Latest ArticlesMulti-response metal cluster supercrystal materials, which can simultaneously display various such as color, photoluminescence, changes by bearing only one stimulus, have huge potential as stimuli-responsive intelligent material, but are rarely reported. Here, we report three Cu8 cluster supercrystals, Cu8-1, Cu8-2, and Cu8-3, with homologous cluster molecule units [Cu8(PNP)3(EPPTA)6](PF6)2 but distinct packing. These supercrystals display bright µs-long photoluminescence with a high quantum yield of up to 26.6% in solid-state at room temperature and aggregation-induced emission (AIE) characteristic. Superior thermal stability and blue-excitable bright yellow emission make Cu8-3 serve as a yellow phosphor for white light-emitting diode. Furthermore, upon being stimulated by solvent vapor and temperature, reversible supercrystal-to-supercrystal transformations can be witnessed accompanied by remarkable color and luminescence switching. This work not only provides a kind of Cu cluster supercrystal model but also motivates the further development of metal clusters in multi-response materials.
A novel approach was developed to fabricate a label-free electrochemical aptasensor for specific detection of mercury ions (Hg2+). This involved modifying polylysine (PLL)-coated black phosphorus-porous graphene (BP-PG) nanocomposites (PLL/BP-PG) onto the surface of glassy carbon electrodes (GCE), which were further modified with gold nanoparticles (AuNPs) to combine with a thiolated aptamer (Apt) capable of specifically recognizing Hg2+. BP-PG was synthesized using the solvothermal method and covalently bonded to form BP-PG nanosheets, resulting in significant enhanced electrochemical properties of the PLL/BP-PG composite. Furthermore, the PLL/BP-PG composite was improved environmental stability of BP and provided a considerable quantity of -NH2 for bonding to AuNPs firmly by assembling. The physical properties and electrochemical behavior of the substrate materials were investigated using various characterization techniques, and analytical parameters were optimized. It is shown that, the Apt/AuNPs/PLL/BP-PG/GCE had a linear response (R2 = 0.999) with good selectivity and high sensitivity over the Hg2+ range of 1–10,000 nmol/L. The proposed sensor has a detection limit of 0.045 nmol/L and can be employed for detecting of Hg2+. It also obtained satisfying results in river water, soil and vegetable samples.
Oxygen evolution reaction (OER), occurring at the anode of electrochemical water splitting requires a comprehensive understanding of oxygen electrocatalysis mechanism to optimize its efficiency. Atomically dispersed transition metal supported by nitrogen-doped carbon is featured with excellent catalytic performance. Herein, we report a Mg/Co bimetal site which utilizes Mg 3p electrons with strong binding of *OH (the first key reaction intermediates in the free energy diagram) to trigger the OER reaction and Co 3d itinerant character to regulate the binding strength of *O. Benefiting from the fine-tuned adsorption/desorption possesses, the optimized catalyst delivers superior OER activity with low overpotential, i.e., 310 mV at a current density of 10 mA/cm2 and 455 mV at 100 mA/cm2. Moreover, the current density is able to be maintained at 10 mA/cm2 for 10 h, consistent with the theoretical simulations for oxidization process, which demonstrates stable configurations after multiple *OH modification, revealing robust applicability in alkaline medium.
This review profiles twelve fluorine-containing drugs approved by the US Food and Drug Administration (FDA) for the clinic in 2023. These small molecule drugs represent such therapeutic areas as cancer, neuromuscular disorder, immunodeficiency, virology, and infectious diseases. Medicinal chemistry discovery, biological activity, and synthetic routes have been discussed for each drug. Also, new trends in structural positioning, functionality, and degree of fluorination are discussed. Besides fluorination, the importance of amino acid residues and chirality in the design of new pharmaceuticals is highlighted.
