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Modifying separator with metal oxides has been considered as a strong strategy to inhibit the shuttling of soluble polysulfide in the lithium-sulfur battery (Li-S battery). Manganese dioxide (MnO2), one kind of transition metal oxide, is widely applied to decorate the PP (Polypropylene) separator. However, the fabrication by physical coating is always multistep and complicated. Here, we design a simple and fast method to chemically decorate separator. Based on the oxidizing property of acidic KMnO4 solution, the PP separator was oxidized and an ultrathin self-assembled MnO2 layer was directly constructed on one side of separator, by immersing in acidic KMnO4 solution for only 1 h. The self-assembled MnO2 layer has the synergistic effect of adsorption and catalytic conversion on polysulfides, which can effectively inhibit the shuttle effect. It can also help battery to maintain excellent electrochemical kinetics in the electrochemical cycle and maintain the effective recycling of active substances. As a result, the shuttling of polysulfide is greatly prohibited by this novel functional separator, and cycling stability is outstandingly improved, with a low-capacity decaying of 0.058% after 500 cycles at 0.5C. The rapid and simple modification method proposed in this study has a certain reference value for the future large-scale application of lithium-sulfur battery.

As a secondary Li-ion battery with high energy density, lithium-sulfur (Li-S) batteries possess high potential development prospects. One of the important ingredients to improve the safety and energy density in Li-S batteries is the solid-state electrolyte. However, the poor ionic conductivity largely limits its application for the commercial market. At present, the gel electrolyte prepared by combining the electrolyte or ionic liquid with the all-solid electrolyte is an effective method to solve the low ion conductivity of the solid electrolyte. We present a cross-linked gel polymer electrolyte with fluoroethylene carbonate (FEC) as a solid electrolyte interface (SEI) film formed for Li-S quasi-solid-state batteries, which can be simply synthesized without initiators. This gel polymer electrolyte with FEC as an additive (GPE@FEC) possesses high ionic conductivity (0.830 × 10-3 S/cm at 25 °C and 1.577 × 10-3 S/cm at 85 °C) and extremely high Li-ion transference number (tLi+ = 0.674). In addition, the strong ability toward anchoring polysulfides resulting in the high electrochemical performance of Li-S batteries was confirmed in GPE@FEC by the diffusion experiment, X-ray photoelectron spectroscopy analysis (XPS), and scanning electron microscopy (SEM) mapping of the S element. Such a high ion conductivity (IC) gel polymer electrolyte enables a competitive specific capacity of 940 mAh/g at 0.2C and supreme cycling performance for 180 cycles at 0.5C, which is far beyond that of conventional poly(ethylene oxide)-based quasi-solid-state Li-S batteries.

Soil salinisation is an important factor limiting the cultivation and distribution of Prunus mume. Therefore, identifying the regulation mechanism of salt tolerance of P. mume will promote its cultivation and molecular breeding. In this study, the garden tree species P. mume ‘Meiren’ was investigated, with a soil NaCl content (w/w) of 0.3%. Photosynthetic gas exchange parameters, relative electrical conductivity, malondialdehyde, osmoregulation substances, and antioxidant enzyme activity were measured in the early (3d), middle (10d), and late (30d) stages of stress. Salt treatment was applied for 0 h, 6 h, 24 h, and 72 h; following this, the gene library was constructed from the leaves. The results showed that the CBL-CIPK, mitogen-activated protein kinase, calcium-dependent protein kinase, and abscisic acid signalling pathways were involved in salt stress signal transduction of P. mume. Furthermore, bHLH, WRPK, ERF, and MYB were identified as potential key transcription factor families of salt tolerance in P. mume. Combined with determined physiological responses, the results showed that early salt stress inhibited the activities of RuBisCO, chlorophyll synthase, glutamyl tRNA reductase, divinyl reductase, and magnesium chelatase; resultantly, this led to a reduction in the photosynthetic rate. Also, it was found that P5CS, SS, LEA, and dehydrin regulated the synthesis of proline, soluble sugar, and macromolecular protein to alleviate osmotic stress. POD gene plays an important role in scavenging reactive oxygen species due to its regulation of POD activity. The findings of this research reveal the internal mechanism of the physiological response and provide a foundation for the construction of a genetic regulatory network in response to salt stress in P. mume.

A binder is an important component in lithium-ion batteries and plays a significant role in maintaining the properties of active substances. Most studies in the field of binders have only focussed on physical properties such as bonding performance. Here, a polyacrylic acid-modified binder was designed and adapted to Li[Ni0.8Co0.1Mn0.1]O2, which enhanced the electrochemical stability of Li[Ni0.8Co0.1Mn0.1]O2 from 30.2 to 66.6% (300 cycles at 1 C). We for the first time discovered that this was caused by a chemical reaction between polyacrylic acid and the residual lithium on the surface during the cycling, which formed a lithium propionic acid coating layer and maintained the stability of the layered structure.

Phenyl-1,2-benzoselenazol-3(2H)-one (ebselen) is a classical mimic of glutathione peroxidase (GPx). Thioredoxin interaction endows ebselen attractive biological functions, such as antioxidation and anti-infection, as well as versatile therapeutic usage. Accordingly, application of ebselen analogues in biosensing, chemical labeling, imaging analysis, disease pathology, drug development, clinical treatment, etc. have been widely developed, in which mercaptans, reactive oxygen species, reactive sulfur species, peptides, and proteins were involved. Herein, focusing on the application of ebselen-agents in biochemistry, we have made a systematic summary and comprehensive review. First, we summarized both the classical and the innovative methods for preparing ebselen-agents to present the synthetic strategies. Then we discussed the full functional applicability of ebselen analogues in three fields of biochemical analysis including the fluorescence sensing and bioimaging, derivatization for high throughput fluorescence analysis, and the labeling gents for proteomics. Finally, we discussed the current challenges and perspectives for ebselen-agents as analytical tools in biological research. By presenting the multifunctional applicability of ebselen, we hope this review could appeal researchers to design the ebselen-related biomaterials for biochemical analysis.

