Latest ArticlesGraphite tailings produced by natural graphite is usually regarded as garbage to be buried underground, which would result in a certain waste of resources. Here, in order to explore the utilization of natural graphite tailings (NGT), a liquid-polyacrylonitrile (LPAN) is used to modify the NGT fragments and aggregate them together to form secondary graphite particles with low surface area and high tap density. Moreover, the modified NGT show much better electrochemical performances than those of original one. When tested in full cells coupled with NMC532 cathode, the material achieves a high rate capability and cycle stability at the cutoff voltage of 4.25 V as well as 4.45 V, which maintains 84.32% capacity retention after 500 cycles at 1 C rate (4.25 V), higher than that of the pristine one (73.65%). The enhanced performances can be attributed to the use of LPAN to create a unique carbon layer upon graphite tailings to reconstruct surface and repair defects, and also to granulate an isotropic structure of secondary graphite particles, which can help to weaken the anisotropy of Li+ diffusion pathway and form a uniform, complete and stable solid-electrolyte-interface (SEI) on the surface of primary NGT fragments to promote a fast Li+ diffusion and suppress lithium metal dendrites upon charge and discharge.
Carbon aerogels prepared from renewable nano building blocks are rising-star materials and hold great promise in many fields. However, various defects formed during carbonization at high temperature disfavor the stress transfer and thus the fabrication of flexible carbon aerogel from renewable nano building blocks. Herein, a structural defect-reducing strategy is proposed by altering the pyrolysis route of cellulose nanofiber. Inorganic salt that inhibits the generation of tar volatilization during pyrolysis can prevent the formation of various structural defects. Microstructure with fewer defects can reduce stress concentration and remarkably enhance the compressibility of carbon aerogel, thus increasing the maximum stress retention of carbon aerogel. The carbon aerogel also has high stress sensor sensitivity and excellent temperature coefficient of resistance. The structural defect-reducing strategy will pave a new way to fabricate high-strength carbon materials for various fields.
While nickel(Ⅱ) complexes have been widely used as catalysts for carbon-carbon coupling reactions, the exploration of their photophysical and photochemical properties is still in the infancy. Here, a series of square-planar Ni(Ⅱ) complexes [(diNHC)NiX2] bearing chelating benzimidazole-based bis(N-heterocyclic carbene) ligands and varying anionic coligands (1, X = Cl; 2, X = Br; 3, X = I) are synthesized and structurally characterized. In solid state, both 1 and 2 exhibit orange-red photoluminescence under ambient conditions. The photophysical and electrochemical measurements along with density functional theory (DFT) calculations reveal that the low-energy emissions can be attributed to singlet excited states with ligand-to-ligand charge-transfer (LLCT) character. This work suggests that strong-field N-heterocyclic carbene ligands play a crucial role to achieve the luminescence of Ni(Ⅱ) complexes.
We have synthesized two copper nanoclusters (NCs) with a protection of the same ligand diphenylphosphino-2-pyridine (C17H14NP, dppy for short), formulated as Cu4(dppy)4Cl2 and Cu21(dppy)10, respectively. The former one bears a distorted tetrahedron Cu4 core with its six edges fully protected by chlorine and dppy ligands, while the latter presents a symmetric Cu21 core on which ten dppy molecules function as monolayer protection via well-organized monodentate or bidentate coordination. Interestingly, the Cu4(dppy)4Cl2 cluster exhibits a strong yellow emission at ~577 nm, while Cu21(dppy)10 displays dual emissions in purple (~368 nm) and green (~516 nm) regions respectively. In combination with TD-DFT calculations, we demonstrate the origin of altered emissions and unique stability of the two copper nanoclusters pertaining to the ligand coordination and metallic superatomic states.
The irregular defects and residual tumor tissue after surgery are challenges for effective breast cancer treatment. Herein, a smart hydrogel with self-adaptable size and dual responsive cargos release was fabricated to treat breast cancer via accurate tumor elimination, on-demand adipose tissue regeneration and effective infection inhibition. The hydrogel consisted of thiol groups ended polyethylene glycol (SH-PEG-SH) and doxorubicin encapsulated mesoporous silica nanocarriers (DOX@MSNs) double crosslinked hyaluronic acid (HA) after loading of antibacterial peptides (AP) and adipose-derived stem cells (ADSCs). A pH-cleavable unsaturated amide bond was pre-introduced between MSNs and HA frame to perform the tumor-specific acidic environment dependent DOX@MSNs release, meanwhile an esterase degradable glyceryl dimethacrylate cap was grafted on MSNs, which contributed to the selective chemotherapy in tumor cells with over-expressed esterase. The bond cleavage between MSNs and HA would also cause the swelling of the hydrogel, which not only provide sufficient space for the growth of ADSCs, but allows the hydrogel to fully fill the irregular defects generated by surgery and residual tumor atrophy, resulting in the on-demand regeneration of adipose tissue. Moreover, the sustained release of AP could be simultaneously triggered along with the size change of hydrogel, which further avoided bacterial infection to promote tissue regeneration.
