Controllable Construction of Amino-Functionalized Dynamic Covalent Porous Polymers for High-Efficiency CO2 Capture from Flue Gas

The design of high-efficiency CO₂ adsorbents with low cost, high capacity, and easy desorption is of high significance for reducing carbon emissions, which yet remains a great challenge. This work proposes a facile construction strategy of amino-functional dynamic covalent materials for effective CO₂ capture from flue gas. Upon the dynamic imine assembly of N-site rich motif and aldehyde-based spacers, nanospheres and hollow nanotubes with spongy pores were constructed spontaneously at room temperature. A commercial amino-functional molecule tetraethylenepentamine could be facilely introduced into the dynamic covalent materials by virtue of the dynamic nature of imine assembly, thus inducing a high CO₂ capacity (1.27 mmol·g⁻¹) from simulated flue gas at 75 °C. This dynamic imine assembly strategy endowed the dynamic covalent materials with facile preparation, low cost, excellent CO₂ capacity, and outstanding cyclic stability, providing a mild and controllable approach for the development of competitive CO₂ adsorbents.     

Mechanically strong and stiff supramolecular polymers enabled by fiber reinforced long-chain alkane matrix

Fiber-reinforced-concrete (FRC) mechanism refers short discrete fibers that are uniformly distributed and randomly oriented, which offers an effective way to improve the mechanical performance of concrete. In the design of supramolecular polymers, an analogous concept of FRC appears to have been considered very rarely-although fibrous structure has been frequently observed/generated during the supramolecular polymerization. In this work, we apply the alkane thermosets, octadecane (C₁₈H₃₈) and tetracosane (C₂₄H₅₀), taking the role of “concrete”, and the low-molecular-weight monomer with long alkyl chains as the essential “fiber” component, to fabricate the “fiber reinforced supramolecular polymer”. Very much like FRC mechanism in material science, the resulting fiber reinforced supramolecular polymer thus exhibit unusually high mechanical strength and stiffness, which is unprecedented in the conventional supramolecular strategy.     

Ultrafast synthesis of near-infrared-emitting aqueous CdTe/CdS quantum dots with high fluorescence

The traditional aqueous route to synthesis CdTe/CdS Core/shell (c/s) quantum dots (QDs) via decomposition of Cd-thiol complexes is usually time consuming. Herein, an ultrafast and facile aqueous synthetic approach under atmospheric pressure for CdTe/CdS c/s QDs with emission from the green to the near-infrared window (535–820 nm) is reported. With purified CdTe core QDs diluted in solution of Cd-3-mercaptopropionic acid (MPA) complexes, CdTe/CdS c/s QDs with emission wavelengths at 700 and 800 nm can be obtained within 20- and 45-min refluxing under the optimized experimental conditions, respectively. This is the most rapid way to prepare CdTe/CdS c/s QDs in aqueous phase, and the obtained QDs were highly luminescent without postsynthesis treatment. The influences of various experimental factors, including Cd²⁺ concentration, MPA-to-Cd ratio, pH value, and dilution ratio on the growth rate and luminescent properties of the obtained CdTe/CdS c/s QDs, have been taken into consideration. The three processes “purification-dilution-addition” ensure the synthesis environment with high pH value and low core concentration and have a marked impact on the rapid synthesis rate and the resulting high fluorescence of CdTe/CdS c/s QDs.     

利用自由基引发的1,2-炔基迁移实现非活性烯烃的炔膦酰化

研究了1,4-烯炔衍生物与二芳基膦氧化物在银介导下发生的炔酰化反应.该反应利用自由基引发的1,2-炔基迁移策略合成了一系列γ-酮膦氧化物,产率适中.该反应机理可能涉及膦中心自由基与乙烯基的加成、3-exo-dig环化和1,2-炔基迁移等连续的过程,一步形成了C-P、C-C键等化学键,实现了非活性烯烃的双官能化.     

Bioinspired and Mechanically Strong Fibers Based on Engineered Non‐Spider Chimeric Proteins

Silk‐protein‐based fibers have attracted considerable interest due to their low weight and extraordinary mechanical properties. Most studies on fibrous proteins focus on the recombinant spidroins, but these fibers exhibit moderate mechanical performance. Thus, the development of alternative structural proteins for the construction of robust fibers is an attractive goal. Herein, we report a class of biological fibers produced using a designed chimeric protein, which consists of the sequences of a cationic elastin‐like polypeptide and a squid ring teeth protein. Remarkably, the chimeric protein fibers exhibit a breaking strength up to about 630 MPa and a corresponding toughness as high as about 130 MJ m^?3, making them superior to many recombinant spider silks and even comparable to some native counterparts. Therefore, this strategy is a novel concept for exploring bioinspired ultrastrong protein materials through the development of new types of structural chimeric proteins.     

