Latest ArticlesLi-ion batteries with solid polymer electrolytes (SPEs) are safer than conventional liquid electrolytes due to the absence of highly flammable liquid electrolytes. However, their performance is limited by the poor Li+ transport in SPEs at room temperature. Anion-containing polymer-chains incorporated SPEs (ASPEs) are therefore developed to enhance Li+ diffusion kinetics. Herein, we propose a novel and feasible strategy to incorporate the anion-containing polymer-chains, such as lithiated perfluorinated sulfonic acid (PFSA), into polyvinylidene fluoride (PVDF) polymer-based SPEs. The immobile anion groups from the PFSA-chains impede the migration of mobile anion groups dissociated from the Li salt. The transference number is thus raised from ~0.3 to 0.52 with the introduction of anion-containing polymer-chains into SPEs. The electrostatic repulsion among anion-containing chains also reduces the close chain stacking and brings 159% increase in the ionic conductivity to 0.83 × 10−3 S/cm at 30 ℃ in contrast with the pure PVDF-based SPE. In addition, LiFeO4/Li batteries with ASPEs exhibit 55% capacity boost at 0.5 C in contrast to the capacity of batteries with pure-PVDF SPEs, and also offer more than 1000 charge/discharge cycles. Our research findings potentially offer a facile strategy to design thermal stable SPEs with superior Li+ transport behaviors towards developing high-performance SPEs-based batteries.
Despite the improving coverage of preventative vaccines,hepatitis B remains a severe global public health problem,with more than 250 million patients living with hepatitis B virus (HBV) infection. Current available therapies,including nucleos(t)ide analogs and peginterferon,can control HBV replication but fail to eliminate covalently closed circular DNA (cccDNA) and achieve a cure. The HBV core protein (Cp) is a well-conserved structural protein,self-assembling to form the viral capsid. It involves in or modulates almost every stage of the HBV lifecycle,which makes it an attractive target for the development of new anti-HBV therapies. HBV core protein allosteric modulators (CpAMs) have become a hotspot in recent years. Herein,we provide a concise report focusing on the various medicinal chemistry strategies involved in the latest research (2018–2022) of HBV CpAMs,including high throughput screening (HTS),virtual screening (VS),drug repositioning,natural products,substitution decorating approach,scaffold hopping,molecular hybridization,prodrug strategy and conformational constraint strategy,to provide guidance for further development of new and effective anti-HBV drugs.
The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention. Here, an integrated strategy is proposed by rational designing multifunctional architecture to manipulate the redox kinetics of polysulfides, specifically, by employing iron atoms (Fe-As) and iron-species nanoparticles (Fe-NPs) co-embedded nitrogen-doped carbon nanotube (Fe-NCNT) as catalyst and host for sulfur. The synergistic cooperation of Fe-As and Fe-NPs provides efficient active sites to facilitate the diffusion, strengthen the affinities, and promote the conversion reactions for polysulfides. Furthermore, the NCNT not only offers practical Li+ transport pathways but also immobilize the polysulfides effectively. Benefiting from these merits, the Fe-NCNT/S electrodes exhibit high initial specific capacity of 1502.6 mAh/g at 0.1 C, outstanding rate performance (830 mAh/g at 2 C), and good cycling performance (597.8 mAh/g after 500 cycles with an ultralow capacity fading rate of 0.069% per cycle). This work features the distinct interaction of iron atom-nanoparticles on facilitating immobilization-diffusion-transformation process of polysulfides, and it also expected to pave the way for the application in practical Li-S batteries.
Electrochromic devices (ECDs) have exhibited promising applications in the fields of energy-saving intelligent buildings and next-generation displays because of their simple structure, low power consumption, and multicolor displays. W18O49/polyaniline (PANI) hybrid films are prepared and assembled to ECDs. Compared with pure PANI and W18O49 films, the hybrid film exhibits superior electrochemical and electrochromic performance, including high optical modulation (70.2%), large areal capacity (79.6 mF/cm2), and good capacitance retention. The excellent electrochemical and electrochromic performance is ascribed to the formation of the donor (PANI)-acceptor (W18O49) pair, the porous structure in the nanowires, and the large surface area, which enhance electron delocalization of the W18O49/PANI, improve the ion diffusion rate, and increase the charge storage sites. Furthermore, benefitting from the outstanding optical, electrical, and multifunctional properties, the W18O49/PANI hybrid film-based ECD platform is expected to play an important role in electrochromism and energy storage.
An eco-friendly and convenient method is developed herein for the synthesis of S-aryl dithiocarbamates via visible-light-induced SET process of an EDA complex between thianthrenium salt functionalized arenes and dithiocarbamate anions under mild aqueous micellar conditions. This strategy indirectly realizes the method for constructing S-aryl dithiocarbamates through site-selective C−H functionalization of arenes. Most importantly, the reaction proceeded smoothly without addition of any photocatalyst, and the by-product thianthrene is recycled in quantity, ultimately minimizing the production of chemical waste. This protocol provides a promising synthesis candidate for the construction of valuable S-aryl dithiocarbamates, which also opens up a new avenue for micellar photocatalysis.
