Latest ArticlesThe bicarbonate-formate (HCO3− – HCO2−) interconversion provides a promising cycle for a conveniently accessible hydrogen storage system via reversible dehydrogenation and hydrogenation processes. Existing catalytic systems often use organic solvents, tedious optimization as well as manipulation of pH values, solvent, pressure and various additives. Herein, we present an operational, robust, safe and cost-effective catalytic system for hydrogen storage and liberation. We have established a unique catalytic system with two different solid organometallic assemblies (NHC-Ru and NHC-Ir) that facilitate the reversible transformation between sodium formate and bicarbonate in aqueous solutions collaboratively and efficiently. Notably, the NHC-Ru catalyst is privileged for the hydrogenation of sodium bicarbonate, whereas the NHC-Ir component enables the dehydrogenation of sodium formate, all in a single reaction vessel. What sets this system apart is its simplicity. The H2 discharging and recharging is simply regulated by heating the mixture with or without H2. Remarkably, this process requires no extra additives or supplementary treatments. Moreover, the reversible hydrogen storage system is durable and can be reused for over 30 cycles without a discernible decline in activity and selectivity. The strategic paradigm in this study shows significant practical potential in hydrogen fuel cell applications.
Utilizing superwettability micro/nanostructures to enhance the condensation heat transfer (CHT) performance of engineering materials has attracted great interest due to its values in basic research and technological innovations. Currently, exploring facile micro/nanofabrication approaches to create high-efficiency CHT surfaces has been one of research hotspots. In this work, we propose and demonstrate a type of new superwettability hybrid surface for high-efficiency CHT, which consists of superhydrophobic nanoneedle arrays and triangularly-patterned superhydrophilic microdots (SMDs). Such hybrid surface can be fabricated by the facile growth of densely-packed ZnO nanoneedles on the Zn-electroplated copper surface followed by fluorosilane modification and mask-assisted photodegradation. Through regulating the diameters and interspaces of SMDs, we obtain the optimized triangularly-patterned hybrid surface, which shows 42.7% higher CHT coefficient than the squarely-patterned hybrid surface and 58.5% higher CHT coefficient than the superhydrophobic surface. The key of such hybrid surface design is to considerably increase CHT coefficient brought about by SMD-triggered drop sweeping at the cost of slightly reducing heat transfer area of superhydrophobic functional zone for drop jumping. Such new strategy helps develop advanced CHT surfaces for high-efficiency electronic cooling and energy utilization.
Achieving seamless tiling through the self-assembly of organic species has long fascinated scientists for its potential applications across various fields. However, constructing periodic nanostructures with high-order tessellation remains challenging, particularly in achieving precise control at the supramolecular level. In this study, we present the successful creation of multiple seamless 2D tessellations on Au (111) surface using versatile hexagonal tiles derived from a singular molecular unit, namely 2,6,10-tribromotricycloquinazoline. Through scanning tunneling microscopy imaging, seven distinct 2D tessellations, ranging from regular to semiregular to k-uniform tilings, are unveiled at the molecular level. Density functional theory calculations provide a theoretical basis for the formation of these complex 2D tessellation, highlighting the important role of the variability of Br···Br/H contacts in facilitating complex seamless 2D tessellations on surface. This work opens avenues for exploring possibilities in constructing intricate tiling patterns with diverse applications.
Gliomas are the most common intracranial tumors with poor survival and high mortality. Furthermore, the clinical efficacy of current drugs is still not ideal; despite the development of several therapeutic drugs over the past decades and tumor progression or recurrence is inevitable in many patients. RNAi-based therapy presents a novel disease-related gene targeting therapy, including otherwise undruggable genes, and generates therapeutic options. However, the therapeutic effect of siRNA is hindered by multiple biological barriers, primarily the blood-brain barrier (BBB). A glycoprotein-derived peptide-mediated delivery system is the preferred option to resolve this phenomenon. RDP, a polypeptide composed of 15 amino acids derived from rabies virus glycoprotein (RVG), possesses an N-type acetylcholine receptor (nAChR)-binding efficiency similar to that of RVG29. Given its lower cost and small particle size when used as a ligand, RDP should be extensively evaluated. First, we verified the brain-targeting efficacyy of RDP at the cellular and animal levels and further explored the possibility of using the RDP-oligoarginine peptide (designated RDP-5R) as a bio-safe vehicle to deliver therapeutic siRNA into glioma cells in vitro and in vivo. The polypeptide carrier possesses a diblock design composed of oligoarginine for binding siRNA through electrostatic interactions and RDP for cascade BBB- and glioma cell-targeting. The results indicated that RDP-R5/siRNA nanoparticles exhibited stable and suitable physicochemical properties for in vivo application, desirable glioma-targeting effects, and therapeutic efficiency. As a novel and efficient polypeptide carrier, RDP-based polypeptides hold great promise as a noninvasive, safe, and efficient treatment for various brain diseases.
The tert-butyl nitrite as a bifunctional reagent mediated radical alkene difunctionalization has emerged as a powerful strategy for synthesis of structurally diverse oxime-containing compounds. However, the phosphorus-centered radical initiated transformations remain largely elusive. Herein, a visible-light-induced radical phosphinoyloximation of alkenes with secondary phosphine oxides and tert-butyl nitrite has been developed under photocatalyst- and metal-free conditions. This protocol features mild conditions, broad substrate scope, good functional tolerance, and operational simplicity, yielding a diverse array of α-phosphinoyl oximes in moderate to good yields with high stereoselectivities. The photomediated homolytic cleavage of ONO bond of tert-butyl nitrite generates the reactive tert-butoxyl radical and persistent NO radical to act as both HAT reagent and the source of oximes.
