Latest ArticlesNicotinamide adenine dinucleotide (NADH) regeneration is necessary for the sustainable application of enzymatic industry. The Rh-based complex [Cp*Rh(bpy)(H)]+ has been widely used as an important mediator in NADH regeneration systems, but it is limited by complexity and high cost. Here, a Z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots (CN-CNQD). The resultant catalyst achieved a high yield of NADH in a mediator-free (M-free) system of 0.283 mmol L−1 g−1 min−1, which is 5.29 times that of pure CN. ADH enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21% selectivity in the M-free system. Mechanism research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system, while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free system. The immobilized Rh shows more competitiveness than [Cp*Rh(bpy)(H)]+. This study contributes to the construction of an M-free system for further application in greener, lower-cost enzymatic processes.
We report SiO2-supported monometallic Pt, Pd, Au, Ni, Cu and Co catalysts for proton-driven NAD+ regeneration, co-producing H2. All metals are fully selective to NAD+ where the order of turnover frequencies (Pt > Pd > Cu > Au, Ni and Co) coincides with those otherwise observed in electrochemical hydrogen evolution reactions. This has revealed that NADH is capable of converting the metal sites into a "cathode" without an external potential and the NADH to NAD+ reaction involves transferring electron and hydrogen atom separately. Electron-deficient Ptδ+ (on CeO2) enhances TOF and the heterogeneous Pt/CeO2 catalyst is recyclable without losing any activity/selectivity.
Paclitaxel (PTX) is widely applied for the treatment of unresectable and metastasis breast carcinoma as well as other cancers, whereas its efficacy is always impeded by poor solubility. Liposomes are one kind of the most successful drug carriers which are capable of solubilizing PTX and improving patients' tolerance owing to excellent biocompatibility and biodegradability. However, poor compatibility between PTX and liposomes compromises the stability, drug loading and anti-tumor capacity of liposomal formulations. To address this issue, three lipids with various chain lengths, namely, myristic acid (MA, 14C), palmitic acid (PA, 16C) and stearic acid (SA, 18C), were conjugated to PTX via ester bonds and the synthesized prodrugs with high lipophilicity were further formulated into liposomes, respectively. All liposomes show high stability and drug loadings, as well as sustained drug release. The chain lengths of lipids are negatively correlated with drug release and enzymatic conversion rates, which further impact the pharmacokinetics, tumor accumulation, and anti-tumor efficacy of liposomal PTX. Neither rapid nor slow drug release facilitates high tumor accumulation as well as anti-tumor efficacy of PTX. Among all liposomes, PTX-PA-loaded liposomes show the longest circulation and highest tumor accumulation of PTX and exert the most potent anti-tumor capacities in vivo, owing to its moderate drug release and enzymatic conversion rate. Witnessing its superior safety, PTX-PA liposomes hold potential for further clinical translation.
Small interfering RNA (siRNA)-based gene silencing has been considered as a potential therapy modality against inflammatory diseases. Nevertheless, the effective delivery of siRNA to desired destination still remains challenging due to poor stability, high molecular weight and negative charge. Currently, ionizable lipid nanoparticle (LNP) has been extensively used as vector for effective delivery of siRNA. Herein, we report a mannose-modified LNP (M-MC3 LNP@TNFα) loading tumor necrosis factor α (TNFα) siRNA for targeting liver macrophages, achieving effectively inhibit acute liver injury. The M-MC3 LNP@TNFα not only increases the internalization of LNP by macrophages, but also enhances the gene silencing efficiency of TNFα in vitro. Additionally, the M-MC3 LNP@TNFα exhibits higher accumulation in liver of healthy mice than that of MC3 LNP@TNFα (un-modified LNP) owing to the targeting effect of mannose. As expected, the M-MC3 LNP@TNFα significantly suppresses the expression of TNFα and ameliorates liver damage in acute liver injury model. Such a LNP targeting siRNA delivery holds great potential for the treatment of diseases associated with liver in the future.
Antimicrobial photodynamic therapy (aPDT) has been considered a noninvasive and effective modality against the bacterial infection of peri–implantitis, especially the aPDT triggered by near-infrared (NIR) light due to the large penetration depth in tissue. However, the complexity of hypoxia microenvironments and the distance of aPDT sterilization still pose challenges before realizing the aPDT clinical application. Due to the long lifespan and transmission distance of therapeutic gas molecules, we design a multi-functional gas generator that combines aPDT as well as O2 and CO gas release function, which can solve the problem of hypoxia (O2) in PDT and the problem of inflammation regulation (CO) in the distal part of peri–implant inflammation under near-infrared (NIR) irradiation. In the composite nanoplatform that spin-coated on the surface of titanium implants, up-conversion nanoparticles (UCNPs) were involved in converting the NIR to visible, which further excites the partially oxidized stannic sulfide (SnS2), realizing the therapeutic gas release. Indocyanine green (ICG) was further integrated to enhance the aPDT performance (Ti-U@SnS2/I). Therefore, reactive oxygen species (ROS), CO, and O2 can be controllably administered via a composite nano-platform mediated by a single NIR light (808 nm). This implant surface modification strategy could achieve great self-enhancement antibacterial effectiveness and regulate the lingering questions, such as relieving the anoxic microenvironment and reaching deep infection sites, providing a viable antibiotic-free technique to combat peri–implantitis.
