Latest ArticlesAchieving efficient adsorption and separation of C2H2/CO2 mixtures is a goal that people have always pursued to improve the situation of high energy consumption brought by traditional separation technologies in industry today. High-nuclearity metal cluster-based MOFs with different functionalities are promising for this separation, but it is a complicated and difficult task to precisely control their structures. The strategy of pore-space partition (PSP) is a powerful way to construct this type MOFs, which has the characteristic of isostructural relationship, and can be resulted in a similar performance for them. Therefore, it is an interesting work to explore the effect of MOFs property by adjusting the size of PSP dividers. Herein, three tetranuclear Cu(Ⅱ) cluster-based MOFs (FJU-112/113/114) with dual functionalities has been successfully obtained by PSP strategy with various lengths of divider units. With the highest microporosity and unique functional site, FJU-114 realized a good improvement in the adsorption and separation performance of C2H2/CO2. The gas adsorption and lab-scale C2H2/CO2 breakthrough experiments demonstrated that FJU-114 exhibits the highest adsorption uptake of 77 cm3/g for C2H2, and shows the best separation factor of 4.2 among three MOFs. The GCMC simulation reveals that a stronger adsorption binding site of C2H2 in FJU-114a located in the cage Ⅱ near the unchanged tetranuclear copper node, combined with its high microporosity to achieve the effect of dual functionalities for the improvement performance of C2H2 adsorption and separation.
Lithium-sulfur batteries are considered to be a new generation of high energy density batteries due to their non-toxicity, low cost and high theoretical specific capacity. However, the development of practical lithium-sulfur batteries is seriously impeded by the sluggish multi-electron redox reaction of sulfur species and obstinate shuttle effect of polysulfides. In this study, a porous lanthanum oxychloride (LaOCl) nanofiber is designed as adsorbent and electrocatalyst of polysulfides to regulate the redox kinetics and suppress shuttling of sulfur species. Benefiting from the porous architecture and luxuriant active site of LaOCl nanofibers, the meliorative polarization effect and sulfur expansion can be accomplished. The LaOCl/S electrode exhibits an initial discharge specific capacity of 1112.3 mAh/g at 0.1 C and maintains a superior cycling performance with a slight decay of 0.02% per cycle over 1000 cycles at 1.0 C. Furthermore, even under a high sulfur loading of 4.6 mg/cm2, the S cathode with LaOCl nanofibers still retains a high reversible areal capacity of 4.2 mAh/cm2 at 0.2 C and a stable cycling performance. Such a porous host expands the application of rare earth based catalysts in lithium-sulfur batteries and provides an alternative approach to facilitate the polysulfides conversion kinetics.
Neuropathic pain (NP) is one of the most common pathological pain types and is associated with limited treatment options; moreover, it affects patients’ quality of life and causes a heavy social burden. Despite the emphasis on inhibiting neuronal apoptosis to relieve NP, the crucial role of a neuroinflammation is often overlooked. Therefore, refocusing on the regulation of microglia polarization to create a more conducive environment for neuron holds great potential in NP treatment. In recent years, small interfering RNAs (siRNAs) had become an attractive therapeutic option. However, an efficient loading and delivery system for siRNA is still in lack. In our study, a nanostructured tetrahedral framework nucleic acid loaded with the small interfering RNA C–C chemokine receptor 2 (T-siCCR2) was successfully designed and synthesized for use in NP rat model in vivo and in a lipopolysaccharide (LPS)-induced inflammatory environment in vitro. This nanoscale complex is endowed with structural stability and satisfactory delivery efficiency while assuring the silencing effect of siRNA-CCR2. In vivo, T-siCCR2 treatment exhibited favorable effects on pain relief and functional improvement in the NP animal model by directly targeting microglia. In vitro, T-siCCR2 counteracts LPS-induced inflammation by inhibiting the differentiation of microglia toward the M1 phenotype, thus playing a neuroprotective role. RNA sequencing was subsequently performed to elucidate the underlying mechanism involved. These results indicate that T-siCCR2 may serve as a potential treatment option for NP in the future.
The large current density of electrochemical CO2 reduction towards industrial application is challenging. Herein, without strong acid and reductant, the synthesized BiVO4 with abundant oxygen vacancies (Ovs) exhibited a high formate Faradaic efficiency (FE) of 97.45% (-0.9 V) and a large partial current density of -45.82 mA/cm2 (-1.2 V). The good performance benefits from the reconstruction of BiVO4 to generate active metal Bi sites, which results in the electron redistribution to boost the OCHO* formation. In flow cells, near industrial current density of 183.94 mA/cm2 was achieved, with the FE of formate above 95% from 20 mA/cm2 to 180 mA/cm2. Our work provides a facily synthesized BiVO4 precatalyst for CO2 electroreduction.
Van der Waals (vdW) ferroelectric-semiconductor heterojunction provides reconfigurable band alignment based on optical/electrical-assisted polarization switching, which shows great potential to construct artificial visual neural systems. However, the mechanical exfoliation fabrication scheme for proof-of-concept demonstrations and fundamental studies is cumbersome and not scalable for practical application. Here, we present a synthetic strategy for the large-scale and high crystallinity growth of planar/vertical α-In2Se3/MoS2 heterojunctions by dynamically tuning the growth temperature. Furthermore, based on the α-In2Se3/MoS2 heterostructures, photo-synapse devices are designed and fabricated to simulate visual neural systems functions, including multistate storage, optical logic operation, potentiation and depression, paired-pulse facilitation (PPF), short-term memory (STM), long-term memory (LTM), and Learning-Forgetting-Relearning. By coupling the spatiotemporally relevant optical and electric information, the device can mimic the superior biological visual system's light adaptation and Pavlovian conditioning. This work provides a strategy for dynamically tuning the orientation of ferroelectric-semiconductor heterojunction stacks and will give impetus to applying all-in-one sensing and memory-computing artificial vision systems.