Conventionally, organic radicals adhere to the Aufbau principle, the energy level of the singly occupied molecular orbital (SOMO) is not below the highest occupied molecular orbital (HOMO), but somewhat abnormal phenomena have appeared recently. In this study, we introduce a novel strategy by incorporating unique NHC-Au-X units into a tris(2,4,6-trichlorophenyl)methyl (TTM) system to create metal-involved open-shell complexes, denoted as TTM-NHC-Au-X (X = I, Br, or Cl). Density-functional theory calculations were used to predict an inversion in the energy of the SOMO and highest doubly occupied molecular orbital (HOMO) of TTM-NHC-Au-I, which is supported by experimental results. Organometallic radicals TTM-NHC-Au-X demonstrated distinct properties with different coordinated halides. The radical behaviors have been investigated by EPR, UV–vis spectroscopy and cyclic voltammetry, additional structural information provided by structurally comparing related the precursor complexes given by X-ray crystallography. TTM-NHC-Au-I with SOMOHOMO conversion (SHC) features a highly thermal decomposition temperature up to 305 ℃. Furthermore, the photostability of TTM-NHC-Au-I was found to be 75 and 23 times greater than that of TTM-NHC-Au-Br and TTM-NHC-Au-Cl, respectively. These findings provide valuable insights into the structural and electronic design principles governing the occurrence of SOMOHOMO conversion in open-shell systems.
Effective design of nanoheterostructure anode with high ion/electron migration kinetics can give electrode with superior electrochemical performance. However, the design and preparation of nanoheterostructure composites with high-capacity and long cycling life in half and pouch full cells remain a big challenge. Here, a novel micro-pore MnS/Mn2SnS4 heterostructure nanowire were in situ encapsulated into the N and S elements co-doped amorphous carbon tubes (abbreviated as (MnS/Mn2SnS4)@N,S-ACTs) and showed superior energy storage properties in Na-/Li-ion half cells and pouch full cells. The Na-/Li-storage capabilities improvement are attribute to the strong synergistic effect between MnS/Mn2SnS4 heterostructure and N,S-ACTs protective layer, the former induces an local built-in electric field between Mn2SnS4 and MnS during charging/discharging, accelerating interfacial ion/electron diffusion dynamics, the latter effective maintains the morphology and volume evolution during Na+/Li+ charging/discharging, achieving a long-term cycling stability (e.g., high discharge capacity of 79.2 mAh/g with the capacity retention of 79.3% can be gained after 2200 cycles at 3 C in (MnS/Mn2SnS4)@N,S-ACTs//LiFePO4 pouch full cells; a high capacity of ~34 mAh/g at 10 C can be got with a Coulombic efficiency of 100% after 1000 cycles in pouch (MnS/Mn2SnS4)@N,S-ACTs//Na3V2(PO4)2O2F full cells.
Sodium (Na) metal batteries have gained increasing attention more recently, owing to their high energy densities and cost efficiencies, but are severely handicapped by the unsatisfactory Coulombic efficiency (CE) and cycling stability stemming from dendrite growth on Na anodes. In this study, we developed a strategy of direct ink writing (DIW) 3D printing combined with electroless deposition to construct a hierarchical Cu grid coated with a dense nanoscale Ag interfacial layer as the host material for Na plating. The sodiophilic Ag interface contributes to a fall in the Na nucleation energy, hence enabling uniform Na deposition on each 3D-printed filament. The constructed 3D-printed structure can effectively moderate the electric-field distribution and lower the local current density for relieving Na inhomogeneous growth, as confirmed by finite element simulation and Na plating/stripping morphology evolution results. In particular, the unique 3D structure also promotes the lateral growth of Na, thus the volume change of Na metal was accommodated to stabilize the solid electrolyte interphase (SEI). As a result, the CE of the half-cell can reach 99.9% at the current density of 1 mA/cm2 after 300 cycles and the full-cell exhibits outstanding electrochemical performance (capacity retention of 91.0% after 500 cycles at 2 C).
