Latest ArticlesWe report the unprecedent Pd(I) catalyzed ring-opening arylation of cyclopropyl-α-aminoamides. This protocol allows facile access to biologically important α-ketoamide-containing oligopeptides and even more challenging peptide-natural product conjugates. Site selectivity was achieved by introduction of special unnatural amino acids, which also meets the requisite of bioorthogonal chemistry. Mechanism investigations reveals a distinct domino radical ring-opening process through Pd(I) catalysis.
The hydrosilylation of unsaturated carbon-carbon bonds is one of the most critical reactions in silicone industrial production. The homogeneous Speier's catalyst, Karstedt's catalyst, and other noble metal-based catalysts are widely used. However, simplifying the separation of the homogeneous catalyst from reaction products and reducing the high cost of precious metals is still challenging. This review describes the recent development of heterogeneous catalysts for alkene, alkyne, and allene hydrosilylations, which can effectively solve problems in homogeneous hydrosilylation.
A photoinduced copper-catalyzed alkoxyl triggered C−C bond cleavage/aminocarbonylation cascade is presented. Through adjusting the structure of alkoxyl radical precursors, functionalized lactones and keto-amides were synthesized with good yields and excellent functional group tolerance under redox-neutral conditions. Notably, this protocol enables the integration of lactone fragments with many amine drugs and drug fragments.
Closed pores formed in hard carbons play an essential role in sodium storage at plateau region. However, the effect of different structural features on the diffusion of sodium ions into closed pores remains unclear. Herein, a precursor reconstruction strategy is conducted to regulate carbon microstructures including interlayer spacing, defect concentration, and closed pore volume by changing the ratio of aromatic and polysaccharide components. Aromatic structure parts tend to develop disordered carbons with fewer defects, larger interlayer spacing, and smaller closed pore volume, while polysaccharide components prefer to form disordered carbons with more defects, smaller interlayer spacing, and larger closed pore volume. Through the correlation analysis of microstructure features and the sodium storage capacity below 0.1 V. It finds that the intercalation capacity is proportional to the ratio of pseudo-graphitic domains, whereas the pore filling capacity appeared at lower potential gradually decreases with the increasing defect concentration due to homo-ionic repulsion effect, without linear correlation with short-range microcrystalline and closed pore volume. The optimized sample with suitable interlayer spacing and defect concentration exhibits a high plateau capacity of 241.7 mAh/g. This work provides insights into the exploitation of closed pore sodium storage performance.
Traditional photo-electcatalyst structures of small noble metal nanoparticles assembling into large-scale photoactive semiconductors still suffer from agglomeration of noble metal nanoparticles, insufficient charge transfer, undesirable photoresponse ability that restricted the photo-electrocatalytic performance. To this end, a novel design strategy is proposed in this work, namely integrating small-scale photoactive materials (doped graphene quantum dots, S,N-GQDs) with large-sized noble metal (PdP) nanoflowers to form novel photo-electrocatalysts for high-efficient alcohol oxidation reaction. As expected, superior electrocatalytic performance of PdP/S,N-GQDs for ethylene glycol oxidation is acquired, thanks to the nanoflower structure with larger specific surface area and abundant active sites. Furthermore, nonmetal P are demonstrated, especially optimizing the adsorption strength, enhancing the interfacial contact, reducing metal agglomeration, ensuring uniform and efficient doping of S,N-GQDs, and ultimately significantly boost the catalytic activity of photo-electrocatalysts.