Recycling and reusing spent graphite have become urgent tasks, with massive numbers of lithium-ion batteries (LIBs) from hybrid electric vehicles (HEVs)/electric vehicles (EVs) retired every year. Meanwhile, interlayer designs based on carbon materials have attracted widespread attention to suppress the polysulfide shuttle effect in high-energy-density lithium–sulfur (Li–S) batteries. Nevertheless, designing simple and low-cost carbon-derived interlayers still remains a great challenge. Spent graphite possesses a porous structure, defects, and polar functional groups that were formed in situ, which can significantly confine polysulfides through a combination of physical and chemical adsorption. Meanwhile, transition metals introduced due to the dissolution of cathode active materials can also anchor polysulfides via S–TM bonding, as well as improving electrical conductivity and boosting polysulfide conversion kinetics. Herein, spent graphite recycled from waste LIBs was employed for the first time as a functional interlayer for Li–S batteries based on its intrinsic properties. The spent-graphite-derived interlayer exhibited remarkably enhanced trapping and catalytic performance toward polysulfides. A high discharge capacity of 968 mA h g−1 with a low decay rate of 0.08% per cycle over 500 cycles at 1 C can be obtained. The present work not only provides a promising strategy for the design of interlayers, but it also shows a high-value application of spent graphite.

Interactions between microorganisms and clay minerals influence the transport and cycling of metal contaminants in both marine and terrestrial environments. The present study was conducted to quantify the adsorption of dissolved cadmium, Cd(II), under seawater-like conditions to the marine cyanobacterium Synechococcus sp. PCC 7002, three common clay minerals (kaolinite, montmorillonite and illite), as well as cell-clay aggregates. We show here that the Synechococcus-only experiments removed the most Cd above pH 5.5, followed in decreasing order by aggregates of 50% cells:50% individual clays, aggregates of cells and all 3 clays, and individual clays. Electron microscope imaging showed that clays associated in a tangential edge-on orientation to the cells in Synechococcus-clay mineral aggregates. A non-electrostatic surface complexation modeling approach was used to fit Cd adsorption onto Synechococcus cells and individual clay minerals. The resulting Cd binding constants were then used in consort with surface functional group pKa values and site concentrations to accurately predict the extent of Cd adsorption onto the Synechococcus-clay mineral aggregates using the component additivity (CA) approach. We observed that the addition of cyanobacterial cells to clay mineral suspensions led to significantly larger mean aggregate sizes of clay minerals, enhancing the clay sedimentation rate. Although specifically focused on Cd, our study indicates that the ratio of bacterial plankton to clay minerals is an important determinant in terms of understanding the rate with which metals are transferred from the water column to the seafloor.

The increased application of layered oxide (LiCoO2) lithium ion batteries (LIBs) for electronic products will result in lots of spent layered cathodes in the near future. Furthermore, the explorati...

A palladium(II)-catalyzed direct 2-arylation of indoles by tetraarylstannanes with oxygen (balloon) as the oxidant at room temperature has been developed. Various tetraarylstannanes can be employed as aryl sources for 2-arylation of indoles in up to 89% yield, providing a practical and efficient catalytic protocol for accessing 2-arylindoles.

Biological functions of chondroitin sulfate, including anti-oxidation and anti-inflammation, are associated with its molecular weight. This study aimed to evaluate the correlation between antioxidant activity and molecular weights of chondroitin sulfate derived from bovine nasal cartilage (BCS). BCS extracted by compound enzymatic method was further purified via DEAE-cellulose column separation to obtain BCS-II (129.4 kDa), which was further degraded by H2O2-Vc to obtain four subfractions: BCS-II-1 (92.7 kDa), BCS-II-2 (54.1 kDa), BCS-II-3 (26.3 kDa), and BCS-II-4 (19.7 kDa). Changes in the physicochemical properties of BCS-II before and after degradation were compared via FT-IR, NMR and monosaccharide composition analysis. Finally, antioxidant activities of BCS-II and its subfractions BCS-II-1–4 were compared. Our results showed that the H2O2-Vc system did not disrupt the primary functional group of BCS-II, with no significant change in sulfate content between BCS-II and its degraded fractions; however, uronic acid levels increased in degraded fractions when compared with BCS-II. In vitro, BCS-II-4 displayed the lowest molecular weight and had the strongest antioxidant activity. Therefore, the antioxidant activity of chondroitin sulfate in vitro is robustly associated with its molecular weight, and low-molecular-weight chondroitin sulfate can be used as an antioxidant in the food and pharmaceutical industries and other sectors.

Iridium-catalyzed oxidative o-alkenylation of benzylamines with acrylates was enabled by the directing group pentafluorobenzoyl (PFB). Density functional theory calculations were performed to explore the detailed reaction mechanism. The calculated results reveal that N-deprotonation prior to C–H activation is favored over direct C–H activation. Moreover, C–H activation is reversible and not the rate-determining step, which has been supported by the experimental observation. The regio- and stereoselectivity of ethyl acrylate insertion are controlled by the steric effect and the carbon atom with a larger orbital coefficient of the π* antibonding orbital in the nucleophilic attack, respectively. The migratory insertion of ethyl acrylate is computationally found to be rate-determining for the whole catalytic cycle. Finally, the seven-membered ring intermediate IM11 undergoes a sequential N-protonation and β-H elimination with the assistance of AcOH, rather than β-H elimination and reductive elimination proposed experimentally, to afford the o-alkenylated product. IM11 is unable to directly cyclize through C–N reductive elimination because both sp3-hybridized N and C atoms are unfavorable for N–C reductive elimination. The origin of the directing group PFB preventing the product and intermediates undergoing aza-Michael addition has been explained.

The Ni(0)-catalyzed coupling of benzimidazole with 1,1-disubstituted allenes represents a new strategy for achieving controllable C–H allylations, alkenylations and dienylations. To understand the detailed mechanisms and origins of the switchable selectivities, density functional theory (DFT) calculations were conducted. The results using a tBu-substituted allene demonstrate that the formation of the allylated product involves a Ni-catalyzed C–H activation mechanism through ligand-to-ligand-hydrogen transfer (LLHT) under base-free conditions. In contrast, a Ni/NaOtBu co-promoted C–H activation mechanism is newly proposed in the presence of NaOtBu, which is remarkably different from the previously reported literature. The novel mechanism emphasizes that NaOtBu abstracts the Ni-activated heterocyclic (ipso-C)H atom followed by turnover limiting Ni slippage, and subsequently the allylated product is generated after alkene insertion and protonation. The strong electrostatic attraction between Ni and heterocyclic ipso-C in the Ni slippage pre-intermediate is critical for facilitating the Ni slippage. Once formed, the allylated product, assisted by NaOtBu, further evolves into a more stable alkenylated isomer. Employing a (tert-butyldimethylsilyl)-ether substituted allene as the substrate, the NaOtBu-induced chemoselectivity for dienylation vs. alkenylation was also probed and it was found that the O(tBu)–H⋯O(Si) hydrogen bonding interaction in the C–O(Si) cleavage pre-intermediate remarkably weakens the adjacent C–O(Si) σ-bond, thereby resulting in an exclusive C–O(Si) cleaved dienylation product. Further theoretical predictions suggest that the chemoselectivity might be reversed by replacing tBu in NaOtBu by the withdrawing C(CF3)3 group.