In 2023, The MOE Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important results in the five research directions. First, for controllable catalytic polymerization, a new silicon-centered organoboron binary catalyst was developed for copolymerization of epoxides, and a series of cooperative organocatalysts were proposed for ring-opening copolymerization of chalcogen-rich monomers. Second, with respect to microstructure and rheology, axially encoded metafiber demonstrated its capacity for integrating multiple electronics, while artificial nacre materials showed improved strength and toughness due to interlayer entanglement. Third, concerning separating functional polymers, interfacial polymerization was monitored via aggregation-induced emission, and vacuum filtration was applied to assist interfacial polymerization. Fourth, in terms of biomedical functional polymers, we designed antibacterial materials such as a novel quaternary ammonium salt that enables polyethylene terephthalate recycling and its antibacterial function, nanozyme-armed phage proved its efficiency in combating bacterial infection, and also transition metal nanoparticles showed capacities in antibacterial treatments. We also made achievements in biomedical materials, including polymeric microneedles for minimally invasive implantation and functionalization of cardiac patches, as well as ROS-responsive/scavenging prodrug/miRNA balloon coating to promote drug delivery efficiency. Besides, methods and mechanisms of RNA labeling has been developed. Fifth, about photo-electro-magnetic functional polymers, through-space conjugation was successfully manipulated by altering subunit packing modes, room-temperature phosphorescent hydrogels were synthesized via polymerization-induced crystallization of dopant molecules, and single crystals of both fullerene and non-fullerene acceptors were grown in crystallized organogel, with their photodetection performance further explored. The related works are reviewed in this paper.
Rare earth ions (RE3+)-doped double perovskites have attracted tremendous attention for its fascinating optical properties. Nevertheless, RE3+ generally exhibits poor photoluminescence quantum yield (PLQY) for their parity-forbidden 4f-4f transition and the low doping concentration. Herein, we reported Sb3+/Sm3+-codoped rare earth-based double perovskite Cs2NaLuCl6 that enables efficient visible and near-infrared (NIR) emission, which stems from self-trapped exciton (STE) and Sm3+, respectively. Benefit from up to 72.89% energy transfer efficiency from STE to Sm3+ and high doping concentrations due to similar ionic activity between Sm3+ and Lu3+, thus eruptive PLQY of 74.58% in the visible light region and 23.12% in the NIR light region can be obtained. Moreover, Sb3+/Sm3+-codoped Cs2NaLuCl6 exhibits tunable emission characteristic in the visible light region under different excitation wavelengths, which can change from blue emission (254 nm excitation) to white emission (365 nm excitation). More particularly, only the NIR emission can be captured by the NIR camera when a 700 nm cutoff filter is added. The excellent stability and unique optical properties of Sb3+/Sm3+-codoped Cs2NaLuCl6 enable us to demonstrate its applications in NIR light-emitting diode, triple-mode fluorescence anti-counterfeiting and information encryption. These findings provide new inspiration for the application of rare earth-based double perovskite in optoelectronic devices.
The hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) are the two half reactions that make up the over water splitting reaction. Increasing oxygen evolution reaction rate wound immensely raise the efficiency of over water splitting reaction because it is the rate limiting reaction in water splitting reaction. The key to improve OER performance is the development and utilization of advanced catalysts. As one of the most potential catalysts for HER, it has gradually attracted the attention of researchers in the aspect of catalytic OER. It is very necessary to review the research progress of Transition metal dichalcogenides (TMDs) in catalytic OER to promote the research process in the field. In this review, we comprehensively and systematically summarized the strategies to improve TMDs electrocatalytic OER. First of all, structural regulation of TMDs-based electrocatalyst was summarized in detail, mainly including size engineering, defect engineering, doping engineering, phase engineering and heterojunction engineering. Once more, magnetic field regulation as a representative of external field regulation to improve TMDs electrocatalytic OER performance was discussed in depth. Last but not least, the strategies to improve TMDs electrocatalytic OER is prospected and some views on the development of this field are also put forward, which are expected to enhance the catalytic efficiency of TMDs for OER.
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