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A practical electrochemical strategy for the direct synthesis of arenesulfonyl fluorides from industrial feedstock nitroarenes is described. The key to success lies in using a cheap ionic liquid N-methylimidazolium p-toluenesulfonate ([Mim]TolSO3) as an effective additive and electrolyte to facilitate the selective reduction of nitroarenes to the corresponding aniline intermediate, promoting the desired fluorosulfonylation with broad functional group tolerance under mild conditions. [ABSTRACT FROM AUTHOR]

Although antibacterial platforms involving nanozymes have been extensively investigated, there are still problems of poor reactive oxygen species generation efficiency and obstinate bacterial biofilms. Developing a nanozyme-photothermal therapy nanoplatform with superior sterilization effects and minimal side effects would be a good alternative for completely eliminating bacteria and biofilms. Herein, an ultrathin PdMo bimetallene nanozyme with a planar topology and boosted metal utilization, exhibiting excellent photothermal and peroxidase-like activity, is designed for synergistic nanozyme-photothermal sterilization applications and accelerated wound healing. The superior catalytic activity of PdMo bimetallene nanozymes could convert a biosafe concentration of hydrogen peroxide (H2O2) into large quantities of toxic hydroxyl radicals (•OH) under laser irradiation, enhancing bacterial membrane permeability and thermal sensitivity for efficient removal of bacteria and biofilms. In addition, PdMo bimetallene presents a good wound-healing ability according to the results of fibroblast proliferation and collagen deposition with minor side effects. This work would provide an innovative avenue for developing metallene-based nanozymes for biomedical applications. [ABSTRACT FROM AUTHOR]

Bone tumors are invasive diseases with a tendency toward recurrence, disability, and high mortality rates due to their grievous complications. As a commercial polymeric biomaterial, polymethylmethacrylate (PMMA) cement possesses remarkable mechanical properties, injectability, and plasticity and is, therefore, frequently applied in bone tissue engineering. Numerous positive effects in bone tumor treatment have been demonstrated, including biomechanical stabilization, analgesic effects, and tumor recurrence prevention. However, to our knowledge, a comprehensive evaluation of the application of the PMMA cement in bone tumor treatment has not yet been reported. This review comprehensively evaluates the efficiency and complications of the PMMA cement in bone tumor treatment, for the first time, and introduces advanced modification strategies, providing an objective and reliable reference for the application of the PMMA cement in treating bone tumors. We have also summarized the current research on modifications to enhance the anti-tumor efficacy of the PMMA cement, such as drug carriers and magnetic hyperthermia. [ABSTRACT FROM AUTHOR]

Catalytic pyrolysis of polyethylene (PE) can produce benzene, toluene, and xylene (BTX) as important building-block chemicals, and selectivity control is key to its economic and ecological efficiency. Here, we report a synergistic effect between Pt and ZSM-5 for selective production of BTX from catalytic pyrolysis of PE by providing mechanistic insights into reaction pathways of key intermediates and regulation of the rate-controlling step. A high yield (52%) of BTX was obtained at 450 °C under atmospheric pressure using a Pt/ZSM-5 catalyst, where Pt mainly exists in the metallic state with a cuboctahedral crystal structure. In contrast, thermal pyrolysis of PE produced linear alkenes/alkanes of wide carbon number distribution, and catalytic pyrolysis of PE over ZSM-5 led to a low BTX yield of 21% with C1–C4 alkenes/alkanes being the major products even at a higher temperature (500 °C). It was found that the introduction of Pt into ZSM-5 significantly decreased the aromatization onset temperature, suggesting a reduction of apparent activation energy for the aromatization of alkene intermediates during catalytic pyrolysis of PE. Density functional theory calculations reveal that the aromatization of intermediate ethylene proceeds via oligomerization, cyclization, and dehydrogenation, and the energy barrier of the rate-controlling step, i.e., dehydrogenation of on Pt/ZSM-5 is much lower than that on ZSM-5. As a result, Pt enhanced the aromatization rates of light alkenes formed by PE cracking over the acid sites in ZSM-5, the synergistic effects of which contributed to the high BTX yield on Pt/ZSM-5. [ABSTRACT FROM AUTHOR]

