Developing 3D hosts is one of the most promising strategies for putting forward the practical application of lithium(Li)-based anodes. However, the concentration polarization and uniform electric field of the traditional 3D hosts result in undesirable "top growth" of Li, reduced space utilization, and obnoxious dendrites. Herein, a novel dual-gradient 3D host (GDPL-3DH) simultaneously possessing gradient-distributed pore structure and lithiophilic sites is constructed by an electrospinning route.
View Article and Find Full Text PDFPoly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) are favorable for all-solid-state lithium metal batteries (ASSLBs) to ensure safety and enhance energy density. However, their narrow work windows and unstable electrode/electrolyte interfaces hinder their practical application in high-voltage ASSLBs. Although introducing additives in SPEs has been proven to be effective to address the above issues, it could hardly optimize both cathode and anode interfaces by an individual additive.
View Article and Find Full Text PDFComposite solid-state electrolyte (CSE) incorporated with fluorine-containing functional additives usually endows the assembled cell with improved electrochemical performance by forming stable electrode/electrolyte interfaces. However, most of fluorine-containing additives are prone to hydrolysis, which is not suitable for the large-scale preparation of CSEs. In this work, an antihydrolysis and fluorine-containing additive of magnesium 2,3,4,5,6-pentafluorophenylacetate (MgPFPAA) is successfully synthesized and then used to regulate the properties of the electrode/electrolyte interfaces of the all-solid-state lithium batteries (ASSLBs).
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries are regarded as one of the promising advanced energy storage systems due to their ultrahigh capacity and energy density. However, their practical applications are still hindered by the serious shuttle effect and sluggish reaction kinetics of soluble lithium polysulfides. Herein, g-CN nanosheets and graphene decorated with an ultrafine Co-species nanodot heterostructure (Co@g-CN/G) as separator coatings were designed following a facile approach.
View Article and Find Full Text PDFLithium (Li) metal is considered as one of the attractive anodes for next-generation high-energy-density batteries due to its ultrahigh theoretical specific capacity and low potential. However, many great challenges including uncontrolled dendrite growth and undesired side reactions during repeated cycling still seriously hinder its practical application in Li metal secondary batteries. Herein, we report the hexachloro-1,3-butadiene (HCBD) molecule as a functional additive to stabilize the Li anode by forming a stable solid electrolyte interface (SEI) layer with high Li ion conductivity via in situ surface and electrochemical reactions.
View Article and Find Full Text PDFPoly(ethylene oxide) (PEO)-based composite solid electrolytes (CSEs) are considered as one of the most promising candidates for all-solid-state lithium batteries (ASSLBs). However, a key challenge for their further development is to solve the main issues of low ionic conductivity and poor mechanical strength, which can lead to insufficient capacity and stability. Herein, β-cyclodextrin (β-CD) is first demonstrated as a multifunctional filler that can form a continuous hydrogen bond network with the ether oxygen unit from the PEO matrix, thus improving the comprehensive performances of the PEO-based CSE.
View Article and Find Full Text PDFThe sluggish redox kinetic and shuttle effect of polysulfides still obstruct the commercial application of lithium-sulfur (Li-S) batteries. Herein, a nanocomposite consisting of well-dispersed and lamellar-like shape CoS anchored on g-CN nanosheets (CoS@g-CN) is prepared firstly, and then it is integrated on a polypropylene membrane combined with little conductive Ketjen black (KB) to fabricate a multifunctional and quite thin interlayer, with a thickness of only ∼ 2.1 um and areal mass loading of ∼ 0.
View Article and Find Full Text PDFLithium sulfur (Li-S) batteries represent one of the most promising future power batteries due to their remarkable advantages of low cost and ultrahigh theoretical energy density. However, the commercial applications of Li-S batteries have long been plagued by the shuttling effect of polysulfides and sluggish redox kinetics of these species. Herein, we designed a novel battery separator coated by a europium oxide-doped porous Ketjen Black (EuO/KB) and tested its performance for the Li-S batteries for the first time.
View Article and Find Full Text PDFXanthinuria is a rare genetic metabolic disorder, the biochemical mechanism of xanthinuria is the disturbance of purine to uric acid metabolism due to the deficiency of xanthine dehydrogenase/xanthine oxidase (XDH/XO) and aldehyde oxidase 1 (AOX1). Xanthinuria has large clinical variability and only about half of all patients have urolithiasis. In this article, we present one xanthinuria case from an unrelated family, which diagnosed by clinical, biochemical and finally confirmed by molecular genetics.
View Article and Find Full Text PDFA green route modulated by the addition of CaCl during the potassium compound-assisted synthesis is developed for the first time for the synthesis of nitrogen-rich hierarchical porous carbon (NRHPC) with high external surface area and moderate total pore volume. The NRHPCN constructed by nanosheets is capable of simultaneously achieving high gravitational and volumetric capacity for supercapacitors (SCs).
View Article and Find Full Text PDFA Co(II)-catalyzed pyridyl C-H bond carbenoid insertion with α-diazoacetates has been realized. This transformation features a highly regioselective C-C bond formation at the C3-position of pyridines, providing an efficient access to diverse α-aryl-α-pyridylacetates.
View Article and Find Full Text PDFNitrogen-doped porous carbons have been extensively investigated to improve the specific capacitance in aqueous electrolytes by increasing the specific surface area and nitrogen content and by optimizing the pore structure. However, research on the effect of electrolyte cations on the specific capacitance of these materials is rare, especially for neutral electrolytes. Herein, a nitrogen-rich hierarchically porous carbon (NRHPC) with a high nitrogen content of 12.
