Latest ArticlesTwo-dimensional (2D) mesoporous pseudocapacitive polymer/graphene heterostructures combine the advanced merits of 2D materials and mesoporous materials, possessing unique nanosheet structure, large specific surface area (SSA), abundant oxygen/nitrogen-containing groups, desirable electrical conductivity and admirable electrochemical redox activity, and hold great potential for constructing high-performance planar micro-supercapacitors (MSCs). Herein, we demonstrate the interfacial assembly of 2D mesoporous polydopamine/graphene (mPDG) heterostructures with well-defined mesopore structure (12 nm) and adjustable thickness (7.5–14.1 nm) for planar high-energy pseudocapacitive MSCs. Attributed to medium thickness, exposed mesopore of 12 nm and large SSA of 108 m2/g, the mPDG with 10.8 nm thickness reveals prominent mass capacitance of 419 F/g and impressive cycling stability with ~96% capacitance retention after 5000 cycles. Furthermore, the symmetric mPDG-based MSCs with "water-in-salt" gel electrolyte present wide voltage window of 1.6 V, superior volumetric energy density of 11.5 mWh/cm3, outstanding flexibility and self-integration ability. Therefore, this work offers a new platform of controllably synthesizing 2D mesoporous heterostructures for high-performance MSCs.
With the increasing emergence of bacterial infections, especially multidrug-resistant (MDR) bacteria, poses an urgent threat. This study demonstrated a novel multifunctional nanotheranostics platform developed by the strategic integration of both in-situ bio-assembly imaging and target bacteria inactivation. Through the introduction of copper ions into bacteria, the Cu2+ could spontaneously bio-self-assembled into a multifunctional copper nanoclusters (NCs) which efficiently enhanced epigallocatechin gallate (EGCG) uptake into bacteria. While visualizing the bacteria, the developed theranostic nanoplatform exhibited highly efficient disinfection activities with negligible side effects as reflected by higher cell viability and insignificant hemolytic effects. Furthermore, the exosomal formulation of EGCG integrated with Cu2+ showed an increased intracellular antibacterial activity, which could eliminate most of the methicillin-resistant Staphylococcus aureus (MRSA) phagocytosed by macrophages, guide macrophages toward M2-like phenotype polarization and alleviate inflammation, without exhibiting obvious cytotoxicity on host RAW264.7. The regimen could be viewed as an effective strategy for the sterilization of intractable bacterial infections.
Diatomic-site catalysts (DASCs) have emerged as a kind of promising heterogeneous candidate catalysts for electrochemical CO2 reduction (ECR), which is considered to retain the advantage of single-atom catalysts (SACs) but also introduce opportunities to exceed the limit of single-atom catalysts. In the past few years, tremendous progress has been achieved in this field. Herein, the recent progress in ECR on DASCs has been summarized. It will start with the classification of DASCs. Then the challenges in the precise fabrication and characterization of DASCs have been emphasized. By introducing the advanced ECR performance on DASCs, superior to that on SACs, the synergistic effects of the dual metal atoms are highlighted, as this origin of the advanced ECR performance on DASCs is comprehensively summarized. Finally, the major challenges and perspectives of DASCs have been proposed to shed light on the development of DASCs for ECR application.
Rationally designed novel cost-effective hydrogen evolution reaction (HER) electrocatalysts with controlled surface composition and advanced structural superiority is extremely critical to optimize the HER performance. Polyoxometalates (POMs) with structural diversity and adjustable element compositions represent a promising precursor for rational design and preparation of HER electrocatalysts. Herein, a series of transition metal-doped MoS2 materials with different surface engineered structures (Fe, Cr, V doping and S vacancies) (M-MoS2/CC, M = Fe, Cr and V) were fabricated by a simple hydrothermal-vulcanization strategy using Keplerate polyoxomolybdate nanoball ({Mo72Fe30}, {Mo72Cr30}, {Mo72V30}, {Mo132}) as precursors. The enlarged interlayer spacing as well as the integration of homogeneous transition metal doping and abundant sulfur vacancies endows prepared M-MoS2/CC with superior HER electrocatalytic performance and excellent long-term working stability in both acidic and alkaline media. The optimized Fe-MoS2/CC afford current densities of 10 and 50 mA/cm2 at overpotentials of 188/272 mV and 194/394 mV in 0.5 mol/L H2SO4 and 1.0 mol/L KOH aqueous solution, respectively, outperforming most of reported typical transition metal sulfide-based catalysts. This work represents an important breakthrough for POMs-mediated highly efficient transition metal sulfide-based HER electrocatalysts with wide range pH activity and may provide new options for the rational design of promising HER electrocatalysts and beyond.
The severe interfacial charge recombination as well as the stability issues brought by the Li-TFSI still hinder the commercialization of high-performance perovskite solar cells (PSCs). Here, a polyoxometalates (POMs)-based complex, POM@ ionic liquid (IL), is synthesized and applied as an effective additive that simultaneously enhances the performance and stability of PSCs. The interactions between POM@IL complex and Li-TFSI inhibit the aggregation of Li-TFSI. The synergistic oxidation of POM@IL complex and Li-TFSI towards 2, 2′, 7, 7′-tetrakis[N, N-di(4-methoxyphenyl)amino]-9, 9'-spirobifluorene (Spiro-OMeTAD) effectively enhances the electrical properties of hole transport layer film and the photovoltaic performances of PSCs. The champion device modified with the POM@IL complex yields an excellent power conversion efficiency (PCE) of 22.73%. Moreover, the incorporation of POM@IL improves the humidity stability of PSCs. After storing under high humidity conditions (25 ℃, 60% RH) for 1200 h, the POM@IL modified device retained a remarkable 81.2% of its initial PCE. This work provides new insight into constructing POMs-based materials for high-performance photovoltaic devices.
