Synergistic Effect of Boron Nitride and Carbon Domains in Boron Carbide Nitride Nanotube Supported Single-Atom Catalysts for Efficient Nitrogen Fixation

Developing the low-cost and efficient single-atom catalysts (SACs) for nitrogen reduction reaction (NRR) is of great importance while remains as a great challenge. The catalytic activity, selectivity and durability are all fundamentally related to the elaborate coordination environment of SACs. Using first-principles calculations, we investigated the SACs with single transition metal (TM) atom supported on defective boron carbide nitride nanotubes (BCNTs) as NRR electrocatalysts. Our results suggest that boron-vacancy defects on BCNTs can strongly immobilize TM atoms with large enough binding energy and high thermal/structural stability. Importantly, the synergistic effect of boron nitride (BN) and carbon domains comes up with the modifications of the charge polarization of single-TM-atom active site and the electronic properties of material, which has been proven to be the essential key to promote N₂ adsorption, activation, and reduction. Specifically, six SACs (namely V, Mn, Fe, Mo, Ru, and W atoms embedded into defective BCNTs) can be used as promising candidates for NRR electrocatalysts as their NRR activity is higher than the state-of-the art Ru(0001) catalyst. In particular, single Mo atom supported on defective BCNTs with large tube diameter possesses the highest NRR activity while suppressing the competitive hydrogen evolution reaction, with a low limiting potential of −0.62 V via associative distal path. This work suggests new opportunities for driving NH₃ production by carbon-based single-atom electrocatalysts under ambient conditions.     

不同尺寸的NdFeB稀土永磁体热退磁行为研究

针对不同类型及不同尺寸的两类NdFeB永磁体分别研究了它们随温度变化的热退磁行为。采用样品的整体剩余磁通来表征热退磁过程中磁体性能的变化。结果表明,Pc较小的永磁体温度稳定性较差,随温度的升高,样品的剩余磁通迅速衰减;Pc<<0.1的普通型永磁体,温度为100℃时样品的剩余磁通损失超过60%。高矫顽力型永磁体比普通型磁体具有更优越的温度稳定性和高温性能。温度升高主要导致磁体矫顽力降低,140℃时普通型磁体的矫顽力降低约80%,而高矫顽力型磁体的矫顽力只降低了约20%。     

Asymmetric Synthesis VIII: Enantioselective Synthesis of (R) or (S)-α-Substituted Benzylamines VIA Chiral Pinanone Ketimine Template

An excellent asymmetric synthesis of both (R) and (S)-α-substituted benzylamines in optical purity 90.4–99.9% has been achieved by alkylation of a chiral ketimine, prepared from pinanone and benzylamine. Diastereoselectivity in the alkylation is not dependent on the alkyl halides.     

One-pot synthesis of N-aryl propargylamine from aromatic boronic acid,aqueous ammonia,and propargyl bromide under microwave-assisted conditions

A facile,one-pot synthesis of N-aryl propargylamine from aromatic boronic acid,aqueous ammonia,and propargyl bromide has been achieved under microwave-assisted conditions.The reactions can be smoothly completed within a total 10 min through a two-step procedure,including copper-catalyzed coupling of aromatic boronic acids with aqueous ammonia and following propargylation by propargyl bromide.     

Li-ion-conductive Li2TiO3-coated Li[Li0.2Mn0.51Ni0.19Co0.1]O2 for high-performance cathode material in lithium-ion battery

Journal of Solid State Electrochemistry - Li2TiO3 is used as a novel coating material to modify Li(Li0.2Mn0.51Ni0.19Co0.1)O2 electrode to enhance the electrochemical performance of the host...     

Synthesis of Piperidine Nucleosides as Conformationally Restricted Immucillin Mimics

The de novo synthesis of piperidine nucleosides from our homologating agent 5,6-dihydro-1,4-dithiin is herein reported. The structure and conformation of nucleosides were conceived to faithfully resemble the well-known nucleoside drugs Immucillins H and A in their bioactive conformation. NMR analysis of the synthesized compounds confirmed that they adopt an iminosugar conformation bearing the nucleobases and the hydroxyl groups in the appropriate orientation.     

Late-Stage Direct o-Alkenylation of Phenols by PdII-Catalyzed C−H Functionalization

o-Alkenylation of unprotected phenols has been developed by direct C−H functionalization catalyzed by Pd^II. This work features phenol group as a directing group and realizes highly site-selective C−H bond functionalization of phenols to achieve the corresponding products in moderate to excellent yields at 60 °C. The advantages of this reaction include unprecedented C−H functionalization using phenol as a directing group, high regioselectivity, good substrate scope, mild reaction conditions, and high efficiency. To the best of our knowledge, this is the first example of a regioselective C−H alkenylation of unprotected phenols utilizing phenolic hydroxyl group as a directing group. The alkenylation of unprotected tyrosine and intramolecular cyclization are also successfully carried out under this catalytic system in good yields. Furthermore, this novel method enables a late-stage modification of complex phenol-containing bioactive molecules toward a diversity-oriented drug discovery.