Latest ArticlesMetal-nitrogen-carbon materials (M-N-C) are non-noble-metal-based alternatives to platinum-based catalysts and have attracted tremendous attention due to their low-cost, high abundance, and efficient catalytic performance towards the oxygen reduction reaction (ORR). Among them, Fe-based materials show remarkable ORR activity, but they are limited by low selectivity and low stability. To address these issues, herein, we have synthesized FeCu-based M-N-C catalysts, inspired by the bimetal center of cytochrome c oxidase (CcO). In acidic media, the selectivity was notably improved compared with Fe-based materials, with peroxide yields less than 1.2% (< 1/3 of the hydrogen peroxide yields of Fe-N-C catalysts). In addition to Cu-N-C catalysts which can catalytically reduce hydrogen peroxide, the reduction current of hydrogen peroxide using FeCu-N-C-20 exceeded that of Fe-N-C by about 6% when the potential was greater than 0.4 V. Furthermore, FeCu-based M-N-C catalysts suffered from only a 15 mV attenuation in their half-wave potentials after 10, 000 cycles of accelerated degradation tests (ADT), while there was a 30 mV negative shift for Fe-N-C. Therefore, we propose that the H2O2 released from Fe-Nx sites or N-doped carbon sites would be reduced by adjacent Cu-Nx sites, resulting in low H2O2 yields and high stability.
Transition metal phosphide (TMP) based electrocatalysts possessing special crystal and electronic structures attract broad attention in the field of electrocatalysis. Immense effort is made to optimize TMP catalysts aiming to satisfy the electrochemical catalysis performance. In this work, an environmentally friendly in situ green phosphating strategy and spatial limiting effect of the RuCo precursor is employed to fabricate the ruthenium nanoclusters anchored on cobalt phosphide hollow microspheres (Ru NCs/Co2P HMs). The obtained Ru NCs/Co2P HMs electrocatalysts exhibit high hydrogen evolution reaction (HER) activity at wide pH ranges, which require an overpotential of 77 mV to achieve the current density of 10 mA/cm2 in 0.5 mol/L H2SO4 and 118 mV in 1.0 mol/L KOH. Besides, the multifunctional Ru NCs/Co2P HMs exhibit good oxygen evolution reaction (OER) activity with an overpotential of 197 mV to reach the current density of 10 mA/cm2 in 0.5 mol/L H2SO4, which is below that of the commercial RuO2 electrocatalyst (248 mV). A two-electrode electrolyzer is assembled as well, in acid electrolyte, it achieves a current density of 10 mA/cm2 at a voltage of 1.53 V, which is superior to that of the benchmark of precious metal-based electrolyzer (1.58 V).
One 6-metal Zn-Nd complex [Zn2Nd4L2(OAc)10(OH)2(CH3OH)2] (1) with Schiff base ligand bis(3-methoxysalicylidene)ethylene-1,2-phenylenediamine (H2L) was constructed, and it has nanoscale rectangular structure (8×11×28 Å). Excited by ligand-centered absorption bands, 1 shows NIR emission of Nd3+ ion. Interestingly, 1 exhibits lanthanide luminescent response towards metal ions, especially to alkali metal ions (Li+, Na+ and K+) at ppm level.
The synthesis of borylated organofluorines is of great interest due to their potential values as synthons in modular construction of fluorine-containing molecules. Reported herein is a rhodium-catalyzed hydroboration of aryl gem-difluoroalkenes leading to a series of α-difluoromethylated benzylborons. The use of cationic rhodium catalyst and a biphosphine ligand with large bite angle was crucial for reactivity by offering good regioselectivity and diminishing the undesired β-F elimination. Preliminary derivatizations of the products were conducted to showcase the utility of this protocol.
Carbon nanotubes (CNTs), as one-dimensional nanomaterials, show great potential in energy conversion and storage due to their efficient electrical conductivity and mass transfer. However, the security risks, time-consuming and high cost of the preparation process hinder its further application. Here, we develop that a negative pressure rather than a following gas environment can promote the generation of cobalt and nitrogen co-doped CNTs (Co/N-CNTs) by using cobalt zeolitic imidazolate framework (ZIF-67) as a precursor, in which the negative pressure plays a key role in adjusting the size of cobalt nanoparticles and stimulating the rearragement of carbon atoms for forming CNTs. Importantly, the obtained Co/N-CNTs, with high content of pyridinic nitrogen and abundant graphitized structure, exhibit superior catalytic activity for oxygen reduction reaction (ORR) with half-wave potential (E1/2) of 0.85 V and durability in terms of the minimum current loss (2%) after the 30, 000 s test. Our development provides a new pathway for large-scale and cost-effective preparation of metal-doped CNTs for various applications.