Photo-driven water splitting photoelectrochemical cells by tandem organic dye sensitized solar cells with I−/I3− as redox mediator

Dye-sensitized photoelectrochemical tandem cells have shown the promise for light driven hydrogen production from water owing to the low cost,wide absorption spectra in the visible region and ease to process of their constitutive photoelectrode materials.However,most photo-driven water splitting photoelectrochemical cells driven by organic dye sensitized solar cells exhibit unsatisfactory hydrogen evolution rate,primarily attributed to their poor light capturing ability and low photocurrent performance.Here we present the construction of a tandem system consisting of an organic blue-colored S5 sensitizer-based dyesensitized photoelectrochemical cell(DSPEC) wired in series with three spectral-complemental dyes BTA-2,APP-3 and APP-1 sensitizers-based dye-sensitized solar cell(DSC),respectively.The two spectral-complemental chromophores were used in DSC and DSPEC to ensure that the full solar spectrum could be absorbed as much as possible.The results showed that the photocurrent of tandem device was closely related to the open-circuit voltage(Voc) of sensitized DSC,in which the tandem configuration consisting of S5 based DSPEC and BTA-2 based DSC gave the best photocurrent.On this basis,tandem device with the only light energy and no external applied electrical bias was further constructed of BTA-2 based 2-junction DSC and S5 based DSPEC and obtained a photocurrent of 500 μA cm-2 for hydrogen generation.Furthermore,I-/I3-was used as a redox couple between dye regeneration and O2 production on the surface of Pt-IrO2/WO3.The strategy opens up the application of pure organic dyes in DSC/DSPEC tandem device.     

Re‐Appearance of Cooperativity in Ultra‐Small Spin‐Crossover [Fe(pz){Ni(CN)4}] Nanoparticles

A reverse nanoemulsion technique was used for the elaboration of [Fe(pz){Ni(CN)₄}] nanoparticles. Low‐temperature micellar exchange made it possible to elaborate ultra‐small nanoparticles with sizes down to 2 nm. When decreasing the size of the particles from 110 to 12 nm the spin transition shifts to lower temperatures, becomes gradual, and the hysteresis shrinks. On the other hand, a re‐opening of the hysteresis was observed for smaller (2 nm) particles. A detailed ⁵⁷Fe Mössbauer spectroscopy analysis was used to correlate this unusual phenomenon to the modification of the stiffness of the nanoparticles thanks to the determination of their Debye temperature.     

Discovery of a new nontoxic cuprate superconducting system Ga-Ba-Ca-Cu-O

Superconductivity is observed in a new nontoxic cuprate system Ga-Ba-Ca-Cu-O,with T_c=82 K for Ga Ba_2Ca_5Cu_6O_(14+δ)(Ga-1256)and T_c=116 K probably for Ga Ba_2Ca_3Cu_4O_(10+δ)(Ga-1234)or Ga Ba_2Ca_2Cu_3O_(8+δ)(Ga-1223),respectively.All compounds are fabricated by solid state reaction method under high pressure and high temperature.Samples are characterized by resistivity,magnetization and X-ray diffraction(XRD)measurements.The temperature dependence of magnetization measured in both zero-field-cooled and field-cooled processes on one sample(S1)shows two superconducting transitions at about 82 K and113 K.The estimated shielding fraction for the phase with T_cof 82 K is about 67%,while the fraction for another phase with T_(c )of 113 K is quite small.The XRD Rietveld refinement for S1 indicates two main phases existing in the sample,Ga-1256 with fraction of about 58%and non-superconducting Ca_(0.85)Cu O_2with fraction of about 42%respectively.Thus,we can conclude the superconducting phase with transition temperature of 82 K is due to Ga-1256.The resistivity measurement also confirms the superconductivity for S1,and the resistivity reaches zero at about 82 K.The temperature dependence of magnetization for another sample(S2)shows much higher superconducting shielding fraction for the phase with T_cof 116 K,which may be a promising prospective for the synthesis of Ga-1234 or Ga-1223 phase.