Herein, ultrasmall nanostructured Co3O4 particles have been prepared by a facile two-step synthetic method and furthermore applied to lithium-ion batteries. Benefitting from an increased specific surface area and improved tolerance for volume expansion, they deliver an extremely high specific capacity of 1432.7 mA h g−1 at 0.1 A g−1 and an outstandingly long cycle life with about 511.2 mA h g−1 at 10 A g−1 after 2000 cycles. This work will pave a new way to engineer advanced electrode materials for long-lived high-rate lithium-ion batteries. [ABSTRACT FROM AUTHOR]

The precise configuration of metal pair sites at the atomic level in dual-metal single-atom catalysts (DACs) is key but challenging. Herein, we correlate the heteronuclear metal pair-site with the intrinsic structure of donor atoms in DACs, during which intramolecular heteroatoms, e.g., methionine, are shown adept at narrowing the atomic spacing of metal atoms to produce pairwise active sites. Then, guided by this "intramolecular coordinating confinement" strategy, the biomass-derived nanocarbon-containing native intramolecular N,S heteroatoms are impressively applied to fabricate DACs with N,S–carbon coordinated uniform (Cu,Mn) hetero-nuclear active pairs on a gram-scale (>5 g). The as-synthesized (Cu,Mn)/NSC electrocatalyst exhibits superior oxygen reduction reaction (ORR) activity, delivering a half-wave potential of 0.93 V vs. RHE in alkaline media and 0.78 V vs. RHE in acid media. The unique microenvironment in DACs for the ORR is deeply visualized by simulated calculations. This work provides a solution to challenges in controllable and scalable fabrication of DACs. [ABSTRACT FROM AUTHOR]

Li–CO2 batteries have attracted close attention due to their ability to simultaneously store energy and capture CO2. The development of suitable catalytic cathodes plays a decisive role in promoting the electrochemical performance of Li–CO2 batteries. Herein, an electrocatalytic cathode material based on oxygen-decorated CoP nanosheets is reported. Benefiting from the enhanced electrical conductivity brought about by the presence of P element, the construction of catalytically active sites brought about by the presence of Co–O bonds, and the full exposure of catalytically active sites brought about by the two-dimensional morphology, Li–CO2 batteries exhibit good cycling characteristics (>1000 h) and excellent discharge capacity (13 200 mA h g−1). Density functional theory (DFT) calculations demonstrate that the efficient construction of O–Co–P bonds is the key to improving the performance of electrocatalytic cathodes. This provides an effective reference for the subsequent development of efficient catalytic cathodes. [ABSTRACT FROM AUTHOR]

The ingenious design of high-performance tin-based lithium-ion batteries (LIBs) is challenging due to their poor conductivity and drastic volume change during continuous lithiation/delithiation cycles. Herein, we present a strategy to confine heterostructured SnSe2–SnO2 nanoparticles into macroscopic nitrogen-doped carbon microbelts (SnSe2–SnO2@NC) as anode materials for LIBs. The composites exhibit an excellent specific capacity of 436.3 mA h g−1 even at 20 A g−1 and an ultrastable specific capacity of 632.7 mA h g−1 after 2800 cycles at 5 A g−1. Density Functional Theory (DFT) calculations reveal that metallic SnSe2–SnO2 heterostructures endow the lithium atoms at the interface with high adsorption energy, which promotes the anchoring of Li atoms, and enhances the electrical conductivity of the anode materials. This demonstrates the superior Li+ storage performance of the SnSe2–SnO2@NC microbelts as anode materials. [ABSTRACT FROM AUTHOR]

Visible (VIS) and near-infrared (NIR) mechanoluminescence (ML) materials have been developed rapidly for use in energy conversion, biological applications and mechanical sensing. The realization of visible and NIR ML in single host materials meets the dual requirements of visualization and anti-interference for high-precision mechanical sensing. In this work, Mn2+ single-doped magnesium aluminate spinel MgAl2O4 with excellent ML performance was studied in detail. Bright, visible green and NIR ML were achieved under mechanical stimulation, and the ratio between visible and NIR ML intensity can be regulated by manipulating the doping concentration of Mn2+. The generation of ML without additional pre-irradiation proved that the self-powered ML phenomenon was independent of trap. The functional relationship between mechanical parameters and ML intensity indicated that the doped spinel can be used for visualization, anti-interference and non-contact mechanical sensing. In addition, the NIR ML of MgAl2O4:Mn2+, centered at 835 nm, is located in the first NIR window (NIR-I, 650–950 nm), which effectively penetrates living tissue such as skin, fat, and lean meat, respectively, showing that it has potential applications in in vivo optical imaging. [ABSTRACT FROM AUTHOR]

