In response to the call for safer high‐energy‐density storage systems, high‐voltage solid‐state Li metal batteries have attracted extensive attention. Therefore, solid electrolytes are required to be ...stable against both Li anode and high‐voltage cathodes; nevertheless, the requirements still cannot be completely satisfied. Herein, a heterogeneous multilayered solid electrolyte (HMSE) is proposed to broaden electrochemical window of solid electrolytes to 0–5 V, through different electrode/electrolyte interfaces to overcome the interfacial instability problems. Oxidation‐resistance poly(acrylonitrile) (PAN) is in contact with the cathode, while reduction tolerant polyethylene glycol diacrylate contacts with Li metal anode. A Janus and flexible PAN@Li1.4Al0.4Ge1.6(PO4)3 (80 wt%) composite electrolyte is designed as intermediate layer to inhibit dendrite penetration and ensure compact interface. Paired with LiNi0.6Co0.2Mn0.2O2 and LiNi0.8Co0.1Mn0.1O2 cathodes, which are rarely used in solid‐state batteries, the solid‐state Li metal batteries with HMSE exhibit excellent electrochemical performance including high capacity and long cycle life. Besides, the Li||Li symmetric batteries maintain a stable polarization less than 40 mV for more than 1000 h under 2 mA cm−2 and effective inhibition of dendrite formation. This study offers a promising approach to extend the applications of solid electrolytes for high‐voltage solid‐state Li metal batteries.
A heterogeneous multilayered structure that expands the electrochemical window of solid electrolytes is designed. The oxidation‐resistant poly(acrylonitrile) (PAN) and reduction‐tolerant polyethylene glycol diacrylate integrated with the Janus and flexible PAN@Li1.4Al0.4Ge1.6(PO4)3 (80 wt%) composite electrolyte broaden the electrochemical window to 0–5 V, resulting in excellent performance for high‐voltage solid‐state Li‐metal batteries. Additionally, the thickness of electrolyte is below 25 μm.
Garnet‐type electrolytes suffer from unstable chemistry against air exposure, which generates contaminants on electrolyte surface and accounts for poor interfacial contact with the Li metal. Thermal ...treatment of the garnet at >700 °C could remove the surface contaminants, yet it regenerates the contaminants in the air, and aggravates the Li dendrite issue as more electron‐conducting defective sites are exposed. In a departure from the removal approach, here we report a new surface chemistry that converts the contaminants into a fluorinated interface at moderate temperature <180 °C. The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, so that it enables dendrite‐proof Li plating/stripping at a high critical current density of 1.4 mA cm−2. Moreover, the modified interface exhibits high chemical and electrochemical stability against air exposure, which prevents regeneration of contaminants and keeps high critical current density of 1.1 mA cm−2. The new chemistry presents a practical solution for realization of high‐energy solid‐state Li metal batteries.
The detrimental contaminants on a garnet surface are converted into an air‐stable fluorinated interface by a facile chemical approach at moderate temperature (<180 °C). The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, enabling a high critical current density of 1.4 mA cm−2.
Tumour microenvironment (TME) is crucial to tumorigenesis. This study aimed to uncover the differences in immune phenotypes of TME in endometrial cancer (EC) using Uterine Corpus Endometrial ...Carcinoma (UCEC) cohort and explore the prognostic significance. We employed GVSA enrichment analysis to cluster The Cancer Genome Atlas (TCGA) EC samples into immune signature cluster modelling, evaluated immune cell profiling in UCEC cohort (n = 538) and defined four immune subtypes of EC. Next, we analysed the correlation between immune subtypes and clinical data including patient prognosis. Furthermore, we analysed the expression of immunomodulators and DNA methylation modification. The profiles of immune infiltration in TCGA UCEC cohort showed significant difference among four immune subtypes of EC. Among each immune subtype, natural killer T cells (NKT), dendritic cells (DCs) and CD8+T cells were significantly associated with EC patients survival. Each immune subtype exhibited specific molecular classification, immune cell characterization and immunomodulators expression. Moreover, the expression immunomodulators were significantly related to DNA methylation level. In conclusion, the identification of immune subtypes in EC tissues could reveal unique immune microenvironments in EC and predict the prognosis of EC patients.
