Carbon nitride with encapsulated nickel for semi-hydrogenation of acetylene: pyridinic nitrogen is responsible for hydrogen dissociative adsorption

A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride (CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorption and activation of hydrogen while nickel itself is physically isolated from the contact with reactive molecules. For the selective hydrogenation of acetylene in large amount of ethylene, the catalyst shows excellent ethylene selectivity than the nickel catalyst itself, which is almost totally unselective. Meanwhile, the CN itself is inactive for the reaction. The results of characterization demonstrate that pyridinic nitrogen doped in the carbon matrix should be the active sites for hydrogen dissociative adsorption. The theoretical calculations further confirm the results and provide with the detail in the electron transfer between nickel and CN in the catalyst. The current results supply a new concept for design of high performance catalyst.     

三维Zakharov-Kuznetsov方程解的衰减性

考虑三维Zakharov-Kuznetsov方程的初值问题,证明了该初值问题解的指数衰减性.这个性质与加权Sobolev空间中解的持久性及该问题解的唯一连续性相关.     

Malononitrile-involved Michael addition polymerization: An efficient and facile route for cyano-rich polyesters with programmable thermal and mechanical properties

An efficient, atom-economic, oxygen-tolerant, and water-tolerant strategy has been established to synthesize cyano-rich polyesters. Four kinds of organic bases, 1,1,3,3-tetramethylguanidine (TMG), 4-dimethylaminopyridine, triethylamine, and 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) were explored for accelerating Michael addition polymerization of malononitrile and 1,4-butandiol diacrylate. TMG can promote the polymerization efficiently under mild conditions to quantitatively afford polyester with high-molecular weight and moderate polydispersity. The comparison of the kinetic studies of TMG and TBD reveals that TMG shows better catalytic performance, while the catalysis of TBD brings about oligomers in spite of the higher efficiency at early age of the polymerization. Moreover, other diacrylate compounds could also be quantitatively polymerized to afford polyesters with high molecular weight. When dimethacrylate is chose as the monomer, the polymerization becomes sluggish. All the afforded polyesters display programmable thermal and mechanical properties that are closely related to their chemical structures.     

Random copolymerization of macromonomers as a versatile strategy to synthesize mixed-graft block copolymers

The random copolymerization of norbornene-functionalized macromonomers was explored as a method of synthesizing mixed-graft block copolymers (mGBCPs). The copolymerization kinetics of a model system of polystyrene (PS) and poly(lactic acid) (PLA) macromonomers was first analyzed, revealing a gradient composition of side chains along the mGBCP backbone. The phase separation behavior of mGBCPs with PS and PLA side chains of various backbone lengths and side chain molar ratios was investigated, and increasing the backbone length was found to stabilize the phase-separated nanostructures. The graft architecture was also demonstrated to improve the processability of the mGBCP, compared to a linear counterpart. Investigations of mGBCPs comprised of polydimethylsiloxane and poly(ethylene oxide) side chains exemplified the diverse self-assembled morphologies, including a Frank-Kasper A15 phase, that can be obtained with mGBCPs synthesized by random copolymerization of macromonomers. Lastly, a ternary mGBCP was synthesized by the copolymerization of three macromonomers.     

CRISPR-Cas12a System for Biosensing and Gene Regulation

Clustered regularly interspaced short palindromic repeats (CRISPR) is a promising technology in the biological world. As one of the CRISPR-associated (Cas) proteins, Cas12a is an RNA-guided nuclease in the type V CRISPR-Cas system, which has been a robust tool for gene editing. In addition, due to the discovery of target-binding-induced indiscriminate single-stranded DNase activity of Cas12a, CRISPR-Cas12a also exhibits great promise in biosensing. This minireview not only gives a brief introduction to the mechanism of CRISPR-Cas12a but also highlights the recent developments and applications in biosensing and gene regulation. Finally, future prospects of the CRISPR-Cas12a system are also discussed. We expect this minireview will inspire innovative work on the CRISPR-Cas12a system by making full use of its features and advantages.     

Computational Insights into the Allosteric Effect and Dynamic Structural Features of the SARS-COV-2 Spike Protein

COVID-19 caused by SARS-COV-2 is continuing to surge globally. The spike (S) protein is the key protein of SARS-COV-2 that recognizes and binds to the host target ACE2. In this study, molecular dynamics simulation was used to elucidate the allosteric effect of the S protein. Binding of ACE2 caused a centripetal movement of the receptor-binding domain of the S protein. The dihedral changes in Phe329 and Phe515 played a key role in this process. Two potential cleavage sites S1/S2 and S2′ were exposed on the surface after the binding of ACE2. The binding affinity of SARS-COV-2 S protein and ACE2 was higher than that of SARS-COV. This was mainly due to the mutation of Asp480 in SARS-COV to Ser494 in SARS-COV-2, which greatly weakened the electrostatic repulsion. The result provides a theoretical basis for the SARS-COV-2 infection and aids the development of biosensors and detection reagents.     

Introduction of phosphate groups into metal-organic frameworks to synthesize MIL-101(Cr)-PMIDA for selective adsorption of U(VI)

Journal of Radioanalytical and Nuclear Chemistry - Metal-organic frameworks (MOFs) MIL-101(Cr)-PMIDA with phosphate groups were prepared for the adsorption of U(VI). The morphology and structure of...