Two-dimensional (2D) MXenes have emerged as an archetypical layered material combining the properties of an organic-inorganic hybrid offering materials sustainability for a range of applications. Their surface functional groups and the associated chemical properties' tailorability through functionalizing MXenes with other materials as well as hydrophilicity and high conductivity enable them to be the best successor for various applications in textile industries, especially in the advancement of smart textiles and remediation of textile wastewater. MXene-based textile composite performs superb smartness in high-performance wearables as well as in the reduction of textile dyes from wastewater. This article critically reviews the significance of MXenes in two sectors of the textile industry. Firstly, we review the improvement of textile raw materials such as fiber, yarn, and fabric by using MXene as electrodes in supercapacitors, pressure sensors. Secondly, we review advancements in the removal of dyes from textile wastewater utilizing MXene as an absorbent by the adsorption process. MXene-based textiles demonstrated superior strength through the strong bonding between MXene and textile structures as well as the treatment of adsorbate by adsorbent (MXene in the adsorption process). We identify critical gaps for further research to enable their real-life applications.
We report a facile template-free fabrication of heterostructured Co3O4/CuO hollow nanospheres using pre-synthesized Co/Cu-glycerate as conformal precursor. The introduction of copper nitrate in the solvothermal reaction system of glycerol/isopropanol/cobalt nitrate readily induces the conversion from solid Co-glycerate to hollow Co/Cu-glycerate nanospheres, and the effect of the Co/Cu atomic ratio on the structure evolution of the metal glycerates as well as their corresponding oxides were investigated. When examined as anode materials for lithium-ion batteries, the well-defined Co3O4/CuO hollow nanospheres with Co/Cu molar ratio of 2.0 demonstrate excellent lithium storage performance, delivering a high reversible capacity of 930 mAh/g after 300 cycles at a current density of 0.5 A/g and a stable capacity of 650 mAh/g after 500 cycles even at a higher current density of 2.0 A/g, which are much better than their counterparts of bare CuO and Co3O4. The enhanced lithium storage performance can be attributed to the synergistic effect of the CuO and Co3O4 heterostructure with hollow spherical morphology, which greatly enhances the charge/electrolyte transfer and effectively buffers the volume changes upon lithiation/delithiation cycling.
Partial substitution of polyoxometalate (POM) is an efficient route to modulate the catalytic property of maternal POM. In this work, a new Keggin type POM involving {Ni6} cluster, {[Ni(H2O)2(Dach)2][Ni(Dach)2]2}{[Ni6Cl(μ-OH)3(H2O)(Dach)3(WO4)(PW9O34)][Ni6(μ-OH)3(H2O)2(Dach)3(WO4)(PW9O34)]}Cl·27H2O, (1, Dach = 1,2-diaminocyclohexane) was synthesized. Compounds 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene (AOB) in water. The apparently different results from that with the matrix {PW9O34} ({PW9}) suggest the successful regulation of the catalytic property of {PW9} by the introduction of the {Ni6} cluster into the skeleton. The experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites, which are respectively responsible for the oxidation and condensation steps in the production of AOB. The good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites, respectively.
Diversity-oriented synthesis is a powerful and interesting synthetic tool for the rapid construction of structurally complex and privileged scaffolds from readily accessible starting materials. To date, diversity-oriented synthesis mostly relies on the employment of versatile reagents. Versatile reagents can be regulated as controllable and flexible building blocks for multipurpose utilizations. Over the past decade, a variety of multifunctional reagents have been developed. However, most versatile reagents usually need multi-step synthesis, thus restricting their wide application to a large extent. In terms of the practicalities and universalities, we prefer to pay more attention to the utilization of simple and practical versatile reagents with multiple reactivities, mainly including atropaldehyde acetals, aryl methyl ketones, vinylene carbonate, vinyl azides, aryldiazonium salts, rongalite, halodifluoromethyl compounds. Most importantly, these versatile reagents can also play different roles simultaneously in the same reaction, in which their different reactivities are converged into the final target products. Such strategy can not only offer more possibilities for the synthesis of several active pharmaceutical ingredients, but also minimize the occurrence of some side reactions by lessening the varieties of materials. Also, a perspective is given at the end of this review.
As a new concept having emerged in last few years, the "deep eutectic solvents" (DESs) effect integrated into the imprinting technology inevitably exposes design limitations of stimuli-responsive molecularly imprinted polymers (MIPs), as well as inadequate analysis of the adsorption performance of MIPs. Herein, a simple yet defined N-isopropylacrylamide/(3-acrylamidopropyl) trimethylammonium chloride (NIPAM/APTMAC) binary DESs system was proposed to prepare intelligent MIPs with thermo-sensitivity. Accordingly, magnetic and thermo-responsive MIPs based on functional monomers-derived DESs (TM-DESs-MIPs1) were synthesized, revealing DESs effect-regulated affinity/kinetics for the enhanced adsorption capability, eco-friendly thermo-regulated elution for high release efficiency, and simple magnetic separation, along with superior selectivity to rhein (RH) and good regeneration ability. TM-DESs-MIPs1 were utilized to extract RH from Cassiae semen samples coupled with high performance liquid chromatography (HPLC), yielding satisfactory recoveries (79.47%−110.82%) and low limits of detection (LOD) (16.67 µg/L). Another two kinds of MIPs adopting the thermo-responsive moiety-derived DESs effect strategy further demonstrated great applicability of such intelligent MIPs for analyses of complicated samples.
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