Herein, a bimetallic sulfide Fe0.4Co0.6S2@NC nanobox was prepared via a simple two-step synthetic route. The N-doped carbon coated hollow nanobox was derived from a Prussian blue analogue (PBA) and applied for an SIB anode. As expected, it exhibits a high capacity (486.6 mA h g−1 at 0.1 A g−1) and displays an excellent cycling stability (230 mA h g−1 at 10 A g−1 after 900 cycles). [ABSTRACT FROM AUTHOR]

The output performance of triboelectric nanogenerators (TENGs) basically depends on the inherent nature of friction electrode materials. In this work, a series of isostructural Cu(I)-CPs (coordination polymers) with different terminal coordination groups from the same main group, formulated as [Cu(μ3-H3ttc)X]n (1: X = Cl, 2: X = Br and 3: X = I; H3ttc = trithiocyanuric acid), were chosen as the friction electrode materials to fabricate TENGs (Cl-, Br- and I-TENG based on compounds 1–3, respectively) to clearly clarify the influence of chemical microcomposition on the output performance of TENGs. The results indicated that the polarity of the compounds determined from dielectric constants was greatly affected by the halogen elements, which plays a decisive role in the output performance of the TENGs. I-TENG based on the Cu(I)-CP containing the least electronegative halogen atoms but with the largest polarity had the largest output performance, followed by Br- and Cl-TENG. As a practical application, I-TENG was used as a power source to construct a self-powered anticorrosion system to protect metal materials from corrosion. [ABSTRACT FROM AUTHOR]

Biosensors are currently among the most commonly used devices for analysing biomarkers and play an important role in environmental detection, food safety, and disease diagnosis. Researchers have developed multimodal biosensors instead of single-modal biosensors to meet increasing sensitivity, accuracy, and stability requirements. Metal nanoparticles (MNPs) are beneficial for preparing core probes for multimodal biosensors because of their excellent physical and chemical properties, such as easy regulation and modification, and because they can integrate diverse sensing strategies. This review mainly summarizes the excellent physicochemical properties of MNPs applied as biosensing probes and the principles of commonly used MNP-based multimodal sensing strategies. Recent applications and possible improvements of multimodal biosensors based on MNPs are also described, among which on-site inspection and sensitive detection are particularly important. The current challenges and prospects for multimodal biosensors based on MNPs may provide readers with a new perspective on this field.

Although antibacterial platforms involving nanozymes have been extensively investigated, there are still problems of poor reactive oxygen species generation efficiency and obstinate bacterial biofilms. Developing a nanozyme-photothermal therapy nanoplatform with superior sterilization effects and minimal side effects would be a good alternative for completely eliminating bacteria and biofilms. Herein, an ultrathin PdMo bimetallene nanozyme with a planar topology and boosted metal utilization, exhibiting excellent photothermal and peroxidase-like activity, is designed for synergistic nanozyme-photothermal sterilization applications and accelerated wound healing. The superior catalytic activity of PdMo bimetallene nanozymes could convert a biosafe concentration of hydrogen peroxide (H 2 O 2 ) into large quantities of toxic hydroxyl radicals (•OH) under laser irradiation, enhancing bacterial membrane permeability and thermal sensitivity for efficient removal of bacteria and biofilms. In addition, PdMo bimetallene presents a good wound-healing ability according to the results of fibroblast proliferation and collagen deposition with minor side effects. This work would provide an innovative avenue for developing metallene-based nanozymes for biomedical applications.