Background: DNA sensors are innate immune receptors that detect intracellular endogenous or exogenous DNA. They are critical to trigger immune response against DNA viral and intracellular bacterial infection, and are involved in inflammatory diseases and tumorigenesis. Recent accumulating evidences indicated that DNA sensors are also crucial for controlling the development of colorectal cancer (CRC). However, a systematic study on the expression profile of DNA sensors in CRC and their clinical significance are still lacking. Methods: We investigated the expression profile of DNA sensors in CRC and their clinical significance by taking advantage of clinical CRC samples, mouse AOM/DSS treatment model, and Oncomine ® bioinformatics platform. Results: Our study identified that the expression of DNA sensors, including AIM2, DAI, as well as inflammasome molecules ASC/IL-18, TLR9 and adaptor MyD88, and DDX60 decreased in human CRC, whereas the expression of DHX9, DHX36, and DDX41 significantly increased. Among them, the expression of AIM2/ASC/IL-18, MyD88, DAI, DHX36, and DDX60 were associated with cancer stages. In addition, we also performed correlation analysis between DNA sensors and their main signaling molecules to explore the possible mechanisms. The results showed that there were positive correlations between AIM2 and ASC/IL-18, DHX9 and MAVS, and TLR9 and MyD88 expression. In addition, the gene expression patterns of some DNA sensors were confirmed by Western-blot analysis. Conclusions: Our study revealed that the expression of multiple DNA sensors was deregulated in CRC and might be involved in tumor development. More importantly, the study identified that, among all these DNA sensors, AIM2, DAI, and DDX60 could be potentially critical for diagnosis, prognosis, and therapy of CRC and deserve further investigation.

In practice, high fidelity fluorescence imaging in vivo faces many issues, for example: (1) the fluorescence background of the probe is bleached by the wide intensity scale of fluorescence microscopy, displaying an inherent false negative background (FNB); and (2) the dosage of the probe has to be increased to achieve sufficient intensity for in vivo imaging, causing a vicious cycle that exacerbates the FNB. Herein, we constructed a fluorophore (F)–electron donor (D)–electron regulator (R) system, and thereby developed a dual modulation strategy for the de novo design of high fidelity probes. Using cross-talk modulation, the probe allows: (1) enhanced ESET (excited state electron transfer) from F to D, which minimizes the inherent FNB based on synergistic PET (photo induced electron transfer); and (2) the inhibition of PET and weakening of ESET from F to D to maximize the reporting intensity to further reduce the FNB, which is additionally enhanced by an overdose of the probe. To test the implementation, we constructed a 7-hydroxy-2-oxo-2H-chromene-3-carbaldehyde (HPC) series of probes, with HPC (F) as the fluorophore, 2-hydrazinylpyridine, which was screened as an electronically adjustable donor (D), and electronic regulators (R). In particular, HPC-7 and HPC-8 provided cell/zebrafish imaging with negligible background even using the rather low fluorescence scale of microscopy (a region for revealing hidden background). Interestingly, with the specificity of HPC for reporting zinc, we achieved probe HPC-5, which possesses both an ultralow inherent FNB and optimal reporting intensity for tissue and in vivo imaging, enabling the in vivo imaging of zinc in mice for the first time. Under this high-fidelity mode, the fluorescence monitoring of zinc ions during the development of liver cancer in mice was successfully performed. We envision that the dual modulation strategy with the F–D–R system could provide a useful concept for the de novo design of practical probes., We engineered a cross-talk electron transfer strategy using an F–D–A system to reduce the false negative background for high fidelity imaging in vivo.

In order to determine trace impurities in the nuclear grade UF4, an analysis method based on the standard addition and 103Rh internal standardization techniques combined with ICP-MS has been established. The examination tests, including comparison with the quantity of trace impurities assigned in a certified reference uranium oxide and determination of the standard addition recovery, were performed to validate the accuracy and precision of the method. Total 42 trace impurity elements from Li to Bi were determined, with the method detection limit for the 42 impurities were found in the range of 0.0004–0.072 μg g−1. The recoveries were varied from 92% to 111%, and the relative deviations for most of the impurity elements were less than 10%. The method has been verified to meet the requirements of quality control for the UF4 and will be used in the molten salt reactor.

A novel efficient photoelectrochemical (PEC) sensor was assembled for curcumin (Cur) detection using 2-mercaptoacetic acid (TGA)-capped CdTe nanoparticles and nickel tetra-amined phthalocyanine-linked graphene oxide (TGA-CdTe@NiTAPc-Gr). The TGA-CdTe nanoparticles could be firmly immobilized on the thin film structure of NiTAPc-Gr in a hydrogen-bonded manner, thus producing the proposed PEC sensor with a high photoelectrochemical activity of TGA-CdTe nanoparticles and excellent stability of NiTAPc-Gr. The TGA-CdTe@NiTAPc-Gr thin film showed a stronger blue light absorption property than the individual precursors, and this resulted in the sensitive detection of Cur ranging from 0.25–100 μM with a detection limit of 12.50 nM. In addition, the PEC sensor exhibited a high sensitivity and selectivity and quite good reproducibility. Thus, it shows potential for Cur detection in real samples.

The mechanism of ruthenium-catalyzed [4 + 1] annulation of benzamide and propargyl alcohol has been investigated by density functional theory calculations. The reaction undergoes N–H and C–H deprotonations by a concerted metalation-deprotonation mechanism to afford a 5-membered ruthenacyclic species, which then undergoes ring expansion by alkyne insertion to deliver a 7-membered ring intermediate. Our study focused on how the successive hydrogen migrations take place that remains unclear. The 1,2-proton migration and 1,3-proton transfer from O to C are successively finished by using acetate anion as a shuttle (a stepwise process). In contrast to the experimental proposal that the reaction experiences a Ru(II)–Ru(0)–Ru(II) transformation, our study unveiled a Ru(II)–Ru(IV)–Ru(II) transformation in the reaction. In addition, our calculations suggested that the EtO–N bond cleavage rather than the C–H activation is likely to be the rate-determining step for the entire reaction, which is not in contradiction w...