The over-exploitation of fossil fuel energy has brought about serious environmental problems. It would be of great significance to construct efficient energy conversion and storage system to maximize utilize renewable energy, which contributes to reducing environmental hazards. For the past few years, in terms of electrocatalysis and energy storage, carbon fiber materials show great advantages due to its outstanding electrical conductivity, good flexibility and mechanical property. As a simple and low-cost technique, electrospinning can be employed to prepare various nanofibers. It is noted that the functional fiber materials with different special structure and composition can be obtained for energy conversion and storage by combining electrospinning with other post-processing. In this paper, the structural design, controllable synthesis and multifunctional applications of electrospinning-derived functional carbon-based materials (EFCMs) is reviewed. Firstly, we briefly introduce the history, basic principle and typical equipment of electrospinning. Then we discuss the strategies for preparing EFCMs with different structures and composition in detail. In addition, we show recently the application of advanced EFCMs in energy conversion and storage, such as nitrogen species reduction reaction, CO2 reduction reaction, oxygen reduction reaction, water-splitting, supercapacitors and ion batteries. In the end, we propose some perspectives on the future development direction of EFCMs.
A variety of research reports on novel supramolecular topologies have been published over the last years. However, it is still a great challenge to tap into the inner functional properties of these complexes. Herein, two tetranuclear metallamacrocycles 1 and 2 and four octonuclear [2]catenanes 3–6 were constructed successfully via a coordination-driven self-assembly strategy, by conscious design and use of the tetramethyl bidentate pyridine ligand L1, and the appropriate selection of six binuclear half-sandwich rhodium building units with different longitudinal dimensions. The complexes have been fully characterized by single crystal X-ray diffraction analysis and NMR spectroscopy. Furthermore, near-infrared photothermal studies of the obtained [2]catenanes reveal different photothermal response in solid and solution states, which may be attributed to a strong fluorescence quenching effect of the half-sandwich organometallic fragment and different conjugated effect of Cp*Rh based building blocks in the interlocking structures. The photothermal conversion efficiencies of [2]catenanes 4–6 fall in the range 30.5%–16.5% respectively. This contribution aims to play a key role in the experimental development of Cp*-based photothermal materials.
The microstructure of the active layer in organic photovoltaics (OPVs), such as the size of phase separation, purity of the phases, and molecular packing within each phase, plays a crucial role in influencing the behavior of excitons and charge carriers within the active layer. It is also a key determinant of the photovoltaic performance of the device. During the optimization of OPV devices, the use of additives has been demonstrated to be an effective strategy in microstructure control, leading to enhanced performance. Therefore, the quest for stable and efficient novel additives, along with an exploration and summarization of the mechanisms underlying additive-induced microstructure control, is essential for a better understanding of the developmental trends of high-performance additives. In this review, we categorize additives based on their chemical structures and discuss their effects on the microstructure of the active layer from both thermodynamic and kinetic perspectives. Furthermore, we elaborate on the working mechanisms and their impact on the photovoltaic performance of the devices. This review provides an overview of recent advances in additives for OPVs, offering potential guidance for the future development of additives and further optimization of the active layer in photovoltaic devices.
Inkjet printing has emerged as a potential solution processing method for large-area patterned films. During inkjet printing, a single droplet without satellite droplet is required for high-quality film. Herein, we propose a strategy for obtaining a single droplet by adjusting the reduced concentration (c/c*, where c* is the critical overlap concentration) in the range of 1.0–1.5. Droplet formation can be categorized into three distinct regimes: (1) c/c* < 1.0, satellite droplet; (2) c/c* = 1.0–1.5, single droplet; (3) c/c* > 2.0, no droplet. Furthermore, an inertial-capillary balance led to the 2/3-power scaling of the minimum radius with time for the solutions of c/c* < 1.0. However, for the solutions of c/c* = 1.0–1.5, the ligament radius decreased exponentially with time. Moreover, the Weissenberg number was higher than the critical value of 0.5, indicating that the polymer chains underwent coil-stretch transition. The viscoelastic-capillary balance dominated instead of the inertial-capillary balance. The resulting viscoelastic resistance reduced the length of the ligament and increased the velocity difference between the satellite and main droplets. Consequently, a single droplet was formed. In addition, the law can be successfully generalized to various molecular weights, molecular structures and solvents.
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