Latest ArticlesA series of heterotrinuclear Ti2Ni(CO)n– (n = 6–9) carbonyls have been generated via a laser vaporization supersonic cluster source and characterized by mass-selected photoelectron velocity-map imaging spectroscopy. Quantum chemical calculations have been carried out to identify the structures and understand the experimental spectral features. The results indicate that a building block of Ti-Ti-Ni-C four-membered ring with the C atom bonded to Ti, Ti, and Ni is dominated in the n = 6–8 complexes, whereas a structural motif of Ti-Ti-Ni triangle core is preferred in n = 9. These complexes are found to be capable of simultaneously accommodating all the main modes of metal-CO coordination (i.e., terminal, bridging, and side-on modes), where the corresponding mode points to the weak, moderate, high CO bond activation, respectively. The number of CO ligands for a specific bonding mode varies with the cluster size. These findings have important implications for molecular-level understanding of the interaction of CO with alloy surfaces/interfaces and tuning the appropriate CO activation via the selection of different metals.
The biocompatibility and biodegradability of peptide self-assembled materials makes them suitable for many biological applications, such as targeted drug delivery, bioimaging, and tracking of therapeutic agents. According to our previous research, self-assembled fluorescent peptide nanoparticles can overcome the intrinsic optical properties of peptides. However, monochromatic fluorescent nanomaterials have many limitations as luminescent agents in biomedical applications. Therefore, combining different fluorescent species into one nanostructure to prepare fluorescent nanoparticles with multiple emission wavelengths has become a very attractive research area in the bioimaging field. In this study, the tetrapeptide Trp-Trp-Trp-Trp (WWWW) was self-assembled into multicolor fluorescent nanoparticles (TPNPs). The results have demonstrated that TPNPs have the blue, green, red and near infrared (NIR) fluorescence emission wavelength. Moreover, TPNPs have shown excellent performance in multicolor bioimaging, biocompatibility, and photostability. The facile preparation and multicolor fluorescence features make TPNPs potentially useful in multiplex bioanalysis and diagnostics.
Lithium-rich manganese-based material shows great potential as the high specific cathode materials due to its low cost, environmental friendliness, high operating voltage and simple preparation process. However, the poor capacity retention and cycling performance caused by its unstable structure during cycling restrict the commercialization. In this work, Li1.2Ni0.16Mn0.56Co0.08O2 was synthesized utilizing a Co-precipitation method and different amount of La(PO3)3 (La(PO3)3 = 2 wt%, 4 wt% and 6 wt%) was selected as the coating layer to resolve the above issues. During the calcination process, La(PO3)3 reacts with impurities such as LiOH and Li2CO3 on the lithium-rich surface to reduce the residual lithium on the surface, thus improving the interfacial stability, slowing down the corrosion of the electrolyte, and finally enhancing its electrochemical performance. The cathode materials coated with 4% of La(PO3)3 showed the best electrochemical performance in terms of capacity retention and cycling performance compared to the pristine NCM. The high initial discharge capacity of 214.21 mAh/g and capacity retention of 94.2% after 100 cycles at 0.1 C can be obtained. This work provides an effective strategy to protect the cathode from corrosion and will promote its further practical applications in high specific Li-ion batteries.
The construction of highly active catalysts for methanol oxidation reaction (MOR) is central to direct methanol fuel cells. Tremendous progress has been made in transition metal phosphides (TMPs) based catalysts. However, TMPs would be partially damaged and transformed into new substances (e.g., Pt-M-P composite, where M represents a second transition metal) during Pt deposition process. This would pose a large obstacle to the cognition of the real promoting effects of TMPs in MOR. Herein, Co2P co-catalysts (Pt-P/Co2P@NPC, where NPC stands for N and P co-doped carbon) and Pt-Co-P composite catalysts (Pt-Co-P/NPC) were controllably synthesized. Electrocatalysis tests show that the Pt-Co-P/NPC exhibits superior MOR activity as high as 1016 mA/mgPt, significantly exceeding that of Pt-P/Co2P@NPC (345 mA/mgPt). This result indicates that the promoting effect is ascribed primarily to the resultant Pt-Co-P composite, in sharply contrast to previous viewpoint that Co2P itself improves the activity. Further mechanistic studies reveal that Pt-Co-P/NPC exhibits much stronger electron interaction and thus manifesting a remarkably weaker CO absorption than Pt-P/Co2P@NPC and Pt/C. Moreover, Pt-Co-P is also more capable of producing oxygen-containing adsorbate and thus accelerating the removal of surface-bonded CO*, ultimately boosting the MOR performance.