The gold(iii)-catalyzed annulations of alkynes with anthranils were evaluated using DFT calculations. A unified rationale for the Br-migration on α-imino gold(iii)-carbene was proposed, from which an unprecedented "N-donation/abstraction substitution" mechanism was established using the substituted anthranils, while direct C-H nucleophilic attack was involved with the unsubstituted anthranils. The controlling factors guiding the site-selectivity were uncovered. These computational studies provide insight for developing new α-imino gold(iii)-carbene mediated reactions.

To evaluate the effects of astragaloside on the proliferation, invasion, migration and apoptosis of nonsmall cell lung cancer A549 cells and phosphatidylinositol 3-kinase/protein kinase B/mechanistic target of rapamycin pathway. After A549 cells were treated with 0, 10, 20, 40, 60, 80 and 100 μmol/l astragaloside for 24 h, the survival rate was measured by methyl thiazolyl tetrazolium assay and the half maximal inhibitory concentration was calculated. Astragaloside at half maximal inhibitory concentration was added. Cell invasion, migration and apoptosis were detected by transwell assay, wound healing assay and flow cytometry, respectively. The effects of astragaloside on the expressions of phosphatidylinositol 3-kinase/protein kinase B/mechanistic target of rapamycin pathway-related proteins were detected by western blotting. After different concentrations of astragaloside were added, cell proliferation declined with increasing concentration. Half maximal inhibitory concentration against A549 cell proliferation was 32.2 μmol/l. Compared with blank control group; cell proliferation; invasion and migration were significantly weakened, while apoptosis was enhanced in astragaloside group. The expressions of phosphorylation of phosphatidylinositol 3-kinase, phosphorylation of protein kinase B and phosphorylation of mechanistic target of rapamycin proteins in astragaloside group were significantly lower than those in blank control group. Astragaloside inhibits the proliferation, invasion and migration, and promotes the apoptosis of nonsmall cell lung cancer A549 cells dose-dependently. Inhibiting phosphorylation of phosphatidylinositol 3-kinase, phosphorylation of protein kinase B and phosphorylation of mechanistic target of rapamycin expressions in the phosphatidylinositol 3-kinase/protein kinase B/mechanistic target of rapamycin pathway may be one of the mechanisms of astragaloside.

Vanillin is widely used as a flavor enhancer and is known to have numerous other interesting properties, including antidepressant, anticancer, anti-inflammatory, and antioxidant effects. However, as excess vanillin consumption can affect liver and kidney function, simple and rapid detection methods for vanillin are required. Herein, a novel electrochemical sensor for the sensitive determination of vanillin was fabricated using an iron phthalocyanine (FePc)-based metal–organic framework (MOF). Scanning electron microscopy and transmission electron microscopy showed that the FePc MOF has a hollow porous structure and a large surface area, which impart this material with high adsorption performance. A glassy carbon electrode modified with the FePc MOF exhibited good electrocatalytic performance for the detection of vanillin. In particular, this vanillin sensor had a wide linear range of 0.22–29.14 μM with a low detection limit of 0.05 μM (S/N = 3). Moreover, the proposed sensor was successfully applied to the determination of vanillin in real samples such as vanillin tablets and human serum.

The structure of chondroitin sulfate oligosaccharides (CSOs), especially their sulfation pattern, has been found to be closely related with many biological pathways and diseases. However, detailed functional analysis such as their interaction with glycan binding proteins (GBPs) has been lagging, presumably due to the unavailability of well-defined, diverse structures. Besides challenging chemical and enzymatic synthesis, this is also due to the challenges in their purification at the isomer level and structural analysis owing to their instability, structural complexity, and low mass spectrometry detection sensitivity. Herein, we first used recycling preparative HPLC to separate and purify shark CS tetrasaccharide component labeled by a bifunctional fluorescent linker 2-amino-N-(2-aminoethyl)benzamide (AEAB) at the isomer level. Then, each isomer was derivatized through a multistage procedure including N-acetylation, carboxyl amidation, permethylation, and desulfation with silylating reagent. Structural analysis of each derivatized isomer was performed with ESI-MSn in positive ion mode. A total of 16 isomers of CSO-AEAB were isolated, with a minimum mass component of 0.007 mg and a maximum mass component of 17.53 mg, of which 10 isomers (>90 μg) were structurally analyzed. This preparation and structure analysis of CSOs lay the foundation for further study of the structure-activity relationship of CSOs.

Anammox-based processes and microbial consortia have drawn extensive attention for their use in high-efficiency wastewater treatment technologies. Metals substantially affect the activity of anammox consortia and the quality of wastewater treatment plant effluent. Here, we explored the role of anammox consortia in terms of metals complexation in both single and multi-metal systems. Adsorption edges of single metal cations indicate that the adsorption preference was in the order: Pb(II) > Cd(II) > Cr(VI). A competitive effect was observed in multi-metal cations systems, with Pb(II) being preferably adsorbed and the degree of adsorption somewhat reduced in the presence of either Cd(II) or Cr(VI), while Cd(II) and Cr(VI) were easily exchanged and substituted by other metals. Fourier transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS) further suggest that the adsorption of Pb(II) and Cd(II) are as inner-sphere ion-exchange mechanisms, while Cr(VI) adsorption is mainly by outer-sphere complexation. Density functional theory (DFT) calculations highlight that Cd(II) and Pb(II) have different binding sites compared to Cr(VI), and the order of binding energy (Ebd) of three metal cations were Pb(II) > Cd(II) > Cr(VI). These calculations support the adsorption data in that Pb forms more stable complexes with anammox bacterial surface ligands. Surface complexation modelling (SCM) further predicted both the sorption of single metal cations and competitive adsorption of the three metals to anammox consortia, the exception being Cd at higher loadings. The results of this study highlight the potential role of anammox consortia in removing metal cations from wastewater in treatment systems.

Organisms have built up immunological systems, where mitochondrial SO2 plays conflicting roles in regulating cell apoptosis. However, no exploration on the influence and regulating principle of mitochondrial SO2 to the specific apoptosis type can be found, which brings about a challenge to fluorescent probes. Herein, we optimize the fluorophore and develop a new fluorescent probe FHMI ((E)-4-(3-formyl-4-hydroxystyryl)-1-methylpyridin-1-iumiodide) by equipping an ICT (intramolecular charge transfer) fluorophore HMII ((E)-4-(4-hydroxystyryl)-1-methylpyridin-1-ium iodide) with an aldehyde group that serves as both fluorescence quencher and reporting group. After the optimization, although the nonconjugated electron donor is formed when sensing SO2, the preset ICT fluorophore HMII is permitted to release the fluorescence at the enlarged wavelength. Compared with the traditional design, the probe FHMI exhibits obvious enhanced fluorescence with large red shift. FHMI is successfully applied to the mechanistic e...

