , Masculino , Clonagem Molecular , DNA Complementar/metabolismo , Gametogênese , Filogenia , RNA Mensageiro/análise , Espermatogônias/metabolismo , Testículo/metabolismo , Tartarugas/genética
14.
Cell Death Dis ; 14(11): 760, 2023 11 23.
Artigo em Inglês | MEDLINE | ID: mdl-37993451

RESUMO

Lipid metabolism is the key to ferroptosis susceptibility. However, little is known about the underlying mechanisms in osteosarcoma cells. Functional restriction of bromodomain-containing protein 4 (BRD4) reduced the susceptibility to erastin-induced ferroptosis of osteosarcoma cells both in vitro and in vivo. Mechanically, BRD4 controls the splicing efficiency of the RNA precursor (pre-mACSL3) of ACSL3 (ACSL3) by recruiting serinerich/threonine protein kinase 2 (SRPK2) to assemble the splicing catalytic platform. Moreover, the AMP-binding domain of ACSL3 significantly influences arachidonic acid synthesis and thus determines the susceptibility to erastin-induced ferroptosis. Overall, we found a BRD4-mediated pre-mACSL3 splicing influences erastin-induced ferroptosis by affecting arachidonic acid synthesis in osteosarcoma cells. Data in this study fills some of the gap in understanding the post-transcriptional regulatory mechanisms of ACSL3 and provides new insights into the mechanisms of lipid metabolism regulation and its effect on susceptibility to ferroptosis in osteosarcoma cells.


Assuntos
Ferroptose , Osteossarcoma , Humanos , Proteínas Serina-Treonina Quinases/metabolismo , Ferroptose/genética , Precursores de RNA/genética , Precursores de RNA/metabolismo , Proteínas Nucleares/metabolismo , Proteínas Quinases/metabolismo , Fatores de Transcrição/metabolismo , Ácido Araquidônico/farmacologia , Proteínas de Ligação a RNA , Osteossarcoma/genética , Fatores de Processamento de Serina-Arginina , Proteínas de Ciclo Celular/metabolismo
15.
J Bone Oncol ; 43: 100512, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38021073

RESUMO

Background: Acquired drug-resistance is the major risk factor for poor prognosis and short-term survival in patients with osteosarcoma (OS). Accumulating evidence has revealed that long noncoding RNAs (lncRNAs), including plasmacytoma variant translocation 1 (PVT1), play potential regulatory roles in the malignant development of OS. Considering the subcellular distribution of PVT1 as both nuclear and cytoplasmic lncRNA, a thorough exploration of its extensive mechanisms becomes essential. Methods: The GEO database was utilized for the acquisition of gene expression data, which was subsequently analyzed to fulfill the research objectives. The subcellular localization of PVT1 in OS cells was determined using fluorescence in situ hybridization (FISH) and quantitative real-time polymerase chain reaction (qRT-PCR). Additionally, the sensitivity of OS cells to doxorubicin was comprehensively evaluated through measurements of cell viability, site-specific proliferation capacity, and the relative expression abundance of multidrug resistance-related proteins (MRPs). In order to investigate the differential response of OS cells with varying levels of PVT1 expression to doxorubicin, pulmonary metastasis mice models were established for in vivo studies. Molecular interactions were further examined using the dual-luciferase assay and RNA immunoprecipitation assay (RIP) to analyze the binding sites of miR-15a-5p and miR-15b-5p on PVT1 and G1/S-specific cyclinD1 (CCND1) mRNA. Furthermore, the chromatin immunoprecipitation (ChIP) and dual-luciferase assay were employed to assess the transcriptional activation of the proto-oncogene c-myc (MYC) on the CCND1 promoter and identify the corresponding binding sites. Results: In doxorubicin resistant OS cells, transcription levels of PVT1, MYC and CCND1 were significantly higher than those in original cells. In vivo experiments demonstrated that OS cells rich in PVT1 expression exhibited enhanced tumorigenicity and resistance to doxorubicin. In vitro experiments, it has been observed that overexpression of PVT1 in OS cells is accompanied by an upregulation of CCND1, thereby facilitating resistance to doxorubicin. Nonetheless, this PVT1-induced resistance can be effectively attenuated by the knockdown of CCND1. Mechanistically, PVT1 functions as a competitive endogenous RNA (ceRNA) that influences the expression of CCND1 by inhibiting the degradation function of miR-15a-5p and miR-15b-5p on CCND1 mRNA. Additionally, as a neighboring gene of MYC, PVT1 plays a role in maintaining MYC protein stability, which further enhances MYC-dependent CCND1 transcriptional activity. Conclusion: The resistance of OS cells to doxorubicin is facilitated by PVT1, which enhances the expression of CCND1 through a dual mechanism. This findings offer a novel perspective for comprehending the intricate regulatory mechanisms of long non-coding RNA in influencing the expression of coding genes.