A regiodivergent hydrophosphorylation of enynes with phosphites has been developed using earth-abundant nickel catalyst. The manipulation of regioselectivity can be achieved by regulating the insertion order of alkyne bonds with (RO)2P(O)–Ni–H or R2P(O)O–Ni–H species, respectively. Under the Ni/Xantphos catalysis, 4,1-hydrophosphorylation is selectively obtained while the adding of acid can promote reactions towards 1,2-addition. By employing an additional Pd–H catalysis, 2,1-hydrophosphorylation is also an accessible task in one-pot reaction. Mechanistic studies and analysis have also been performed to interpret the origin of the regioselective regulation. This work highlights the arts in accessing different regioisomers by diverting common elementary reaction steps.
As a high-flux operation mode of thin film composite-forward osmosis (TFC-FO) membrane, active layer facing draw solution (AL-DS) mode suffers from the severe membrane fouling tendency, which is not addressed well. Here, we introduced a photocatalyst (Anatase titanium dioxide, A-TiO2) onto the support layer of TFC-FO membrane via the bonding of polydopamine (PDA) and polytetrafluoroethylene (PTFE), and prepared two photocatalytic membranes, A-TiO2/PDA@TFC and A-TiO2/PTFE@TFC. Compared with the pristine TFC-FO membrane, both A-TiO2/PDA @TFC and A-TiO2/PTFE@TFC had an improved water permeability (10.5 L m−2h−1 and 9.5 L m−2 h−1, respectively) and reduced reverse NaCl flux salt (0.8 g m−2 h−1 and 0.7 g m−2 h−1, respectively) in the AL-DS mode using 1 mol/L NaCl as draw solution and pure water as feed solution. Moreover, in the 16 h fouling experiment using 200 ppm bovine serum albumin (BSA) solution as a representative pollutant, the flux decline rate of both photocatalytic membranes was dramatically alleviated from 39.7% and 21.7% in the darkness to 8.5% and 9.7% under UV irradiation, respectively, indicating a significant anti-fouling capacity of photocatalytic effect. In all, the presence of A-TiO2 endowed membrane with high permeability, high rejection efficiency and excellent anti-fouling capacity under UV spotlight. As bonding agent, PTFE provided the modified membrane with a high photocatalytic effect and high self-cleaning capacity, while PDA increased the membrane permeability and protected membrane against photocatalytic damage. This work provides a simple and feasible method to improve the anti-fouling capacity of TFC-FO membrane in AL-DS mode.
Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxene-pended base ligands. Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(p-phenylene-vinylene) (u-COPV) suspended by the truxene skeleton, the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission (AIE) accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation. In particular, the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.
As an attractive C1 synthon, carbon dioxide (CO2) has been extensively used in organic synthesis to produce carboxylic acids. In this research, stereoselective electrochemical carboxylation of α,β-unsaturated sulfones has been developed under transition-metal-free conditions. All the cinnamic acids and the derivatives are obtained selectively in the E-configuration. Besides, arylpropiolates also can be produced from alkynyl sulfones.
Defect passivation is one of the important strategies to improve the efficiency and stability of perovskite solar cells. In this work, 2,6-di–tert–butyl–4-methylphenol (BHT) as antioxidant was introduced into the perovskite precursor solution to improve the quality of the prepared perovskite films, so that these films performed a larger and uniform grain size. Moreover, the −OH functional group in BHT interacts with I−, thus reducing the density of defect states and inhibiting the non-radiative recombination. The presence of hydrophobic groups in BHT protects the film from moisture erosion and improves the long-term stability of PSCs devices. The maximum photoelectric conversion efficiency of the constructed ITO/SnO2/BHT-MAPbI3/Carbon device is 16.88%, and the unpackaged cell maintains the initial efficiency of 99.3% after 698 h of storage under the environmental condition of 30% humidity. This work provides an efficient approach to improve the performance of printable hole transport layer-free carbon electrode perovskite solar cells.
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