The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising propert...The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising properties of ethylene oxide-based electrolytes,their typical clamp-like coordination geometry leads to crowd solvation sheath and overly strong interactions between Li^(+)and electrolytes,rendering difficult dissociation of Li+and unfavorable solid electrolyte interface(SEI).Herein,we explore weakly solvating characteristics of polyacetal electrolytes owing to their alternately changing intervals between–O–coordinating sites in the main chain.Such structural asymmetry leads to unique distorted helical solvation sheath,and can effectively reduce Li^(+)-electrolyte binding and tune Li^(+)desolvation kinetics in the insitu formed polymer electrolytes,yielding anion-derived SEI and dendrite-free Li electrodeposition.Combining with photoinitiated cationic ring-opening polymerization,polyacetal electrolytes can be instantly formed within 5 min at the surface of electrode,with high segmental chain motion and well adapted interfaces.Such in-situ polyacetal electrolytes enabled more than 1300-h of stable lithium electrodeposition and prolonged cyclability over 200 cycles in solid-state batteries at ambient temperatures,demonstrating the vital role of molecular structure in changing solvating behavior and Li deposition stability for high-performance electrolytes.展开更多
PSMD14 played a vital role in initiation and progression of hepatocellular carcinoma(HCC).However,PSMD14 and its-related genes for the immune prognostic implications of HCC patients have rarely been analyzed.Messenger...PSMD14 played a vital role in initiation and progression of hepatocellular carcinoma(HCC).However,PSMD14 and its-related genes for the immune prognostic implications of HCC patients have rarely been analyzed.Messenger RNA expression profiles and clinicopathological data were downloaded from The Cancer Genome Atlas(TCGA)and International Cancer Genome Consortium(ICGC)database-Liver Hepatocellular Carcinoma(LIHC).Additionally,we used multi-dimensional bioinformatics analysis to construct and validate a PSMD14-based immune prognostic signature(including RBM45,PSMD1,OLA1,CCT6A,LCAT and IVD)for HCC prognosis prediction.Patients in the high-risk group shown significantly poorer survival than patients in the low-risk group.Calibration curves confirmed the good consistency between the clinical nomogram prediction and the actual observation.Gene set enrichment analyses(GSEA)revealed several significantly enriched pathways,which might help explain the underlying mechanisms.Besides,the rt-PCR further validates the expression of seven immune genes in HCC cells.Our study identified a novel PSMD14-based signature for HCC prognosis prediction,it provided new potential prognostic biomarkers and therapeutic targets for immunotherapy of HCC.展开更多
A porous polymeric ligand(PPL)has been synthesized and complexed with copper to generate a heterogeneous catalyst(Cu@PPL)that has facilitated the efficient C-N coupling with various(hetero)aryl chlorides under mild co...A porous polymeric ligand(PPL)has been synthesized and complexed with copper to generate a heterogeneous catalyst(Cu@PPL)that has facilitated the efficient C-N coupling with various(hetero)aryl chlorides under mild conditions of visiblelight irradiation at 80°C(58 examples,up to 99%yields).This method could be applied to both aqueous ammonia and substituted amines,and is compatible to a variety of functional groups and heterocycles,as well as allows tandem C-N couplings with conjunctive dihalides.Furthermore,the heterogeneous characteristic of Cu@PPL has enabled a straightforward catalyst separation in multiple times of recycling with negligible catalytic efficiency loss by simple filtration,affording reaction mixtures containing less than 1 ppm of Cu residue.展开更多
基金financially supported by National Natural Science Foundation of China(52003231,22065037)Yunnan Fundamental Research Projects(202201AW070015)。
文摘The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising properties of ethylene oxide-based electrolytes,their typical clamp-like coordination geometry leads to crowd solvation sheath and overly strong interactions between Li^(+)and electrolytes,rendering difficult dissociation of Li+and unfavorable solid electrolyte interface(SEI).Herein,we explore weakly solvating characteristics of polyacetal electrolytes owing to their alternately changing intervals between–O–coordinating sites in the main chain.Such structural asymmetry leads to unique distorted helical solvation sheath,and can effectively reduce Li^(+)-electrolyte binding and tune Li^(+)desolvation kinetics in the insitu formed polymer electrolytes,yielding anion-derived SEI and dendrite-free Li electrodeposition.Combining with photoinitiated cationic ring-opening polymerization,polyacetal electrolytes can be instantly formed within 5 min at the surface of electrode,with high segmental chain motion and well adapted interfaces.Such in-situ polyacetal electrolytes enabled more than 1300-h of stable lithium electrodeposition and prolonged cyclability over 200 cycles in solid-state batteries at ambient temperatures,demonstrating the vital role of molecular structure in changing solvating behavior and Li deposition stability for high-performance electrolytes.
基金the National Natural Science Foundation of China(81772995 and 81472266)the Excellent Youth Foundation of Jiangsu Province,China(BK20140032)Jiangsu Province’s Key Provincial Talents Program(ZDRCA2016090).
文摘PSMD14 played a vital role in initiation and progression of hepatocellular carcinoma(HCC).However,PSMD14 and its-related genes for the immune prognostic implications of HCC patients have rarely been analyzed.Messenger RNA expression profiles and clinicopathological data were downloaded from The Cancer Genome Atlas(TCGA)and International Cancer Genome Consortium(ICGC)database-Liver Hepatocellular Carcinoma(LIHC).Additionally,we used multi-dimensional bioinformatics analysis to construct and validate a PSMD14-based immune prognostic signature(including RBM45,PSMD1,OLA1,CCT6A,LCAT and IVD)for HCC prognosis prediction.Patients in the high-risk group shown significantly poorer survival than patients in the low-risk group.Calibration curves confirmed the good consistency between the clinical nomogram prediction and the actual observation.Gene set enrichment analyses(GSEA)revealed several significantly enriched pathways,which might help explain the underlying mechanisms.Besides,the rt-PCR further validates the expression of seven immune genes in HCC cells.Our study identified a novel PSMD14-based signature for HCC prognosis prediction,it provided new potential prognostic biomarkers and therapeutic targets for immunotherapy of HCC.
基金the National Natural Science Foundation of China(21704016,21971044)。
文摘A porous polymeric ligand(PPL)has been synthesized and complexed with copper to generate a heterogeneous catalyst(Cu@PPL)that has facilitated the efficient C-N coupling with various(hetero)aryl chlorides under mild conditions of visiblelight irradiation at 80°C(58 examples,up to 99%yields).This method could be applied to both aqueous ammonia and substituted amines,and is compatible to a variety of functional groups and heterocycles,as well as allows tandem C-N couplings with conjunctive dihalides.Furthermore,the heterogeneous characteristic of Cu@PPL has enabled a straightforward catalyst separation in multiple times of recycling with negligible catalytic efficiency loss by simple filtration,affording reaction mixtures containing less than 1 ppm of Cu residue.