Latest ArticlesIn recent years, host-guest interactions of macrocycles have emerged as a promising approach to effectively enhance pure organic room-temperature phosphorescence by inhibiting the nonradiative relaxation while isolating the effects of oxygen and water molecules. In this work, a supramolecular assembly Q[8]-BCPI was constructed by 6-bromoisoquinoline derivative (BCPI) and cucurbit[8]uril (Q[8]). The assembly produced intense green room temperature phosphorescence (RTP) emission and enabled supramolecular recognition and detection of l-tryptophan (L-Trp) and l-tyrosine (L-Tyr). Moreover, the Q[8]-BCPI assembly showed good biocompatibility and low biotoxicity, and had a good staining effect on HeLa cells.
Dendrite growth of zinc (Zn) anode at high current density severely affects the fast-charging performance of aqueous zinc metal batteries (AZMBs). While interfacial modification strategies can optimize Zn performance, challenges such as complicated preparation processes, excessive layer thicknesses, and high voltage hysteresis should be addressed. Herein, we utilize a cost-effective liquid fluorosiloxane, (3,3,3-trifluoropropyl)trimethoxysilane, for scalable modification of Zn foil via drop-casting at room temperature, resulting in an ultra-thin interphase layer of only 20 nm. The Si-O-Zn bonds formed between fluorosiloxane and Zn ensure interfacial stability, and the Si-O-Si bonds between fluorosiloxane molecules help to homogenize the electric field distribution. Additionally, the abundant highly electronegative fluorine atoms on the anode surface act as zincophilic sites, promoting the uniform deposition of Zn2+. Thus, the modified Zn foil (SiFO-Zn) exhibits excellent dendrite suppression, reduced voltage hysteresis, and prolonged cycle life at ultra-high current density (40 mA/cm2), achieving a cumulative areal capacity of 12.9 Ah/cm2. Further, the full cell assembled with 10 µm-thick SiFO-Zn anode and MnO2 cathode achieves 2600 cycles at 5 A/g with minimal capacity degradation, and a large-size (22.5 cm−2) pouch cell powers the light-emitting diode even after reverse bending, demonstrating the potential of AZMBs for fast-charging flexible devices.
Artificial synapses are essential building blocks for neuromorphic electronics. Here, solid polymer electrolyte-gated artificial synapses (EGASs) were fabricated using ITO fibers as channels, which possess an ultra-high sensitivity of 5 mV and a long-term memory time exceeding 3 min. Notably, digitally printed ITO-fiber arrays exhibit an ultra-high transmittance of approximately 99.67%. Biological synaptic plasticity, such as excitatory postsynaptic current, paired-pulse facilitation, spike frequency-dependent plasticity, and synaptic potentiation and depression, were successfully mimicked using the EGASs. Based on the synaptic properties of the EGASs, an artificial neural network was constructed to perform supervised learning using the Fashion-MNIST dataset, achieving high pattern recognition rate (82.39%) due to the linear and symmetric synaptic plasticity. This work provides insights into high-sensitivity artificial synapses for future neuromorphic computing.
Carbon-based materials with single-atom (SA) transition metals coordinated with nitrogen (M-Nx) have attracted extensive attention due to their superior electrochemical CO2 reduction reaction (CO2RR) performance. However, the uncontrolled recombination of metal atoms during the typical high-temperature synthesis process in M-Nx causes deterioration of CO2RR activity. Herein, by using electrospinning, we propose a novel strategy for constructing a highly active and selective SA Fe-modified N-doped porous carbon fiber membrane catalyst (Fe-N-CF). This carbon membrane has an interconnected three-dimensional structure and a hierarchical porous structure, which can not only confine Fe to be single atom as active centers, but also provide a diffusion channel for CO2 molecules. Relying on its special structure and stable mechanical properties, Fe-N-CF is directly used for CO2RR, which presents an excellent selectivity (CO Faradaic efficiency of 97%) and stability. DFT calculations reveals that the synthesized Fe-N4-C can significantly reduce the energy barrier for intermediate COOH* formation and CO desorption. This work highlights the specific advantages of using electrospinning method to prepare the optimal SA catalysts.
