Precise Tuning of Functional Group Spatial Distribution on Porphyrin Rings for Enhanced CO Electroreduction Selectivity.

Molecular catalysts play a critical role in regulating the selectivity of electrocatalytic CO reduction reaction (CORR), yet the understanding of ligand function is largely restricted to modulating the electronic structure of the metal and reaction kinetics. Herein, a hydroxyl (─OH) ligand is introduced into a sterically hindered amino-porphyrin (o-TAPP) to synthesize the atropisomers porphyrin-salicylimine-Cu (o-Cu-Por-Sa) with hydrogen-bonding interactions (O─H⋯O), enabling efficient selection of CO and CH under dual effects. Detailed analysis shows that the ─OH of o-Cu-Por-Sa (αβαβ) forms a noncovalent hydrogen bond with carbonate, characterized by a bond length of 2.

Electrolyte Chemistry Modulation Toward High-Performance and Ultralow-Temperature Silicon Anode.

The high-capacity silicon (Si) anode usually suffers from rapid capacity decay and low Coulombic efficiency in carbonate electrolytes resulting from large volume expansion and unstable solid electrolyte interphase (SEI). In addition, the sluggish electrode kinetics in routine electrolytes at subzero temperatures severely hampers the operational capabilities of Si-based batteries. Herein, a rational electrolyte design strategy is reported to tune the solvation chemistry and interfacial behavior of the electrolyte for high-performance Si anode.

Hydrogenation Reaction Mechanisms on Ni-Doped MoS Catalysts: A Density Functional Theory Study of Sulfur Edge Engineering and Coregulated Electronic Effects.

Precise modulation of local interatomic interactions affecting the electronic structure is an important method to control the catalytic activity and reaction pathways. In this study, we focused on the hydrogenation reaction of naphthalene and employed density functional theory calculations to investigate the specific influence of electronic effects triggered by the coregulation of Ni and sulfur edge engineering on the hydrogenation performance of Ni-doped MoS at different edge sulfur coverages (Ni-MoS-X-θ). Our findings reveal that the interaction between Ni and S in the catalyst matrix material modifies the local electronic structure surrounding the sulfur atoms in the active site.

"Live" Nanomaterials Process Biomimetic Recognition and Assembly In Vivo.

The biomimetic strategy has been widely used in multiple fields, and provides huge convenience to human life. For biomedical application in vivo, the importance of biomimetic materials lies on mimicking the natural process/behavior as well as mimicking the structure/ingredient. Herein, recent advances of materials processing biomimetic recognition and assembly behavior for in vivo applications, including the natural source materials and artificial materials, are summarized.

Carbon-Based Composite Phase Change Materials for Thermal Energy Storage, Transfer, and Conversion.

Phase change materials (PCMs) can alleviate concerns over energy to some extent by reversibly storing a tremendous amount of renewable and sustainable thermal energy. However, the low thermal conductivity, low electrical conductivity, and weak photoabsorption of pure PCMs hinder their wider applicability and development. To overcome these deficiencies and improve the utilization efficiency of thermal energy, versatile carbon materials have been increasingly considered as supporting materials to construct shape-stabilized composite PCMs.

Toward the Application of High Frequency Electromagnetic Wave Absorption by Carbon Nanostructures.

With the booming development of electronic information technology, the problems caused by electromagnetic (EMs) waves have gradually become serious, and EM wave absorption materials are playing an essential role in daily life. Carbon nanostructures stand out for their unique structures and properties compared with the other absorption materials. Graphene, carbon nanotubes, and other special carbon nanostructures have become especially significant as EM wave absorption materials in the high-frequency range.

All-Inorganic Perovskite Quantum Dot-Monolayer MoS Mixed-Dimensional van der Waals Heterostructure for Ultrasensitive Photodetector.

2D transition metal dichalcogenide (2D-TMD) materials and their van der Waals heterostructures (vdWHs) have inspired worldwide efforts in the fields of electronics and optoelectronics. However, photodetectors based on 2D/2D vdWHs suffer from performance limitations due to the weak optical absorption of their atomically thin nature. In this work, taking advantage of an excellent light absorption coefficient, low-temperature solution-processability, and long charge carrier diffusion length, all-inorganic halides perovskite CsPbI Br quantum dots are integrated with monolayer MoS for high-performance and low-cost photodetectors.

Stimuli-Directed Dynamic Reconfiguration in Self-Organized Helical Superstructures Enabled by Chemical Kinetics of Chiral Molecular Motors.

Dynamic controllability of self-organized helical superstructures in spatial dimensions is a key step to promote bottom-up artificial nanoarchitectures and functional devices for diverse applications in a variety of areas. Here, a light-driven chiral overcrowded alkene molecular motor with rod-like substituent is designed and synthesized, and its thermal isomerization reaction exhibits an increasing structural entropy effect on chemical kinetic analysis in anisotropic achiral liquid crystal host than that in isotropic organic liquid. Interestingly, the stimuli-directed angular orientation motion of helical axes in the self-organized helical superstructures doped with the chiral motors enables the dynamic reconfiguration between the planar (thermostationary) and focal conic (photostationary) states.

Multifunctional Hydrogels with Reversible 3D Ordered Macroporous Structures.

prepared by colloidal crystals templating display highly reversible shape memory properties, as confirmed by indirect electron microscopy imaging of their inverse replicas and direct nanoscale resolution X-ray microscopy imaging of the hydrated hydrogels. Modifications of functional groups in the 3DOM hydrogels result in various materials with programmed properties for a wide range of applications.

Brønsted Acid/Lewis Acid Cooperatively Catalyzed Addition of Diazoester to 2-chromene Acetals.

A novel Brønsted acid/Lewis acid dual catalyst system has been developed to promote an efficient C-C bond formation between a range of oxocarbenium precursors derived from chromene acetals and ethyl diazoacetate. The reaction proceeds under mild conditions and is tolerant of common functionalized 2-chromene and isochromene acetals. In addition, an asymmetric variant of diazoacetate addition towards 2-chromene acetal is described.