With the development of a small interfering RNA (siRNA) delivery strategy, increasing siRNA therapeutics for tumor treatment appeared in clinical trials and pre-clinical development. However, the test results of such therapeutics unveiled that efficient siRNA delivery to tumor tissues is still challenging. Albumin is considered an ideal carrier for delivering hydrophobic agents into tumor tissue because it is highly concentrated and long-circulating in blood and has propensity of tumor enrichment. Herein, we synthesized lipid conjugated siRNAs (LsiRNAs), which showed high affinity to albumin. Mechanistically, LsiRNAs non-covalently bind to the hydrophobic core of albumin through its octadecyl tails. The small size of albumin/LsiRNAs allows the complex to penetrate tumor tissue efficiently. Biodistribution test proved that albumin extremely prolonged circulation time and increased tumor retention of associated LsiRNAs. Notably, LsiRNA against programmed death ligand-1 (Pdl1) efficiently suppressed tumor growth as well as prolonged survival time of tumor bearing mice by increasing infiltration of CD8+ T cells as well as promoted the maturation of dendritic cells both in tumor and lymph. Together, LsiRNAs provide a simple but effective way for siRNA tumor delivery that “hitchhikes” on albumin.
Uranium and molybdenum are important strategic elements. The production of 99Mo and the hydrometallurgical process of uranium ore face difficult problems of separation of uranium and molybdenum. In this study, the four phenanthroline diamide ligands were synthesized, and extraction and stripping experiments were performed under different conditions to evaluate the potential application of these ligands for separation of U(Ⅵ) over Mo(Ⅵ). With the growth of alkyl chain, the solubility of ligands could be greatly improved, and the separation effect of U(Ⅵ) over Mo(Ⅵ) gradually increased. The SFU/Mo were around 10,000 at 4 mol/L HNO3. Three stripping agents were tested with the stripping efficiency of Na2CO3 (5%) > H2O > HNO3 (0.01 mol/L). The stripping percentages of the three stripping agents were all close to unity, indicating that the ligands had the potential to be recycled. The chemical stoichiometry of U(Ⅵ) complexes with ligands was evaluated as 1:1 using electrospray ionization mass spectrometry, ultraviolet visible spectroscopy and single-crystal X-ray diffraction. The consistency between theoretical calculation and experimental results further explains the coordination mechanism.
Selective oxidation of biomass-derived monosaccharide into high value-added chemicals is highly desirable from sustainability perspectives. Herein, we demonstrate a surface-functionalized carbon nanotube-supported gold (Au/CNT-O and Au/CNT-N) catalyst for base-free oxidation of monosaccharide into sugar acid. Au/CNT-O and Au/CNT-N surfaces successfully introduced oxygen- and nitrogen-containing functional groups, respectively. The highest yields of gluconic acid and xylonic acid were 93.3% and 94.3%, respectively, using Au/CNT-N at 90 ℃ for 240 min, which is higher than that of using Au/CNT-O. The rate constants for monosaccharide decomposition and sugar acid formation in Au/CNT-N system were higher, while the corresponding activation energy was lower than in Au/CNT-O system. DFT calculation revealed that the mechanism of glucose oxidation to gluconic acid involves the adsorption and activation of O2, adsorption of glucose, dissociation of the formyl C-H bond and formation of O-H bond, and formation and desorption of gluconic acid. The activation energy barrier for the glucose oxidation over Au/CNT-N is lower than that of Au/CNT-O. The nitrogen-containing functional groups are more beneficial for accelerating monosaccharide oxidation and enhancing sugar acid selectivity than oxygen-containing functional groups. This work presents a useful guidance for designing and developing highly active catalysts for producing high-value-added chemicals from biomass.
Peptide and protein drugs with therapeutic effects suffer from their short half-life and low stability, albeit their high efficiency and specificity. To overcome these demerits, long-acting drug delivery systems have been developed, wherein poly(lactic-co-glycolic acid) (PLGA) implants are most preferred owing to their excellent biodegradability and biocompatibility. Dozens of PLGA based products have been approved since 1986, when the first product, named Decapeptyl®, successfully marched into market. To meet the increasing demand for delivering various peptides and proteins, different kinds of technologies have been developed for lab-scale fabrication or industrial manufacture. This review aims to introduce recent advances of PLGA implants, and give a brief summary of fundamental properties of PLGA, fabrication technologies of peptides/proteins-loaded PLGA implants as well as factors influencing the drug release processes. Moreover, challenges and future perspectives are also highlighted.
The design of pseudocapacitive materials by coupling transition metal compounds with a conductive carbon matrix is important for the high performance of supercapacitors. Herein, we construct the Prussian blue analogue derived nickel-cobalt selenides coupling with nitrogen-doped carbon nanofibers (NiCoSe4-NCNFs) by carbonization and selenization of polyacrylonitrile nanofibers. The effect of selenization and element N doping on the morphological structure and surface chemistry of NiCoSe4-NCNFs are evaluated. Due to the accelerated electrolyte ion diffusion, enlarged active surface area and the modified surface chemistry by the strong interaction at NiCoSe4/NCNFs interfaces, NiCoSe4-NCNFs show excellent capacitive behaviors in 1 mol/L KOH, and the specific capacitance is 1257 F/g at 1 A/g with a rate capability of 78% and cyclic stability of 82.9%. The Gibbs free energy of adsorption OH− is calculated by density functional theory to investigate the charge storage mechanism. This work offers a new strategy to construct the transition metal selenides/carbon nanofibers hybrids for high-performance supercapacitor devices.
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