16.
Sci Adv ; 9(44): eadj8171, 2023 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-37922354

RESUMO

All-solid-state batteries (ASSBs) represent a promising battery strategy to achieve high energy density with great safety. However, inadequate kinetic property and poor interfacial compatibility remain great challenges, which impede their practical application. A prototype of dual-ion conductor of Li+ synchronized with Cu+ unlocks a four-electron redox reaction with high reversibility and fast kinetics. As a result, the constructed ASSB exhibited a high reversible capacity of 603.0 mA·hour g-1 and an excellent cycling retention of 93.2% over 1500 cycles. Moreover, because of the ion highway connecting active materials and catholytes constructed by dual-ion conductor, remarkable temperature tolerance (-60°C) and excellent rate performance (231.6 mA·hour g-1 at 20 mA cm-2) were achieved. The superior electrochemical performance can be ascribed to the migration pathway with small energy barrier and low tortuosity once the Cu+ introduced into Li6PS5Cl. This work creates a unique perspective of ASSBs with dual-ion conducting strategy, thus inspiring a potential developing strategy of state-of-the-art ASSBs.

17.
Chem Commun (Camb) ; 58(8): 1219-1222, 2022 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-34985057

RESUMO

A Zn2+-induced reactive separation method for the purification of ß-bromoethylbenzene from α-ß-bromoethylbenzene mixtures is discovered, where the selective decomposition of α-bromoethylbenzene follows a radical mechanism. Zn2+ facilitates the homolysis of the C-Br bond of halohydrocarbons with benzyl bromide, enabling the separation of the corresponding isomers with almost identical physical properties.

18.
ChemSusChem ; 15(7): e202102439, 2022 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-35132790

RESUMO

For a heterogeneous catalytic process, the performance of catalysts could be improved by modifying the active metal with a second element. Determining the enhanced mechanism of the second element is essential to the rational design of catalysts. In this work, Zn was introduced as a second element into Ni/ZrO2 for CO2 hydrogenation. In contrast to Ni/ZrO2 , the selectivity of NiZn/ZrO2 is observed to shift from CH4 to CO. A series of structural characterization results reveals that Zn is atomically dispersed in the NiO and ZrO2 phases as NiZnOx and ZnZrOx , respectively during CO2 hydrogenation, stabilizing a higher valence state of Ni (Niδ+ ) under a hydrogenation atmosphere over Ni-O-Zn site and thus promoting the generation of CO. These findings shed light on the O-mediated bimetallic effect of NiZn/ZrO2 and bring new insight into the rational design of more efficient heterogeneous catalysts.

19.
Environ Sci Pollut Res Int ; 29(20): 30114-30125, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-34997480

RESUMO

Excessive nitrogen (N) load in sediments is at risk of release resulting in the degradation of grass-type lake ecosystems. At present, the occurrence characteristics of N forms and the driving forces of organic N (ON) hydrolysis in the sediments of Taihu Lake were still unclear. Here, 52 sampling sites in 7 lake areas in Taihu Lake were investigated to compare the spatial occurrence characteristics of the sedimentary free N (FN), exchangeable N (EN), acid hydrolyzable N (HN), and residual N (RN) and their associated driving forces. The results showed that the total N contents in the dry sediment ranged from 1811.56 to 5594.06 mg kg-1, and the contribution was in the order of RN > HN > EN > FN. Spatially, RN and total organic carbon were significantly consistently influenced by dam construction and deposition algal residue. The HN concentration was high in the estuaries affected by N inputs from the rivers. The coupling relationship of spatial distribution between ON and N forms was revealed. The factors, i.e., algal residue deposition and terrigenous N inputs, were considered as the main driving forces stimulating the ON hydrolysis in the algae-type lake zones. It can be deduced that controlling terrigenous N inputs and sediment suspension may be the key to inhibiting the transformation from grass-type to algae-type lake ecosystem.


Assuntos
Nitrogênio , Poluentes Químicos da Água , China , Ecossistema , Monitoramento Ambiental , Sedimentos Geológicos/química , Lagos/química , Nitrogênio/análise , Poaceae , Poluentes Químicos da Água/análise
20.
ACS Appl Mater Interfaces ; 14(1): 1203-1211, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34928584

RESUMO

Sodium (Na) metal batteries receive increasing attention because of their high energy densities and low costs that are enabled by the abundant Na resources. However, dendritic growth and low efficiency of Na-metal anodes limit the practical applications of Na-metal batteries. Here, we propose a three-dimensionally pillared structure in which carbonized nanoparticles of zeolite imidazolate framework-8 (ZIF-8) are sandwiched between reduced graphene oxide (rGO) sheets (ZIF-8-C@rGO). Such a pillared structure enables two advantages over rGO. First, the sodiation products of ZIF-8 (NaZn13, Na2O, and N-doped carbon) have a strong chemical affinity to Na metal, thereby inducing favorable nucleation of Na metal to guide Na deposition. Second, the pillared structure could facilitate the diffusion of Na ions through rGO sheets and help homogenize the current distribution, leading to a uniform deposition of Na metal. As a result, ZIF-8-C@rGO exhibits a dendrite-free morphology during Na plating/stripping and excellent cycling stability with high Coulombic efficiency of over 99.8% for at least 2000 h. A symmetric cell could maintain more than 4000 h with a stable average overpotential of only 30 mV at a capacity of 1 mA h cm-2. This work demonstrates that the design of a ZIF-pillared structure could combine thermodynamic and kinetic regulating factors to offer an alternative solution to the development of durable Na electrodes for high-performance Na-metal batteries.

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