Density functional theory (DFT) calculations have been performed to unravel the detailed mechanism of the CpRe(CO)3-catalyzed coupling reaction of CO2 with chloromethyloxirane (R). The mechanisms proposed in previous literature have been examined. However, the computed results seem not to completely rationalize the experimental findings. Alternatively, by performing an exhaustive search on the potential energy surface, we presented a novel CO-assisted mechanism, which provides an effective access to the catalytic coupling. The newly established mechanism involves the C O bond cleavage of R from the less hindered side, release of one CO ligand, CO2 insertion, re-coordination of the dissociated CO ligand, another CO ligand shift, reductive elimination with simultaneous migration of carbonyl substituent, resulting in P and regeneration of CpRe(CO)2. Two CO ligands attached to CpRe(CO)2 play significant roles in lowering the key CO2 insertion and reductive elimination: (i) One CO ligand dissociation prior to CO2 insertion contributes to reduce the electron density on the Re metal, facilitating the CO2 O atom nucleophilic attack. (ii) After performing the migration, another initially inactive CO ligand serves as a carbonyl substituent, which lowers the energy penalty for later reductive elimination through the resultant extra π-interaction and the smaller ring tension energy involved in TS. The theoretical results provide insight into the mechanism of the important coupling reaction and rationalize well the experimental observations.

In hydrogen production industry, thermochemical cycle technology for converting thermal energy into chemical storage energy of hydrogen owns absolute advantages. Compared with other thermochemical cycles, thermochemical cycle technology based on uranium (UTC) is safer and more efficient. This technology consists of three steps, where only the hydrogen production step is unique. In this paper, the verification has been done for this step. Solid products were characterized by XRD and Raman spectroscopy, which were confirmed to be α-Na2U2O7. Gas chromatographic analyses were performed for gas samples, in which hydrogen output was obtained using an internal standard method.

In marginal marine settings, understanding the role that clay minerals play in the transfer of metal cations from the water column to the seafloor is important if the composition of modern muds is to be used as a proxy for the precursors of ancient shale deposits. In this study, we conducted potentiometric titrations of three naturally abundant clay minerals (kaolinite, montmorillonite and illite) in 0.56 M NaCl electrolyte solutions to ascertain the surface reactivity of each clay mineral at seawater ionic strength. Our results demonstrate that all three clay minerals were increasingly anionic as pH increases from 3 to 9, with montmorillonite having the highest negative-charge. The potentiometric titrations and adsorption data were modeled using both non-electrostatic (NEM) and electrostatic (constant-capacitance model, CCM) surface complexation models (SCMs). A two-site surface complexation model, that included one basal siloxane surface site (≡X−) and one amphoteric edge site (≡SOH), provided an excellent fit for the protonation data of each mineral. Cd(II) adsorption experiments were conducted to quantify the magnitude of cation adsorption, which showed that 10 g montmorillonite, illite, and kaolinite powder could bind an equivalent of 4.7 × 10−4 g, 4.3 × 10−4 g, and 4.0 × 10−4 g of Cd, respectively, under conditions relevant to seawater (initial Cd concentration of 8.9 × 10−6 M, and pH = 8). To place this value into the context of modern riverine clay inputs to the ocean, 13.5 × 109 tons of total suspended sediment are deposited annually (Milliman and Meade, 1983) of which 10 to 25% is clay (Manheim et al., 1970; Schroeder et al., 2015). The total amount of Cd adsorbed to suspended clay minerals entering the modern oceans could then amount to approximately 104 to 105 tons per year. The results of this study highlight the potential role of clay minerals in transporting metals from the ocean water column to the seafloor.

Density functional theory (DFT) calculations have been conducted to unravel the mechanisms and chemoselectivities of Au-catalyzed diazo-based couplings with phenyl unsaturated aliphatic alcohols: the propargyl alcohol Ba resulting in the [4 + 1]-cycloaddition product P4a and the allyl alcohol Db giving the [2,3]-σ rearrangement species P5b. P4a formation involves a catalyst interaction with phenyldiazoacetate, N2 release, a hydroxyl O nucleophilic attack of Ba, a [1,4]-H shift, coordination isomerization, 5-endo-dig cyclization, a [4,1]-H shift and a H2O-assisted [1,3]-H shift. After the [4,1]-H shift, the slightly less favorable five-membered ring-opening possibly follows to afford trace P5a ([2,3]-σ rearrangement product), which would be kept in solution due to subsequent irreversible evolution. In addition, the Ba-involved chemoselectivity was probed and explained as follows: (i) both large H(hydroxyl)⋯C(carbene) electrostatic repulsion and strong three-membered ring strain involved in the TS make the formation of the O–H insertion product P1a difficult and (ii) the nucleophilic attack from the C2 atom of Ba brings about a structural twisting and thus increases the energy penalty forming the cyclopropenation product P2a. On the other hand, compared with the sp-C2 atom of Ba, the sp2-C2 atom of Db greatly facilitates the five-membered ring-opening step because of the presence of an extra pπ–pπ orbital overlap and eventually provides P5b exclusively.

Herein, the reaction mechanisms for the rhodium-catalyzed regioselective C7-functionalization of N-acyl indole are theoretically investigated by employing density functional theory (DFT) calculations. The role of the additive AgNTf2 in enhancing the reactivity and selectivity for the C7–H functionalization of N-acyl indole is clarified by calculations. The origins of the effect of the substituent group at the 6-position of N-acyl indole on the regioselectivity are explored by analyzing the electron and steric effects. The 7-olefination product is preferred for the H-substituted substrate (reaction A), which is attributed to the greater nucleophilicity of the C7 atom in comparison to that of the C2 atom. This facilitates the subsequent electrophilic attack of the Rh center. In reaction B with the CF3-substituted substrate, the 2-olefination product is preferred over the 7-olefination product mainly because of the stronger steric effects in TS2(C7)F compared with that in TS2(C2)F.