Due to the limitations of conventional chemotherapy including side effects, poor prognosis, and drug resistance, there is an urgent need for the development of a novel multi-functional combined therapy strategy. Dopamine-modified oxaliplatin prodrug (OXA-DA) was successfully synthesized in this study to ameliorate the organ distribution of oxaliplatin for improving the drug efficacy and reducing toxic side effects, and OXA-DA was applied to develop a porous oxaliplatin cross-linked polydopamine nanoparticle for loading siPD-L1 to construct multifunctional nanoplatform. The multifunctional nanoplatform was modified with poly(2-ethyl-2-oxazoline) (PEOz), which occurred charge reversal in the tumor microenvironment, and exerted the lysosomal escape effect in tumor cells to improve the bioavailability of small interfering RNA targeting programmed cell death-ligand 1 (siPD-L1). The pH-responsive charge reversal, photothermal, biodegradation, lysosomal escape ability, PD-L1 protein degradation, toxicity properties and multiple antitumor effects were comprehensively evaluated in vitro and in vivo experiments. The findings indicated that OXA-DA-siPD-L1@PDA-PEOz excellently induced tumor cell necrosis and apoptosis as a result of the synergistic effect of chemo-photothermal therapy, and upregulated CD8+ T cells produced interferon-γ (IFN-γ) to further attack the tumor cells. In conclusion, the novel nanoplatform-mediated chemo/photothermal/immunotherapy has promising clinical applications in the treatment of malignant tumors.
White light emitting systems of pure organic materials have attracted extensive research interest due to their better compatibility and functional scalability. The reported organic white light materials are mainly based on the multi-channel emission regulation of the compound itself or the mixing of multicolor luminescence materials, but studies on the dependence between multicolor luminescence and the external environment are lacking, which limits the application of these materials in areas such as identification and sensing. This paper reports that the 4- or 3‑hydroxyl-substituted naphthalimides NapH1 and NapH2 form intermolecular hydrogen bonds with adjacent molecules in the environment, and undergo excited-state intermolecular proton transfer under irradiation, resulting in blue-yellow or blue-red dual fluorescence emission, respectively. Since the two compounds have different two-color luminescence channels and the two-color intensity ratio is affected by the environment, and the intermolecular hydrogen bond is determined by the hydrogen bond receptor, polarity, and temperature in the environment, the full spectrum from blue to red light and white light emission can be obtained by adjusting the mixing ratio of the two dyes and the solvent polarity and the ambient temperature. This environmentally sensitive white emission is used to detect the alkalinity of different papers, and the dyed paper can be used as a test strip for acid-base vapor detection.
In the process of electrocatalytic water splitting, the management of gaseous products is an important task. Timely detachment of gaseous products from the electrode surface and the electrolyte is beneficial to the reduction of energy consumption of the electrolytic cell. In the existing industrial electrolytic cells, the circulating pump drives the electrolyte flowing to discharge the gaseous products. Up to now, several much more advanced strategies have been explored to deal with the negative effects of bubbles. In this review, we summarized various strategies for bubble detachment, including electrode design, external field imposing and system upgrading. We also elaborated the principle, functional features, practicability, advantages and limitations of each method. Finally, challenges and perspectives are also provided for the further development of advanced bubbles detachment strategies for efficient hydrogen evolution.
Lithium (Li)–CO2 battery is rising as an attractive energy-storage system with the competence of CO2 conversion/fixation. However, its practical development is seriously hindered by the high overpotential. Herein, a rational design on a highly catalytic Li–CO2 battery electrode built by graphdiyne powder as a multi-functional laminar scaffold with anchored highly dispersed Ru nanoparticles is explored. The strong interaction between the abundant acetylenic bond sites of graphdiyne scaffold and Ru nanoparticles can effectively promote the electrochemical progress and reduce the voltage polarization. The unique channels architecture of the cathodic catalyst with enough space not only accelerates CO2 diffusion and electrons/Li+ transport, but also allows a large amount of accommodation for discharged product (Li2CO3) to assure an advanced capacity. The corresponding Li–CO2 battery displays an advanced discharged capacity of 15,030 mAh/g at 500 mA/g, great capacity retention of 8873 mAh/g at 2 A/g, high coulombic efficiency of 97.6% at 500 mA/g and superior life span for 120 cycles with voltage gap of 1.67 V under a restricted capacity of 1000 mAh/g at 500 mA/g. Ex/in-situ studies prove that synergy between Ru nanoparticles and acetylene bonds of GDY can boost the round-trip CO2RR and CO2ER kinetics.
Viruses are ubiquitous in human life. Some viruses can be used as vectors of genetic engineering and specific pesticides. Other viruses trigger a variety of diseases in humans, animals and plants, resulting in high infection rates and mortality. Therefore, convenient, accurate and rapid detection of viruses is of great significance for the diagnosis and treatment of subsequent diseases. In contrast to traditional methods of detection, which rely on time-consuming and complex techniques such as polymerase chain reaction (PCR), fluorescent probes and imaging methods generate real-time results, with high specificity, and have been widely used in viral detection. In this review, the application of viral fluorescent probes in analyzing the molecular structure, detection and biological imaging is discussed. In particular, we categorized the probes based on their specificity for human and plant viruses, reviewing the latest findings and analyzing their limitations. The potential of fluorescent molecular probes in the treatment of viral disease and environmental analysis, and their possible combinations with protein and immune technology are discussed.
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