Tyrosyl-DNA phosphodiesterase 1 (TDP1) is a member of the phospholipase D family that can downregulate the anticancer effects of the type I topoisomerase (TOP1) inhibitors by hydrolyzing the 3'-phosphodiester bond between DNA and the TOP1 residue Y723 in the critical stalled intermediate that is the foundation of TOP1 inhibitor mechanism of action. Thus, TDP1 antagonists are attractive as potential enhancers of TOP1 inhibitors. However, the open and extended nature of the TOP1-DNA substrate-binding region has made the development of TDP1 inhibitors extremely challenging. In this study, starting from our recently identified small molecule microarray (SMM)-derived TDP1-inhibitory imidazopyridine motif, we employed a click-based oxime protocol to extend the parent platform into the DNA and TOP1 peptide substrate-binding channels. We applied one-pot Groebke-Blackburn-Bienayme multicomponent reactions (GBBRs) to prepare the needed aminooxy-containing substrates. By reacting these precursors with approximately 250 aldehydes in microtiter format, we screened a library of nearly 500 oximes for their TDP1 inhibitory potencies using an in vitro florescence-based catalytic assay. Select hits were structurally explored as their triazole- and ether-based isosteres. We obtained crystal structures of two of the resulting inhibitors bound to the TDP1 catalytic domain. The structures reveal that the inhibitors form hydrogen bonds with the catalytic His-Lys-Asn triads ("HKN" motifs: H263, K265, N283 and H493, K495, N516), while simultaneously extending into both the substrate DNA and TOP1 peptide-binding grooves. This work provides a structural model for developing multivalent TDP1 inhibitors capable of binding in a tridentate fashion with a central component situated within the catalytic pocket and extensions that project into both the DNA and TOP1 peptide substrate-binding regions., Competing Interests: Aspects of the work presented are contained within one or more patent applications. The authors declare that there is no conflict of interest., (This journal is © The Royal Society of Chemistry.)

Herein, ultrasmall nanostructured Co 3 O 4 particles have been prepared by a facile two-step synthetic method and furthermore applied to lithium-ion batteries. Benefitting from an increased specific surface area and improved tolerance for volume expansion, they deliver an extremely high specific capacity of 1432.7 mA h g -1 at 0.1 A g -1 and an outstandingly long cycle life with about 511.2 mA h g -1 at 10 A g -1 after 2000 cycles. This work will pave a new way to engineer advanced electrode materials for long-lived high-rate lithium-ion batteries.

Visible (VIS) and near-infrared (NIR) mechanoluminescence (ML) materials have been developed rapidly for use in energy conversion, biological applications and mechanical sensing. The realization of visible and NIR ML in single host materials meets the dual requirements of visualization and anti-interference for high-precision mechanical sensing. In this work, Mn 2+ single-doped magnesium aluminate spinel MgAl 2 O 4 with excellent ML performance was studied in detail. Bright, visible green and NIR ML were achieved under mechanical stimulation, and the ratio between visible and NIR ML intensity can be regulated by manipulating the doping concentration of Mn 2+ . The generation of ML without additional pre-irradiation proved that the self-powered ML phenomenon was independent of trap. The functional relationship between mechanical parameters and ML intensity indicated that the doped spinel can be used for visualization, anti-interference and non-contact mechanical sensing. In addition, the NIR ML of MgAl 2 O 4 :Mn 2+ , centered at 835 nm, is located in the first NIR window (NIR-I, 650-950 nm), which effectively penetrates living tissue such as skin, fat, and lean meat, respectively, showing that it has potential applications in in vivo optical imaging.

The ingenious design of high-performance tin-based lithium-ion batteries (LIBs) is challenging due to their poor conductivity and drastic volume change during continuous lithiation/delithiation cycles. Herein, we present a strategy to confine heterostructured SnSe 2 -SnO 2 nanoparticles into macroscopic nitrogen-doped carbon microbelts (SnSe 2 -SnO 2 @NC) as anode materials for LIBs. The composites exhibit an excellent specific capacity of 436.3 mA h g -1 even at 20 A g -1 and an ultrastable specific capacity of 632.7 mA h g -1 after 2800 cycles at 5 A g -1 . Density Functional Theory (DFT) calculations reveal that metallic SnSe 2 -SnO 2 heterostructures endow the lithium atoms at the interface with high adsorption energy, which promotes the anchoring of Li atoms, and enhances the electrical conductivity of the anode materials. This demonstrates the superior Li + storage performance of the SnSe 2 -SnO 2 @NC microbelts as anode materials.

Herein, a bimetallic sulfide Fe 0.4 Co 0.6 S 2 @NC nanobox was prepared via a simple two-step synthetic route. The N-doped carbon coated hollow nanobox was derived from a Prussian blue analogue (PBA) and applied for an SIB anode. As expected, it exhibits a high capacity (486.6 mA h g -1 at 0.1 A g -1 ) and displays an excellent cycling stability (230 mA h g -1 at 10 A g -1 after 900 cycles).