LEIYU

A novel method for intermolecular functionalization of terminal and internal alkenes has been designed. The electrophilic reagent, hypervalent iodine, plays a key role in this process by activating the alkene C=C bond for nucleophilic addition of the palladium catalyst. This process generates an iodonium-containing palladium species which undergoes CO insertion. The new approach, intermolecular oxycarbonylaton reactions of alkenes, has been achieved and carried out under mild reaction conditions to produce the corresponding β-oxycarbonylic acids with excellent efficiencies and levels of regio- and diastereoselectivity.

‘Kene activation: A novel method for intermolecular oxycarbonylation of terminal and internal alkenes has been designed. The electrophilic reagent, hypervalent iodine, plays a key role in this process by activating the alkene bond for nucleophilic addition of the palladium catalyst.

An atomic-scale engineered octopod nanoframe architecture (OFA) consisting of 3D catalytic surfaces and beneficial high-index facets is developed via a facile one-pot synthesis method. Based on the reliable recipe and general method, various complex nanoframe architectures are developed. Specially, the PtCu OFAs exhibit exceptional activity and stability for the oxygen reduction reaction and can be easily scaled up to high-quality.

Through a facile and effective strategy by employing lithium molten salts the controlled synthesis of 2H- and 1T-MoS₂ monolayers with high-yield production is achieved. Both phases of MoS₂ monolayers exhibit high stabilities. When used as a catalyst for hydrogen evolution, these phased MoS₂ monolayers deliver respective advantages in the field of electro- and photo-catalytic hydrogen evolution.

The necessity for new sources for greener and cleaner energy production to replace the existing ones has been increasingly growing in recent years. Of those new sources, the hydrogen evolution reaction has a large potential. In this work, for the first time, MoSe₂/Mo core–shell 3D-hierarchical nanostructures are created, which are derived from the Mo 3D-hierarchical nanostructures through a low-temperature plasma-assisted selenization process with controlled shapes grown by a glancing angle deposition system.

Metal–organic frameworks (MOFs) are promising high surface area coordination polymers with tunable pore structures and functionality; however, a lack of good size and morphological control over the as-prepared MOFs has persisted as an issue in their application. Herein, we show how a robust protein template, tobacco mosaic virus (TMV), can be used to regulate the size and shape of as-fabricated MOF materials. We were able to obtain discrete rod-shaped TMV@MOF core–shell hybrids with good uniformity, and their diameters could be tuned by adjusting the synthetic conditions, which can also significantly impact the stability of the core–shell composite. More interestingly, the virus particle underneath the MOF shell can be chemically modified using a standard bioconjugation reaction, showing mass transportation within the MOF shell.

It's a wrap: Sleeve netting provides a cost-effective solution to keep fresh fruits safe and sound. A metal–organic framework (MOF) is used to construct a molecular protective netting on the surface of the rod-like tobacco mosaic virus. The shell thickness was discovered to play a crucial role in the stability of the core–shell composite. More interestingly, the embedded virus particle can be chemically modified using a standard bioconjugation reaction, showing mass transportation within the MOF shell.

To combine flexibility and modifiability towards a more controllable complexity of MOFs, a post-synthetic variable-spacer installation (PVSI) strategy is used to implement kinetic installation/ uninstallation of secondary ligands into/from a robust yet flexible proto-Zr-MOF. This PVSI process features precise positioning of spacers with different length, size, number, and functionality, enabling accurate fixation of successive breathing stages and fine-tuning of pore surface. It shows unprecedented synthetic tailorability to create complicated MOFs in a predictable way for property modification, for example, CO₂ and R22 adsorption/separation, thermal/chemical stability, and extended breathing behavior.

Bringing PSM into dynamic MOFs: Post-synthetic modification (PSM) is used to install/uninstall varied linkers into/from a flexible Zr-MOF. This post-synthetic variable-spacer installation (PVSI) strategy is used to tune elastic deformation, breathing behavior, and stabilization of the framework in controllable and predictable way. Tuning the pore surface leads to a larger surface area and improved gas separation and adsorption capacity.

The catalytic enantioselective synthesis of boronate-substituted tertiary alcohols through additions of diborylmethane and substituted 1,1-diborylalkanes to α-ketoesters is reported. The reactions are catalyzed by readily available chiral phosphine/copper(I) complexes and produce β-hydroxyboronates containing up to two contiguous stereogenic centers in up to 99:1 e.r. and greater than 20:1 d.r. The utility of the organoboron products is demonstrated through several chemoselective functionalizations. Evidence indicates the reactions occur via an enantioenriched α-boryl-copper-alkyl intermediate.

Catalytic enantioselective synthesis of boronate-substituted tertiary alcohols is possible through the title reaction. The reactions are catalyzed by chiral phosphine/copper(I) complexes and produce β-hydroxyboronates containing up to two contiguous stereogenic centers. The utility of the organoboron products is demonstrated through several chemoselective functionalizations. pin=pinacolato, TMS=trimethylsilyl.