View Article and Find Full Text PDFZn(OAc)-catalyzed highly regioselective carbonylacetylation of indoles and pyrroles with α-diazoketones has been developed. This transformation involves a combination of Wolff rearrangement/cross-coupling relay and provides an efficient approach to versatile 3-carbonylacetylindoles and 2-carbonylacetylpyrroles with a broad range of functional group tolerance.
View Article and Find Full Text PDFTo overcome the problems faced by TiO materials for lithium-ion batteries usage, such as easy nanoparticles agglomeration during cycling and poor cycling performance, in this study, TiO nanorods with the controlled phase compositions are prepared via direct pyrolysis of single molecule precursors in combination with a simple washing process. By tuning the external cations in the single source precursors, three TiO samples in a nanorod shape with the compositions of pure anatase, anatase-rutile dual phase, and anatase-TiO(B) dual phase are synthesized successfully. High-resolution transmission electron microscopy, X-ray powder diffraction, and Raman measurements confirm the phase structures and compositions of the three prepared samples.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2017
Carbon-encapsulated Sn@N-doped carbon tubes with submicron diameters were obtained via the simple reduction of C@SnO@N-doped carbon composites that were fabricated by a hydrothermal approach. Sn nanoparticles encapsulated in carbon layers were distributed uniformly on the surfaces of the N-doped carbon nanotubes. The electrochemical performances of the composites were systematically investigated as anode materials in sodium-ion batteries (SIBs).
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2017
An novel exfoliation strategy to few-layered graphene (FLG) combined with in situ synthesized amorphous MnO has been established via a facile and robust ball milling route in the presence of KMnO. The facile synthesis approach has the features of low cost, environmentally friendly nature and scalable capability. As an anode for lithium-ion batteries, amorphous MnO@FLG delivered a wonderful electrochemical performance under extremely operational conditions, that is, an excellent reversible capacity of 856 mAh g at a high current density of 1 A g after 75 cycles under a high temperature of 85 °C.
View Article and Find Full Text PDFA nanocomposite of ultrafine anatase nanoparticles (<5 nm) embedded N-doped carbon (TiO-NPs/NC) with a relatively low specific surface area was successfully synthesized by in situ pyrolysis of a new and cheap single source precursor of (Hen)[Ti(O)(Hcit)(cit)]·12HO (en = ethylenediamine and Hcit = citric acid) under 550 °C and an inert atmosphere. The precursor in crystalline state was isolated from an aqueous solution containing of titanium butoxide, citric acid, hydrogen peroxide, and ethylenediamine and was characterized. The crystal structure was determined by X-ray single crystal diffraction.
View Article and Find Full Text PDFA cobalt(II)-catalyzed regioselective aryl C-H bond oxygenation between arenes and aryl or aliphatic carboxylic acids under bidendate-chelation assistance is developed. This method provides an efficient approach to acyoxy-substituted arenes with a broad range of functional group tolerance. Furthermore, this reaction system could be further applied to the preparation of polyfunctional naphthylenes.
View Article and Find Full Text PDFA Rh(III)-catalyzed carboamination of alkynyl cycloalkanols with arylamines has been developed. This transformation involves a novel Csp-H/Csp-Csp activation relay and provides an efficient approach to versatile 1,2,3-trisubstituted indoles with a broad range of functional group tolerance.
View Article and Find Full Text PDFAn Ir(iii)-catalyzed relay aryl C-H bond carbenoid insertion cascade of N-aryl-2-pyridinamines with diazo Meldrum's acid has been developed. This method provides an efficient approach to multifunctionalized 1,3-dihydroindol-2-ones with a broad range of functional group tolerance. Furthermore, this protocol could be applied for the concise synthesis of bioactive hematopoietic growth factor analogues.
View Article and Find Full Text PDFA Co(III)-catalyzed [4 + 1] cycloaddition of 2-arylpyridines or 2-alkenylpyridines with aldehydes through Csp(2)-H bond activation has been developed. This protocol provides a facile approach to structurally diverse indolizines including benzoindolizines with a broad range of functional group tolerance.
View Article and Find Full Text PDFCopper(I)-catalyzed 5-sulfonation of quinolines via bidentate-chelation assistance has been developed. The reaction is compatible with a wide range of quinoline substrates and arylsulfonyl chlorides. Experimental and theoretical (DFT) investigation implicated that a single-electron-transfer process is involved in this sulfonylation transformation.
View Article and Find Full Text PDFThe Rh(III)-catalyzed regioselective C2-H bond carbenoid insertion/cyclization of N-amidoindoles with α-acyl diazo compounds has been developed. This method provides a novel approach to 2H-pyrimido[1,6-a]indol-1-ones with a broad range of functional group tolerance. The synthetic utilities of the approach are demonstrated by versatile chemical transformations.
View Article and Find Full Text PDFA Rh(iii)-catalyzed cross-coupling/cyclization cascade of α-imino Csp(3)-H bonds with donor/acceptor α-acyl diazocarbonyl compounds has been developed. This novel transformation involves ligand-directed Csp(3)-H bond functionalization with carbenoids under the pyridine-chelation assistance, and offered an efficient access to synthetically versatile polysubstituted N-(2-pyridyl)pyrroles with a broad range of functional group tolerance.
View Article and Find Full Text PDFAn efficient one-pot and transition-metal-free chlorocyclization cascade of 2-aminopyridines with aliphatic carboxylic acids is reported. This transformation provides a novel approach to 2-chloro- or 3-chloro-substituted imidazo[1, 2-α]pyridines with a broad range of substrate scopes.
View Article and Find Full Text PDF