In vivo fluorescence imaging provides vital information required for biomedical research in living animals, and as such plays an essential role in disease assessment. Unfortunately, due to the lack of coherent approaches, in vivo fluorescence visualization is challenging, wasting not only time but the animals used. In recent years, cyanine-based systems have been found to exhibit attractive optical properties with appropriate bio-functionality and therefore have become go-to probes for in vivo research. Herein, we collected the recent breakthroughs using cyanine-based systems associated with use in living mammals, to provide researchers with the required information to develop appropriate strategies able to meet the increasing stringent requirements for practical applications. We concentrate on 6 sites within the cyanine skeleton, including the: meso-position (1), N-indole (2), phenyl-indole (2), cyclohexane (1), which have been used to design symmetric or asymmetric cyanine structures. Substitutions at the meso-position provide fluorescence probes featuring a switch of EWG and EDG, PET, spiro-cyclization, ICT within the cyanine skeleton, or FRET, for visualizing analytes in vivo. Substitution at the N-indole forms a positively charged system with long wavelength emission suitable for in vivo imaging. While, modification of the phenyl-indole contributes to the functional properties, including photoacoustic, photothermal and photodynamic behavior, which can be used for multimodal imaging as well as functional imaging in vivo. With a specific trigger at the N-indole or meso-position, NIR fluorescence pro-drugs could be developed for in vivo tracing of the efficiency of drug delivery. While modification of the cyclohexane can introduce a targeting moiety for the accurate monitoring of tumors or organs. Using these strategies appropriate design platforms can be developed to provide the next generation of optical systems for living animal research. Moreover, we hope this review will enable researchers to design systems with high efficiency for in vivo research, which will reduce both the development time and number of animals required to progress the research.

Silicon monoxide (SiO) has been explored and confirmed as a promising anode material of lithium-ion batteries. Compared with pure silicon, SiO possesses a more stable microstructure which makes better comprehensive electrochemical properties. However, the lithiation mechanism remains in dispute, and problems such as poor cyclability, unsatisfactory electrical conductivity, and low initial Coulombic efficiency (ICE) need to be addressed. Additionally, more attention needs to be paid on the internal relationship between electrochemical performances and structures. In this review, the different preparation processes, the derived microstructure of the SiOx , the corresponding lithiation mechanism, and electrochemical properties are summarized. Researches about disproportionation reaction which is regarded as a key point and other modifications are systematically introduced. Closely linked with structure, the advantages and disadvantages of various SiOx anode materials are summarized and analyzed, and the possible directions toward the practical applications of SiOx anode material are presented. In a word, from the preparation and reaction mechanism of the material to the modifications and future development, a complete and systematical review on SiOx anode is presented.

The mechanisms and chemo- and regioselectivities of divergent (Ni(cod)2/PCy3)-mediated/-catalyzed C(sp3)–F bond activation of 2-trifluoromethyl-1-alkenes (1) with alkynes (2) were investigated by density functional theory (DFT) calculations. The nickel-mediated/-catalyzed reaction involves sequential ligand exchange, alkene coordination, oxidative cyclization (1 + Ni(0) + 2), and first β-F(C(sp3)) elimination to give a common and requisite alkenylnickel(II) species, which bifurcates into either stoichiometric defluorinative [3 + 2] cycloaddition product 3 or catalytic defluorinative coupling products (nonmethylated 5, monomethylated 8, or trimethylated 9) depending on the absence and presence of additional reagents (Et3SiH, ZnMe2, and AlMe3). The Et3SiH-induced formation of 5 is found to be a result of facile metathesis relative to the 5-endo insertion leading to 3. Because of the presence of an F→Zn/Al interaction, ZnMe2/AlMe3 brings the methyl into defluorinative coupling products. In the stoichiometric...

Benzene ring functionalization provides useful alternatives to access indole derivatives and has received much attention in recent years. In this work, the mechanism of Pt(II)-catalyzed cyclization/alkynylation of benziodoxole with pyrrole homopropargylic ethers to generate C5-alkenylated indole derivatives has been studied with the aid of density functional theory (DFT) calculations. We found that five-membered-ring cyclization/six-membered-ring cyclization is competitive in the formation of an indole skeleton. The following aromatization stage prefers the reaction sequence bicarbonate-assisted deprotonation at the C3a position, H2CO3-promoted methoxy elimination at the C7 position, and bicarbonate-assisted deprotonation at the C6 position. In the last alkynylation stage, the oxidative substitution mechanism assisted by H2CO3 is found to be favored over the previously proposed 1,2-iodo shift and oxidative addition. The overall rate-determining step is oxidative substitution. Additionally, an interesting ...

Density functional theory (DFT) calculations have been performed to unravel the mechanism of Lewis-acid-induced Ni(cod)2-catalyzed selective coupling reactions of one diketene and two alkynes. Complex mixtures (unsymmetrical phenylacetic acid P1, symmetrical phenylacetic acid P2 and (3E)-4-ethyl-5-methylene-3-heptenoic acid P3) were obtained in the absence of Et2Al(OEt). P1 formation involves C(sp2)-O oxidative addition of diketene, twice alkyne insertion, intramolecular C═C insertion, acidolysis, and β-H elimination. For P2/P3 formation, the common key issue related to the C═C double bond cleavage of the substrate diketene was explored and found that it was accomplished via a four-membered-ring-closure/four-membered-ring-opening process. And then, P2 was produced via the second alkyne insertion while P3 was accessed by a stoichiometric reaction with HCl. The Et2Al(OEt)-induced chemoselectivity was also probed. It is found that the Ni–O (from Al reagent) bonding facilitates the second alkyne insertion, an...

Measuring the metal binding potential and reactivity of bacterial mats is challenging in alkaline and carbonate-rich systems. Traditional methods used to measure these parameters, such as potentiometric titrations and metal adsorption pH edges, are difficult to implement due to the presence of the carbonate minerals that buffer pH and prevent assessment of mat surface reactivity. Additionally, under alkaline conditions metals may form hydroxide and/or carbonate precipitates. In this study we examined the metal binding capacity of four distinct bacterial mats collected from Fairmont Hot Springs, BC, Canada. To prevent metal precipitation, the bacterial mat concentration was varied under a constant initial cadmium (Cd) concentration of 8.89 μM and at pH 8. In addition to the intact bacterial mats, a carbonate mineral sample and two bacterial mats in which the carbonate mineral was removed via acid-treatment, were used as end-members to assess the mechanisms of reactivity in the whole system. Freundlich adsorption isotherms were used to fit metal adsorption data and directly compare surface reactivity among intact mats and mat components. Two of the intact mats exhibited a higher affinity for Cd compared to the mineral at metal equilibrium concentrations above 2.5 μM, while the other two intact mats had lower affinities under all experimental conditions. Generally, we found the acid-treated mats had higher Cd adsorption capacities than the carbonate mineral. When compared to their equivalent intact mats, only one acid-treated mat had a higher affinity for Cd. Further, we modeled whether metal adsorption in the intact mats, containing microbes and carbonate mineral, could be explained by a linear combination of the observed metal uptake by the organic and inorganic components through end-member experiments. Metal adsorption additivity results were mixed. Metal uptake by one intact mat was found to be additive, while for the other mat the additive model significantly underestimated the observed Cd accumulation. Our study demonstrates the potential, as well as the limitations, of using modified metal adsorption edges to determine the metal binding affinity and surface reactivity of bacterial mats in alkaline and carbonate-rich systems.