Abstract
Na-ion cathode materials operating at high voltage with a stable cycling behavior are needed to develop future high-energy Na-ion cells. However, the irreversible oxygen redox reaction at ...the high-voltage region in sodium layered cathode materials generates structural instability and poor capacity retention upon cycling. Here, we report a doping strategy by incorporating light-weight boron into the cathode active material lattice to decrease the irreversible oxygen oxidation at high voltages (i.e., >4.0 V vs. Na
+
/Na). The presence of covalent B–O bonds and the negative charges of the oxygen atoms ensures a robust ligand framework for the NaLi
1/9
Ni
2/9
Fe
2/9
Mn
4/9
O
2
cathode material while mitigating the excessive oxidation of oxygen for charge compensation and avoiding irreversible structural changes during cell operation. The B-doped cathode material promotes reversible transition metal redox reaction enabling a room-temperature capacity of 160.5 mAh g
−1
at 25 mA g
−1
and capacity retention of 82.8% after 200 cycles at 250 mA g
−1
. A 71.28 mAh single-coated lab-scale Na-ion pouch cell comprising a pre-sodiated hard carbon-based anode and B-doped cathode material is also reported as proof of concept.
The novel free radical‐based cleavage of the enaminone C=C double bond is realized by using N‐halosuccinimides (NXS) in the presence of benzoyl peroxide (BPO) with mild heating, enabling the tunable ...synthesis of α,α‐dihalomethyl ketones and α,α,α‐trihalomethyl ketones under different reaction conditions. The formation of these divergent products involving featured C=C double bond cleavage requires no any metal reagent, and represents one more practical example on the synthesis of poly halogenated methyl ketones via the functionalization of carbon−carbon bond.
Cancer‐associated fibroblasts (CAFs) play crucial roles in tumor progression, given the dependence of cancer cells on stromal support. Therefore, understanding how CAFs communicate with endometrial ...cancer cell in tumor environment is important for endometrial cancer therapy. Exosomes, which contain proteins and noncoding RNA, are identified as an important mediator of cell–cell communication. However, the function of exosomes in endometrial cancer metastasis remains poorly understood. In the current study we found that CAF‐derived exosomes significantly promoted endometrial cancer cell invasion comparing to those from normal fibroblasts (NFs). We identified a significant decrease of miR‐148b in CAFs and CAFs‐derived exosomes. By exogenously transfect microRNAs, we demonstrated that miR‐148b could be transferred from CAFs to endometrial cancer cell through exosomes. In vitro and in vivo studies further revealed that miR‐148b functioned as a tumor suppressor by directly binding to its downstream target gene, DNMT1 to suppress endometrial cancer metastasis. In endometrial cancer DNMT1 presented a potential role in enhancing cancer cell metastasis by inducing epithelial–mesenchymal transition (EMT). Therefore, downregulated miR‐148b induced EMT of endometrial cancer cell as a result of relieving the suppression of DNMT1. Taken together, these results suggest that CAFs‐mediated endometrial cancer progression is partially related to the loss of miR‐148b in the exosomes of CAFs and promoting the transfer of stromal cell‐derived miR‐148b might be a potential treatment to prevent endometrial cancer progression.
miR‐148b promotes endometrial cancer cell invasion and metastasis
Radical C(sp2)–H sulfonylation and C(sp2)–N bond oxygenation enabling the chemoselective synthesis of 3‐sulfonyl chromones by using enaminones and sulfonyl hydrazines were accomplished. The domino ...reactions ran well by using molecular iodine without the assistance of any strong oxidant such as a peroxide or a hypervalent metal salt.
The direct synthesis of 3‐sulfonyl chromones is accomplished for the first time through the tandem reaction of enaminones and sulfonyl hydrazines by C–N bond oxygenation and C(sp2)–H bond sulfonylation under transition‐metal‐free conditions. DMAC=N,N‐dimethylacetamide.
The aim of this paper is to develop a new Atanassov's intuitionistic fuzzy (A-IF) programming method to solve heterogeneous multiattribute group decision-making problems with A-IF truth degrees in ...which there are several types of attribute values such as A-IF sets (A-IFSs), trapezoidal fuzzy numbers, intervals, and real numbers. In this method, preference relations in comparisons of alternatives with hesitancy degrees are expressed by A-IFSs. Hereby, A-IF group consistency and inconsistency indices are defined on the basis of preference relations between alternatives. To estimate the fuzzy ideal solution (IS) and weights, a new A-IF programming model is constructed on the concept that the A-IF group inconsistency index should be minimized and must be not larger than the A-IF group consistency index by some fixed A-IFS. An effective method is developed to solve the new derived model. The distances of the alternatives to the fuzzy IS are calculated to determine their ranking order. Moreover, some generalizations or specializations of the derived model are discussed. Applicability of the proposed methodology is illustrated with a real supplier selection example.
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