Pyrrole is a heterocycle with four carbon atoms and a nitrogen atom, which is extensively used in the pesticide and pharmaceutical industries. In addition, it has a series of analogs such as pyrrolidine, pyrroline, and pyrrolidone. Pesticides containing pyrrole and its analogs have been formally marketed as fungicides, including fenpiclonil, fludioxonil, the insecticide chlorfenapyr, and the herbicide fluorochloridone. In this paper, we analyze the structure-activity relationships (SARs) of pesticides containing these structures. We summarize the characteristics possessed by the most highly active pyrrole and its analogs and provide an overview of research on pyrrole compounds with insecticidal, antimicrobial, herbicidal, and antiviral properties in the past 20 years. It is hoped to provide ideas for the development and design of this type compounds in pesticides and to assist researchers in this area.
The realization of high-efficiency photocatalysis is greatly meaningful to overcome the issues of current energy and environment, in which the core factor is the exploration of photocatalysts with promising semiconductor properties. The Cu-based metal sulfide photocatalysts of CuSbS2 and its derivative of bournonite CuPbSbS3 possess the features of earth-abundant elements, strong photostability, visible-light range bandgap, and high absorption coefficient, possessing great potential for the realization of efficient photocatalytic applications. Although the photocatalysts of CuSbS2 and CuPbSbS3 have been investigated in photocatalysis application of hydrogen production and degradation, the exploration process is still in the early-development stage. In this review, the design concept and semiconductor properties of CuSbS2 and CuPbSbS3 are firstly introduced. Subsequently, the photocatalytic applications of CuSbS2 and CuPbSbS3 photocatalysts, mainly including hydrogen production and degradation, are systematically reviewed. Finally, the challenges and prospects for the further exploration of CuSbS2 and CuPbSbS3 photocatalysts are provided.
Surface-confined metal-organic frameworks have emerged as versatile structures with a broad spectrum of applications such as nanoelectronics, catalysis, sensing, and molecular storage, owing to their unique structural and electronic properties. However, the exploration and optimization of molecular networks typically involve resource-intensive trial-and-error experiments. The complexity comes from factors like metal nodes, organic ligands, substrates, and the preparation conditions. To address this challenge, high-throughput methodologies have been used in materials exploration. In this work, we explored a high-throughput method for preparing sub-monolayer metals with continuous coverage spread on metal surfaces. By employing a physical mask during metal deposition under ultra-high vacuum conditions, we achieved sample libraries with copper (Cu) and silver (Ag) adatoms on the metal substrates, and constructed surface-supported metal-organic frameworks with varying metal-to-molecule stoichiometric ratios. This approach facilitates the exploration of surface-confined metal-organic frameworks, particularly in terms of varying metal-to-ligand stoichiometric ratios, offering an efficient pathway to unlock the potential of these intricate two-dimensional networks.
The development of high-performance carbon-based composite hosts plays decisive roles in the electrochemistry of lithium sulfur batteries. Herein, a novel metal-ion induced gelation self-assembly technology is reported to construct sodium alginate carbon (SAC) based polar hierarchical carbon composites with cross-linked network architecture and in-situ co-grown cross-linked polar nanoparticles. Interestingly, it shows high versatility to an extensive array of materials including metals, alloys, and metallic oxides. As a representative, NiCo alloy nanoparticles are chosen to obtain the SAC/NiCo composite host for sulfur in LSBs, which possess superior physical/chemical adsorption capabilities and catalytic conversion kinetics to polysulfide in virtue of synergistic interaction between the hierarchical pore structures and NiCo catalyst. The designed SAC/NiCo-S cathode shows superior electrochemical performance with excellent rate capacity (2 C: 693.5 mAh/g) and enhanced cycling stability (764.3 mAh/g at 0.1 C after 240 cycles). This work provides a straightforward approach for fabricating multifunctional carbon composites with adjustable component for advanced energy storage system.
Charge-neutral method (CNM) is extensively used in investigating the performance of catalysts and the mechanism of N2 electrochemical reduction (NRR). However, disparities remain between the predicted potentials required for NRR by the CNM methods and those observed experimentally, as the CNM method neglects the charge effect from the electrode potential. To address this issue, we employed the constant electrode potential (CEP) method to screen atomic transition metal-N-graphene (M1/N-graphene) as NRR electrocatalysts and systematically investigated the underlying catalytic mechanism. Among eight types of M1/N-graphene (M1 = Mo, W, Fe, Re, Ni, Co, V, Cr), W1/N-graphene emerges as the most promising NRR electrocatalyst with a limiting potential as low as −0.13 V. Additionally, the W1/N-graphene system consistently maintains a positive charge during the reaction due to its Fermi level being higher than that of the electrode. These results better match with the actual circumstances compared to those calculated by conventional CNM method. Thus, our work not only develops a promising electrocatalyst for NRR but also deepens the understanding of the intrinsic electrocatalytic mechanism.
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