Background: In this study, we have successfully developed a simvastatin (SMV) and miR-21i-loaded poly (D,L-lactide-co-glycolide)/polyethylenimine (PLGA/PEI) nanoparticles (NP) to enhance the therapeutic efficacy in gastric cancers. Methods: The PLGA/PEI nanoparticles by sonication method. The nanoparticles were characterized for in vitro physicochemical and biological assays and pharmacokinetic study was performed in rats. Results: CLSM/FACS results clearly showed the ability of SMV/miR-21i-loaded PLGA/PEI NP (PPN-S21i) to deliver the combinational therapeutics of SMV and miR-21i to the cancer cells. Combination of SMV+miR-21i showed significantly lower cell viability compared to that of free SMV. Our results clearly highlight the importance of simultaneous interaction of SMV+miR-21i and that it could significantly decrease the cell proliferation in BGC-823, SGC-7901 and HGC-27 gastric cancer cells while it was significantly less cytotoxic to normal gastric mucosa cells (GES-1). Cell apoptosis of SMV+miR-21i was significantly higher compared to that of individual drug or miRNA. Finally, pharmacokinetic analysis revealed that PPN-S21i significantly prolonged the blood circulation time of SMV compared to that of free SMV indicating the potential of carrier system. Conclusion: Overall, results clearly indicate that the combination of SMV+miR-21i (gene + drug therapy) might provide a valuable strategy for the clinical management of gastric cancers.

In this study, we report the complete mitochondrial genome of Harpalus sinicus (occasionally named as the Chinese ground beetle) which is the first mitochondrial genome for Harpalus. The mitogenome is 16,521 bp in length, comprising 37 genes, and a control region. The A + T content of the mitogenome is as high as 80.6%. A mitochondrial origins of light-strand replication (OL)-like region is found firstly in the insect mitogenome, which can form a stem-loop hairpin structure. Thirteen protein-coding genes (PCGs) share high homology, and all of them are under purifying selection. All tRNA genes (tRNAs) can be folded into the classic cloverleaf secondary structures except tRNA-Ser (GCU), which lacks a dihydrouridine (DHU) stem. The secondary structure of two ribosomal RNA genes (rRNAs) is predicted based on previous insect models. Twelve types of tandem repeats and two stem-loop structures are detected in the control region, and two stem-loop structures may be involved in the initiation of replication and transcription. Additionally, phylogenetic analyses based on mitogenomes suggest that Harpalus is an independent lineage in Carabidae, and is closely related to four genera (Abax, Amara, Stomis, and Pterostichus). In general, this study provides meaningful genetic information for Harpalus sinicus and new insights into the phylogenetic relationships within the Carabidae.

The Rh(III)-catalyzed oxidative coupling of oxime ether (S1) and cyclopropanol (S2) with Cu(II) as the oxidant features the combination of C-H activation and strained ring opening. The sequential order of C-H activation versus ring opening was investigated with the aid of density functional theory calculations. Prior ring opening due to the release of ring strain is found to be favored over the prior C-H activation. For the prior ring-opening mechanisms, the outer-sphere concerted metalation-deprotonation (CMD) mechanism in C-H bond activation is energetically favored. The outer-sphere CMD mechanism proposed in this work favors solvent effects and affords the N→Rh binding that allows a directing role of the Schiff base group. In conclusion, the reaction was suggested to undergo prior ring opening followed by C-H activation via the outer-sphere CMD mechanism.

As one of the most prospective transitional metal oxide cathode materials for sodium-ion batteries (SIBs), P2-type Na2/3Ni1/3Mn2/3O2 layered oxide generally suffers from sluggish Na+ kinetics and complicated structural evolution. Here, a stable Co-free P2-Na2/3Li1/9Ni2/9Mn2/3O2 cathode material with multilayer oriented stacking nanoplates is reported, which exhibits high hydrostability realized by partial Li element substitution for Ni. A prominent rate capability (71.7% capacity retention at 5 C compared to 0.2 C), an excellent cycling stability (78.7% capacity retention at 2 C after 300 cycles) and a promoted performance even at a higher cutoff potential of 4.4 V were displayed owing to bifunctional strategy of chemical substitution coupled with structure modulation, and the as-synthesized material retains its original structure and electrochemical performance after being aged in water. Moreover, dominant Na+ capacitive storage mechanism, high thermostability and complete solid-solution reaction are explicitly elucidated through quantitative calculation of electrochemical kinetics and in-situ X-ray diffraction technique. These findings reveal the importance of rational chemical substitution and structure modulation strategy, and inspire novel design of high-performance cathode materials for rechargeable SIBs.

Preparing excellent hydroxide precursor is a significant step in the synthesis of high-energy–density Ni-Rich cathode materials. Efforts to address their limited cycle life have focused on the structure of the precursor. Herein, we showed a systematic survey to reveal the structural evolution of Ni-Rich Ni-Co-Al hydroxide precursor under different synthesis conditions. Under a certain pH, the higher the ammonia concentration is, the larger the primary particle size gradually becomes. Simultaneously, at the low pH (pH = 11.2), Ni-Rich Ni-Co-Al hydroxide precursor is consisted of four phases: Ni(OH)2, AlO(OH), Al(OH)3 and Al2(SO4)3 with the space group P-3 m1, Cmcm, P21/n and R-3, respectively. At the harsh pH (pH = 11.8), the precursor is consisted of two phases: Ni(OH)2, and Al(OH)3 with the space group P-3 m1 and P21/n, respectively. This study provided a significant guidance for the design of the precursor with special structure.