Strand displacement reaction enables the construction of enzyme-free DNA reaction networks, thus has been widely applied to DNA circuit and nanotechnology. It has the characteristics of high efficiency, universality and regulatability. However, the existing regulation tools cannot enable effective control of the reaction sequence, which undoubtedly limits the construction of complex nucleic acid circuits. Herein, we developed a regulation tool, toehold lock, and achieved strict control of reaction sequence without loss of the main reaction signal output. Furthermore, we applied the tool to scenarios such as seesaw circuits, AND/OR logic gates, and entropy-driven circuits, and respectively demonstrated its significant superiority compared to the original method. We believe that the proposed toehold lock has greatly optimized the efficiency of DNA strand displacement-based networks, and we anticipate that the tool will be widely used in multiple fields.
Covalent bioactive compounds are successfully used in clinic and attracted intense research efforts in the fundamental study as well as drug development. The advantageous effects of covalent compounds compared with non-covalent ones are highly dependent on electrophilic warheads. Hence, electrophilic warheads with tunable reactivity and selectivity are highly demanded in fields of medicinal chemistry and chemical biology. Herein, we report a novel electrophilic warhead, chloromethyl group activated by thiol-substituted 1,2,4-triazole. Interestingly, a pair of regioisomers could be simultaneously occurred in the step of alkylation during the synthesis of this unique motif. This is a rare example that the alkylation could simultaneously generate these two separable regioisomers of 1,2,4-triazole at the nitrogen or sulfur atom. The covalent-working mechanism of this new warhead is confirmed by various chemoproteomics experiments including target identification and binding site mapping. Importantly, the reactivity and selectivity of this new electrophilic warhead could be efficiently tuned by virtue of stereo effect. Interestingly, one pair of regioisomers (19S and 19X) induced distinct modes of cell death. Isomer 19S could induce apoptosis of colon cancer cells while 19X could induce both apoptosis and ferroptosis. Together, this study provides pairs of novel electrophilic warheads that could be useful not only in supporting the design of covalent compounds for drug discovery but also in providing chemical probes for the fundamental biological study.
Na+ batteries (SIBs) have been emerging as the most promising candidate for the next generation of secondary batteries. However, the development of high-performance and cost-effective anode materials is urgently needed for the large-scale applications of SIBs. In this study, carbon dots confined bimetallic sulfide (NiCo2S4) architecture (NiCo2S4@CDs) was proposed and synthesized from assembling nanosheets into cross-stacked superstructure and the subsequent confinement of carbon dots. This novel decussated structure assembly from nanosheets is greatly beneficial to the structure stability of electrode material during the successive charge/discharge processes. Besides, the CDs based carbon conductive network can enhance the electrical conductivity for facilitating the easy transport of electron/Na+. Benefitting from these advantages, NiCo2S4@CDs exhibits high-rate performance and an ultralong cycling life in SIBs. Specifically, the specific capacity of NiCo2S4@CDs can reach the discharge specific capacity as high as 568.9 mAh/g at 0.5 A/g, which can also maintain 302.7 mAh/g after 750 cycles at 5.0 A/g. Additionally, ex-situ characterization techniques such as ex-situ XRD and ex-situ XPS were employed to further explore the sodium storage mechanism of the NiCo2S4@CDs anode.
Three-dimentional (3D) transition metal selenides with sufficient channels could produce significant superiority on enhancing reaction kinetics for sodium-ion batteries. However, the thorough exploration of 3D architecture with a facile strategy is still challenging. Here we report that a polycrystalline Cu2-xSe film was epitaxial grown on (220) facets-exposed Cu by direct selenization of a nanoporous Cu skeleton, which is obtained by dealloying rolled CuMn@Cu alloy foil. Density functional theory calculation result shows strong adsorption energy for Se atoms on Cu (220) planes during selenization reaction, rendering a low energy consumption. By virtue of this core-shell 3D nanoporous architecture to offer abundant active sites and endow fast electron/ion transportation, the nanoporous Cu2-xSe@Cu-0.15 composite electrode exhibits remarkable sodium-ion storage properties with high reversible capacity of 950.6 µAh/cm2 at 50 µA/cm2, suprior rate capability of 457.6 µAh/cm2 at 500 µA/cm2, as well as an ultra-long stability at a high current density. Mechanism investigation reveals that the electrochemical reaction is a typical conversion-type reaction with different intermediates. This novel electrode synthetic strategy provides useful instructions to design the high-performance anode material for sodium-ion batteries.
Due to their superior fluorescence, phosphorescence, and catalytic capabilities, carbon dots (CDs), an emerging class of fluorescent carbon nanomaterials, have a wide range of potential applications. The properties of CDs have recently been controlled extensively by heteroatom doping. Boron atoms have been effectively doped into the structure of CDs due to their similar size to carbon atoms and excellent electron-absorbing ability to further improve the performance of CDs. In this review, we summarize the research progress of boron-doped CDs in recent years from the aspects of doping strategies, effects of boron doping on different performances of CDs and applications. Starting from the two aspects of single boron doping and boron and other atom co-doping, from different precursor materials to different synthesis methods, the doping strategies of boron-doped CDs are reviewed in detail. Then, the effects of boron doping on the fluorescence, phosphorescence and catalytic performance of CDs and applications of boron-doped CDs in optical sensors, information encryption and anti-counterfeiting are discussed. Finally, we further provide a prospect towards the future development of boron-doped CDs.
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