Biocompatible amphiphilic nanoparticles (NPs) with tunable particle morphology and surface property are important for their applications as functional materials. However, previously developed methods to prepare amphiphilic NPs generally involve several steps, especially an additional step for surface modification, greatly hindering their largescale production and widespread applications. Here, a versatile one-step strategy is developed to prepare biocompatible amphiphilic dimer NPs with tunable particle morphology and surface property. The amphiphilic dimer NPs, which consist of a hydrophobic shellac bulb and a hydrophilic poly(lactic acid) (PLA) bulb with PLA-poly(ethylene glycol) (PEG) on the bulb surface, are prepared in a single step by controlled co-precipitation and self-assembly. Amphiphilic PLA-PEG/shellac dimer NPs demonstrate excellent tunability in particle morphology, thus showing good performances in controlling the interfacial curvature and emulsion type. In addition, temperature-responsive PLA-poly(N-isopropyl acrylamide) (PNIPAM)/shellac dimer NPs are prepared following the same method and emulsions stabilized by them show temperature-triggered response. The applications of PLA-PEG-folic acid (FA)/shellac dimer NPs for drug delivery have also been demonstrated, which show a very good performance. The strategy of preparing the dimer NPs is green, scalable, facile and versatile, which provides a good platform for the design of dimer NPs with tunable particle morphology and surface property for diverse applications.
The utilization of ethane-selective materials for adsorption-based separation technology presents an energy-efficient alternative to cryogenic distillation for ethylene (C2H4) purification from ethane (C2H6). To study the relations between separation performance and pore environments, we carried out the isoreticular chemistry rule to introduce the -NH2 groups into a C2H6-selective MOF [Cu1.5(BTC)(DPU)1.5(H2O)1.5], and successfully improved the adsorption capacity and selectivity for C2H6 over C2H4. The NH2-functionalized MOF [Cu1.5(NH2-BTC)(DPU)1.5(H2O)1.5] with a relatively narrow pore not only forms appropriate pore restriction but also provides additional binding sites to enhance the adsorption capacity of C2H6 relative to C2H4. Both gas adsorption and dynamic breakthrough results indicated that the -NH2 functionalization significantly enhanced the separation performance of materials for C2H6/C2H4 mixtures, allowing the production of C2H4 with a purity of over 99.99% and a productivity of up to 30.02 L/kg in one step. Theoretical calculations revealed that the synergistic effect of appropriate pore confinement and NH2-modified functional surfaces imposed stronger interactions on C2H6 than C2H4.
Density functional theory (DFT) was performed to systematically study the adsorption and dissociation of N2 on Ir(100) and Ir(110) surfaces. By analyzing the properties, including adsorption energies, reaction barriers, and optimal adsorption sites, the hollow (H) sites were finally identified as favorable dissociation sites for N2. The dissociation barriers of N2 are 0.87 eV on Ir(100) and 1.12 eV on Ir(110), which can be overcome at around 348 and 448 K, respectively. Therefore, Ir(100) is screened as a promising catalyst for N2 dissociation compared to Ir(110). This can be attributed to the significantly higher adsorption energy of N2 on the H site of Ir(100) (−0.48 eV) compared to that on Ir(110) (−0.22 eV), leading to different dissociation mechanisms on Ir(100) and Ir(110). Ir(100) can dissociate N2 directly on H site and Ir(110) should firstly capture N2 via bridge site and further transfer the adsorbed N2 to the H site, which will dramatically deteriorate the reactivity of N2 dissociation. In addition, the following protonation processes of dissociated *N atoms are all exothermal at 348 K on Ir(100), indicating that the ammonia synthesis can occur spontaneously as the temperature higher than 348 K. These results have provided a reasonable materials design scheme for subsequent ammonia synthesis.
Aqueous iron-ion batteries are regarded as one of the most promising candidates for grid applications owing to their low cost, high theoretical capacity, and excellent stability of iron in aqueous electrolytes. However, the slow Fe (de)insertion caused by the high polarity of Fe2+ makes it difficult to match suitable cathode materials. Herein, defect-rich MoS2 with abundant 1T phase is synthesized and successfully applied in aqueous iron-ion batteries. Benefit from abundant active sites generated by the heteroatom incorporation and S vacancy, as well as the highly conductive 1T phase, it can deliver a specific capacity of 123 mAh/g at a current density of 100 mA/g, and demonstrates an impressive capacity retention of 88% after 600 cycles at 200 mA/g. This work presents a novel pathway for the advancement of cathode materials for aqueous iron-ion batteries.
Hymoins A–C (1–3), three unusual polycyclic polyprenylated acylphloroglucinols (PPAPs) were isolated from the flowers of Hypericum monogynum. Hymoin A features the first intriguing 6/5/5/5/7 pentacyclic caged PPAP. Hymoin B is characterized by an unprecedented rearranged 5/6/8 tricyclic ring system, while hymoin C represents the first rearranged PPAP with a fantastic spirocyclic 5/6/7 ring system. Their structures were established by extensive spectroscopic analysis, X-ray crystallography, and computational methods. The plausible biosynthetic routes for the compounds were also proposed. In oleic acid (OA)-induced HepG2 cells, all compounds exhibited significant lipid-lowering activity at the concentrations of 2–8 µmol/L. Further mechanistic study implied that compound 1 exhibited excellent lipid-lowering activity in OA-induced HepG2 cells through inhibiting the proteins of free fatty acids synthesis and improving lipidolysis.
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