Surface chemistry focuses on the investigation of the adsorption, migration, assembly, activation, reaction, and desorption of atoms and molecules at surfaces. Surface chemistry plays the pivotal roles in both fundamental science and applied technology. This review will summarize the recent progresses on surface assembly, synthesis and catalysis investigated mainly by scanning tunneling microscopy and atomic force microscopy. Surface assemblies of water and small biomolecules, construction of Sierpiński triangles and surface chirality are summarized. On-surface synthesis of conjugated carbo- and heterocycles and other kinds of carbon nanostructures are surveyed. Surface model catalysis, including single-atom catalysis and electrochemical catalysis, are discussed at the single-atom level.
The rational design of high-performance bifunctional electrocatalysts for overall water splitting (OWS) is the key to popularize hydrogen production technology. The active metal oxyhydroxide (MOOH) formed after surface self-reconfiguration of transition metal sulfide (TMS) electrocatalyst is often regarded as the "actual catalyst" in oxygen evolution reaction (OER). Herein, an Fe doped CoS2/MoS2 hollow TMS polyhedron (Fe-CoS2/MoS2) with rich Mott-Schottky heterojunction is reported and directly utilized as an OWS electrocatalyst. The spontaneous built-in electric field (BEF) at the heterogeneous interface regulates the electronic structure and D-band center of the catalyst. More importantly, the “TMS-MOOH” core-shell structure obtained in the KOH electrolyte shows enhanced OER properties. And the introduction of Fe ions activates the inert basal plane of MoS2, which greatly steps up the performance of HER. Hence, the preferable Fe-CoS2/MoS2–400 presents superior OER activity (η10 = 178 mV, η100 = 375 mV), HER activity (η10 = 92 mV) and ultra-high stability for 50 h. This work has deeply explored the catalytic mechanism of TMS and provided a new idea for the construction of efficient bifunctional catalysts.
Two o-carborane based tetraphenylethene (TPE) cationic cyclophanes O1·4PF6 and O2·4PF6 were synthesized through an SN2 reaction. Their structures were confirmed both possessing Z-shaped cavities in single crystal analysis. The optical properties of these macrocycles were systematically investigated using UV–vis spectroscopy and fluorescence techniques. It is worth noting that the introduction of a methoxy group to the TPE unit enables the synthesis of a near-infrared-emitting macrocycle O2·4PF6. The recognition behaviors of these two macrocycles towards nucleotides were investigated using various techniques including fluorescence titration, UV–vis titration, and transmission electron microscopy (TEM). Interestingly, these cyclophanes exhibited aggregation-induced emission (AIE) effects in water or under the induction of nucleotides.
The carboxylation of readily available organo halides with CO2 represents a practical strategy to afford valuable carboxylic acids. However, efficient carboxylation of inexpensive unactivated alkyl chlorides is still underdeveloped. Herein, we report the electro-reductive carboxylation of CCl bonds in unactivated chlorides and polyvinyl chloride with CO2. A variety of alkyl carboxylic acids are obtained in moderate to good yields under mild conditions with high chemoselectivity. Importantly, the utility of this electro-reductive carboxylation is demonstrated with great potential in polyvinyl chloride (PVC) upgrading, which could convert discarded PVC from hydrophobic to hydrophilic functional products. Mechanistic experiments support the successive single electron reduction of unactivated chlorides to generate alkyl anion species and following nucleophilic attack on CO2 to give desired products.
Photocatalytic hydrogen peroxide (H2O2) synthesis, driven by solar energy, offers a sustainable and cleaner alternative for producing green H2O2 from water and oxygen. 2D photocatalysts have emerged as powerful materials for this purpose due to their unique physiochemical properties such as a flexible planar structure and large surface area. This review provides a comprehensive overview of the latest advances in 2D photocatalytic materials employed in H2O2 synthesis, including metal oxides, metal chalcogenides, bismuth-based materials, graphitic carbon nitrides (g-C3N4), metal−organic frameworks (MOFs), and covalent organic frameworks (COFs). Beginning with an extensive introduction to possible reaction routes for photocatalytic H2O2 synthesis, we summarize the common methods for H2O2 detection, crucial for obtaining reliable results in H2O2 studies. Additionally, we highlight molecular-level modification strategies for 2D photocatalysts, such as surface modification, ion doping, defect engineering, and heterojunction construction, which promote high-efficiency solar-to-chemical conversion for sustainable H2O2 photosynthesis. Furthermore, we discuss key issues and provide perspective outlooks for the efficient and sustainable generation of H2O2 in scale-up industrial production. This review offers in-depth insights into different reaction pathways of H2O2 synthesis and provides design principles for 2D photocatalysts to enhance H2O2 production, guiding the development of efficient photocatalysts for H2O2 synthesis.
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