Gold-catalyzed cyclization of 2-alkynyl-N-propargylanilines provides a step-economic method for the construction of three-dimensional indolines. In this article, the M06 functional of density functional theory was employed to gain deeper insights into the reaction mechanism and the associated intriguing experimental observations. The reaction was found to first undergo Au(I)-induced cyclization to form an indole intermediate, 1,3-propargyl migration, and substitution with the substrate 2-alkynyl-N-propargylaniline (R1) to generate the intermediate product P1, an allene species. Subsequently, Au(I)-catalyzed conversion of P1 into the final product P2, an indoline compound, occurs first through direct cyclization rather than via the previously proposed four-membered carbocycle intermediate. Thereafter, water-assisted oxygen heterocycle formation and proton transfer generate the final product. The calculated activation free energies indicate that P1 formation is 5.9 times slower than P2 formation, in accordance with the fact that P1 formation is rate-limiting. Futhermore, the intriguing experimental phenomenon that P2 can be accessed only after almost all the substrate R1 converts to P1 although P1 formation is rate-limiting was rationalized by employing an energetic span model. We found the initial facile cyclization to form a highly stable indole intermediate in the formation of P1 is the key to the intriguing experimental phenomenon.

Malonyl-CoA decarboxylase (MCD) can control the level of malonyl-CoA in cell through the decarboxylation of malonyl-CoA to acetyl-CoA, and plays an essential role in regulating fatty acid metabolism, thus it is a potential target for drug discovery. However, the interactions of MCD with CoA derivatives are not well understood owing to unavailable crystal structure with a complete occupancy in the active site. To identify the active site of MCD, molecular docking and molecular dynamics simulations were performed to explore the interactions of human mitochondrial MCD (HmMCD) and CoA derivatives. The findings reveal that the active site of HmMCD indeed resides in the prominent groove which resembles that of CurA. However, the binding modes are slightly different from the one observed in CurA due to the occupancy of the side chain of Lys183 from the N-terminal helical domain instead of the adenine ring of CoA. The residues 300 - 305 play an essential role in maintaining the stability of complex mainly through hydrogen bond interactions with the pyrophosphate moiety of acetyl-CoA. Principle component analysis elucidates the conformational distribution and dominant concerted motions of HmMCD. MM_PBSA calculations present the crucial residues and the major driving force responsible for the binding of acetyl-CoA. These results provide useful information for understanding the interactions of HmMCD with CoA derivatives. Proteins 2016; 84:792-802. © 2016 Wiley Periodicals, Inc.

With the aid of density functional theory (DFT) calculations, the Pd-catalyzed reactions of aryl iodide with unsymmetrical alkyne leading to two products containing C(sp 3 )−I bond ( P3 and P4 ) and one product containing a three-membered carbocyclic unit ( P5 ), have been studied theoretically. It is found that both the alkyne insertion and the subsequent C C bond insertion involved in the reaction are the major thermodynamic driving forces. The alkyne insertion instead of the C(sp 3 )−I reductive elimination is predicted to be rate-determinant. Similar barrier heights calculated for the two insertion modes of unsymmetrical internal alkyne ( TS 3-4 and TS 3′-4′ ) lead to the products P3 (47.2%) and P4 + P5 (48.8%) having similar product yields. The intriguing formation of the product containing a three-membered carbocyclic unit ( P5 ) was investigated in details. The second alkene insertion is found to be kinetically more favored than the C(sp 3 )−I reductive elimination, leading to product P5 (39.0%) more productive than P4 (9.8%). The remarkably thermodynamically favored β−H elimination is the key factor enabling formation of P5 . Why significant bulky phosphine ligand such as P(t-Bu) 3 instead of small one such as P(Me) 3 was employed experimentally have also been rationalized based on our calculation results.

Pd-catalyzed decarboxylative Heck-type coupling of 3-chlorobenzo[b]thiophene-2-carboxylic acids with styrenes have been developed as an efficient strategy for the construction of functionalized benzo[b]thiophenes. Theoretical analysis shows that AgCl generated during the reaction, instead of Pd, π-coordinates with the carboxyl O atom, making easy the rate-determining CO2 dissociation. The divergent reactivities of the Cl-substituted and H-substituted 3-benzo[b]thiophene-2-carboxylic acids are mainly due to the presence of the Cl substituent, which reduces the adjacent π-π interplay, thereby significantly contributing to decarboxylation. Therefore, the presence of both AgCl and the Cl substituent are of key importance in ensuring the occurrence of the reaction under the given conditions.

The reaction features combination of C H activation and ring opening of cyclopropanol was studied with the aid of DFT calculations. With the reaction of N-pyrimidylindoline and 1-benzylcyclopropanol as an example to accomplish the alkylation, we found the order of C H activation/ring opening is difficult to occur. Instead, the order of ring opening/C H activation is predicted to be more reasonable, which circumvents the N→Rh bond breaking. Two catalytic cycles were suggested. The first cycle relates to the catalytic oxidation of cyclopropanol by Cu(II) to generate an intermediate product, the vinyl ketone. The mechanism mainly involves prior ring opening of cyclopropanol and β-H elimination. The second cycle relates to the product formation from the resultant intermediate product, in which the C H activation of N-pyrimidylindoline, C C bond insertion of the intermediate product and protonation are included. The insights gained in this study are expected to be pertinent in other reaction systems involving combination of C H activation and ring opening.

Polymer-ceramic composite electrolyte is an effective solution for developing high-performance and flexible all-solid-state lithium metal battery. However, the key bottleneck of composite electrolyte including low ionic conductivity and high interfacial impedance have impeded their industrialization in solid electrolyte lithium batteries. Here we present a polymer-ceramic hybrid electrolyte (polyethylene oxide (PEO)/polyvinylidene fluoride (PVDF)/Li6.4La3Zr1.4Ta0.6O12 (LLZTO)) is designed and modified by trace amount of liquid electrolyte. The addition of PVDF can not only reduce the crystallinity of PEO polymer, but also intensify the affinity between liquid electrolyte and the composite electrolyte. Furthermore, the interfacial modification can synchronously achieve the intimate connection, low interfacial impedance between the electrodes and solid electrolytes by forming the viscoelastic and stable layer. Due to the artful design, the solid-state battery deliver excellent performance. The Li symmetric cells show excellent interface stability without short circuits for 1000h. The assembled LiFePO4/Li cells exhibit a discharge capacity of 160.1 mA h g−1 after 200 cycles at 0.4C and 143.3 mA h g−1 at 5C. The composite solid electrolyte provides an effective and feasible methods to solve the interfacial issues and develop high performance solid lithium metal batteries.