Water-soluble thermoresponsive polymers present either upper critical solution temperature (UCST) or lower critical solution temperature (LCST) depending on the location of their miscibility range with water at high temperatures or at low temperatures. Compared with LCST polymers, the water-soluble UCST polymers are still less explored until now. In this work three copolymers of P(AAm-co-GAA) were synthesized by copolymerizing two acrylamide monomers, acrylamide (AAm) and acrylamide functionalized with natural glycyrrhetinic acid (GAA), using reversible addition-fragmentation chain transfer (RAFT) polymerization. These copolymers exhibited the typical UCST thermoresponsive behavior, and their phase transition temperatures could be easily tuned to around 37 ℃ for potential biological applications. Moreover, the UCST of P(AAm-co-GAA) can be adjusted not only by the content of glycyrrhetinic acid (GA) and polymer concentrations, but also by the host-guest interactions between GA and cyclodextrins (β- and γ-CD). The suitable value of UCST and the biocompatible nature of GA and CDs may endow these copolymers with practical applications in biomedical chemistry
The effects of concentration and an oriented external electric field on the transformations of hydrogenbonded structures of trimesic acid (TMA) and terephthalic acid (TPA) have been investigated at a liquid–solid interface by scanning tunneling microscopy (STM). The triangular periodic TMA framework can be transformed into a flower-like structure by changing the STM sample bias sign in situ. Networks of TMA and TPA are porous at a negative substrate bias, but typically change to relatively compact forms when the polarity of the applied bias is reversed. This change is reversible if the applied bias is reversed. The effects have potentials to locally control the capture and release of analytes in host-guest systems and the 2D morphology in multicomponent layers.
Fragrances are widely used in cosmetics, apparel and detergents. However, the rapid evaporation of the aroma shortens the useful life of the aromatic product. Therefore, improving the fragrance retention time of aromatic products and prolonging the service life of aromatic products are the key scientific problems that need to be solved in current aromatic products. In this study, zwitterionic comb-like lipid polymers were synthesized to encapsulate the fragrance molecule linalool. The results showed that the zwitterionic comb lipid molecules were capable of encapsulating more linalool than linear lipid molecules. At the same time, the zwitterionic comb-like lipid molecules also limited the slow release rate of the aroma, thereby increasing the fragrance retention time of the nano-fragrance.
Stimulus responsive materials can provide a variety of desirable properties in one equipment unit, such as optoelectronic devices, data communications, actuators, memories, sensors and capacitors. However, it remains a large challenge to design such stimulus responsive materials, especially functional materials having both dielectric switch and second harmonic generation (SHG). Here, a new stimuli-responsive switchable material [(CH3)3N(CH2)2Cl]2[Mn(SCN)4(H2O)2] was discovered as a potential second-harmonic generation (SHG) dielectric switch. It is worth noting that it has SHG characteristics before and after undergoing reversible high-temperature phase transitions. In this work, we successfully refined the tetramethylammonium cation to obtain a quasi-spherical cation, which is tetramethylchloroethyl-amine (TMCEM) cation. By substituting H with a halogen, the increased steric hindrance of the molecular makes energy barrier increased, resulting in the reversible high-temperature phase transition. At the same time, the interactions of quasi-spherical cations and [Mn(SCN)4(H2O)2]2- anions affect a non-centrosymmetric structure to induce the SHG effect. These findings provide a new approach to design novel functional switch materials.
A Mn(Ⅲ) mediated radical reaction of new designed multi-functionalized 2-isocyano-6-alkenyl(alkynyl) benzonitriles with arylboronic acids has been developed. This reaction provides a method for the synthesis of pyrroloisoquinoline derivatives through the formation of two C—C bonds and one C—N bond via radical cascade cyclization in one step.
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