Constructing responsive and adaptive materials by dynamic covalent bonds is an attractive strategy in material design. Here, we present a kind of dynamic covalent polyureas which can be prepared from the highly efficient polyaddition reaction of pyrazoles and diisocyanates at ambient temperature in the absence of a catalyst. Owing to multiphase structural design, poly(pyrazole-ureas) (PPzUs) show excellent mechanical properties and unique crystallization behavior. Besides, the crosslinked PPzUs can be successfully recycled upon heating (~130 °C) and the molecular-level blending of polyurea and polyurethane is realized. Theoretical studies prove that the reversibility of pyrazole-urea bonds (PzUBs) arises from the unique aromatic nature of pyrazole and the N-assisting intramolecular hydrogen transfer process. The PzUBs could further broaden the scope of dynamic covalent bonds and are very promising in the fields of dynamic materials.

A highly enantioselective synthesis of indolines by asymmetric hydrogenation of 1H-indoles and 3H-indoles at ambient temperature and pressure, catalyzed by chiral phosphine-free cationic ruthenium complexes, has been developed. Excellent enantio- and diastereoselectivities (up to >99 % ee, >20:1 d.r.) were obtained for a wide range of indole derivatives, including unprotected 2-substituted and 2,3-disubstituted 1H-indoles, as well as 2-alkyl- and 2-aryl-substituted 3H-indoles.

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Super black materials with extremely low reflectance and high absorption of incident light are crucial in various applications with strict optical requirements. However, the existing super black materials suffer from technical complexity in practical use whereas the underlying physics of their ultralow reflectance is still unclear. Herein, hierarchical porous carbon spheres are prepared using poly­(vinylidene chloride-co-vinyl chloride) as a precursor. Dehydrochlorination treatment has proved to be very crucial for the morphology robustness of the porous polymer spheres during carbonization process. Coatings cast from the dispersion of these carbon spheres exhibit a hemispherical reflectance of <0.2% in the visible region and <0.3% in the range of 300–2000 nm, and the lowest reflectance of 0.14% can be reached. This super black coating has great advantages in its easy availability of starting materials, low equipment requirement, and high adaptability onto various substrates. Besides, a theoretical investigation suggests that a small scatterer size and low volume-filling ratio are the two most essential factors in realizing ultralow reflectance, which also offers an instructive guidance for the rational design of super black materials.

The first highly effective and enantioselective hydrogenation of quinolines catalyzed by chiral cationic Ru-diamine complexes in undegassed water was developed.

The construction of a single polymer network with extreme stretchability, relatively high mechanical strength, and fast and facile autonomous room-temperature self-healing capability still remains a challenge. Herein, supramolecular polymer networks are fabricated by synergistically incorporating metal–ligand and hydrogen bonds in poly­(propylene glycol) (PPG). The representative specimen, PPG-Im-MDA-1.5-0.25-Cu, shows a combination of notable mechanical properties involving an extreme stretching ratio of 346 ± 14× and a Young’s modulus of 2.10 ± 0.14 MPa, which are superior to the previously reported extremely stretchable polymeric materials. Notably, the destroyed specimen can fully recover mechanical performances within 1 h. The tunability of mechanical properties and self-healing capability has been actualized by merely tailoring the content of a chain extender. The application of the as-prepared supramolecular PPG network in constructing a flexible and self-healable conductor has been demonstrated. This strategy provides some insights for preparing extremely stretchable and self-healable polymeric materials.

To investigate the detailed mechanisms for lignite methanolysis, we used ReaxFF reactive force field to perform a series of molecular dynamics simulations (MDSs) on a unimolecular model compound. The α-O-4 and β-O-4 types of lignite-related model compounds were selected as representatives of linkages in lignites. The reaction products predicted by ReaxFF MDSs are consistent with those from experimental results reported. The initiation reaction observed in ReaxFF MDSs involving the ether linkage cleavage and methanol participation closely matches the results observed from previously reported experiments. The agreement of these results with available experimental observations demonstrates that ReaxFF MDSs can give an atomistic description of the initiation mechanism for methanolysis and provide useful insights into the complicated reaction processes.

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