All-in-One Zeolite-Carbon-Based Nanotheranostics with Adjustable NIR-II Window Photoacoustic/Fluorescence Imaging Performance for Precise NIR-II Photothermal-Synergized Catalytic Antitumor Therapy.

In the second near-infrared (NIR-II) biowindow, multimodal optical imaging-guided precise antitumor therapy is a novel strategy for high-efficiency tumor theranostics, however, the all-in-one dual NIR-II photoacoustic (NIR-II PA) and NIR-II fluorescence (NIR-II FL) nanoprobes have been rarely reported mainly due to the short of a simple and universal design approach. Herein, a NIR-II PA/NIR-II FL imaging-adjustable nanozyme (HSC-2) is designed and developed to guide precise photothermal-catalytic synergistic therapy. Based on the ionic liquids adsorption capacity, the electronic structure of zeolite nano-Beta (three dimensional 12-ring pore system and large surface area) can be turned from the indirect band gap to direct band gap via doping carbon in the framework, resulting in outstanding NIR-II FL emission characteristics. As the silicon etching reaction proceeds, HSC-2 shows superior dual-modal NIR-II PA/NIR-II FL imaging performance facilitated by the optimal silicon-to-carbon ratio, simultaneously ensuring efficient tumor photothermal therapy (PTT) in the NIR-II window. Impressively, the peroxidase-mimic activity of HSC-2 in the tumor microenvironment could be further remarkably enhanced by its photothermal effect, leading to excellent synergistic PTT/catalytic therapy. Moreover, the HSC-2 exhibits dual-enzyme activity, and its catalase-like property could effectively eliminate excessive ROS for protection of the normal cells.

Hollow carbon-based nanosystem for photoacoustic imaging-guided hydrogenothermal therapy in the second near-infrared window.

Compared with the near-infrared-I spectral window (NIR-I, 650-950 nm), a newly developed imaging and treatment window with a 1000-1700 nm range (defined as the NIR-II bio-window) has attracted much attention owing to its higher spatiotemporal resolution, increased tissue penetration depth and therapeutic efficacy. Herein, we designed a nanotheranostic platform (HC-AB NPs) via loading ammonia borane (AB) into hollow carbon nanoparticles (HCs) for NIR-II photoacoustic (PA) imaging-guided NIR-II hydrogenothermal therapy. Importantly, by exploiting the characteristics of beta zeolite as a hard template and a template-carbonization-corrosion process, the prepared HCs have excellent NIR-II absorption performance and AB loading capacity. With the high biocompatibility of HC-AB NPs, an efficient synergistic anti-tumor strategy has been achieved via high intratumoural accumulation and acid-stimulated H2 release as well as PA-guided precise NIR-II photothermal therapy. The HC-AB NPs as a promising nanotheranostic platform opens a new avenue for high-efficacy NIR-II hydrogenothermal therapy.

Biodegradable Multifunctional Nanotheranostic Based on Ag2S-Doped Hollow BSA-SiO2 for Enhancing ROS-Feedback Synergistic Antitumor Therapy.

Stimuli-responsive silica nanoparticles are an attractive therapeutic agent for effective tumor ablation, but the responsiveness of silica nanoagents is limited by intrastimulation level and silica framework structure. Herein, a biodegradable hollow SiO2-based nanosystem (Ag2S-GOx@BHS NYs) is developed by a novel one-step dual-template (bovine serum albumin (BSA) and cetyltrimethylammonium bromide (CTAB)) synthetic strategy for image-guided therapy. The Ag2S-GOx@BHS NYs can be specifically activated in the tumor microenvironment via a self-feedback mechanism to achieve reactive oxygen species (ROS)-induced multistep therapy. In response to the inherent acidity and H2O2 at the tumor sites, Ag2S-GOx@BHS would accelerate the structural degradation while releasing glucose oxidase (GOx), which could efficiently deplete intratumoral glucose to copious amounts of gluconic acid and H2O2. More importantly, the sufficient H2O2 not only acts as a reactant to generate Ag+ from Ag2S for metal-ion therapy and improves the oxidative stress but also combines with gluconic acid results in the self-accelerating degradation process. Moreover, the released Ag2S nanoparticles can help the Ag2S-GOx@BHS NYs realize the second near-infrared window fluorescence (NIR-II FL) and photoacoustic (PA) imaging-guided precise photothermal therapy (PTT). Taken together, the development of a self-feedback nanosystem may open up a new dimension for a highly effective multistep tumor therapy.

Paeonol inhibits NLRP3 mediated inflammation in rat endothelial cells by elevating hyperlipidemic rats plasma exosomal miRNA-223.

Atherosclerosis (AS) is a multifactorial chronic inflammatory disease, and hyperlipidemia is the important factors leading to AS, which can cause vascular endothelial dysfunction. Paeonol (Pae) is a potential therapeutic drug for AS, and we have previously shown that Pae regulated the expression of monocytes-derived exosomal microRNA-223 (miR-223). However, the mechanisms of the anti-AS effect of Pae are still not fully understood. In this study, we aim to investigate if Pae could inhibit NLRP3 inflammasome mediated inflammation via elevating hyperlipidemic rats plasma-derived exosomal miR-223. We used high-fat-diet induced hyperlipidemic rats as model for further investigation. Rats were treated with Pae (75, 150 or 300 mg/kg) orally, and then exosomes were isolated from hyperlipidemic rat plasma by ultracentrifugation. In vivo experiments confirmed that Pae markedly reduced serum TC, TG, IL-1ß, and IL-6 levels. Both CCK-8 and trypan blue staining showed that the survival rate of rat aortic endothelial cells (RAECs) in the Pae-exo group was higher than that in the model group. Also, Pae-exo dose-dependently increased the survival rate of RAECs and reduced inflammatory cytokines level (IL-1ß, and IL-6). Furthermore, Pae-exo successfully increased the expression of exosomal miR-223 and relieved inflammatory secretion. Finally, decreased expression of NLRP3, ASC, caspase-1 and ICAM-1 indicated that Pae-exo attenuated inflammatory reaction of RAECs by suppressing NLRP3 signaling pathway. Altogether, our results showed that Pae inhibited the downstream NLRP3 inflammasome pathway by increasing the level of miR-223 in plasma derived exosomes of hyperlipidemic rats, providing new insights in the treatment of AS with the use of Pae.

A sinter-resistant catalytic system based on ultra-small Ni-Cu nanoparticles encapsulated in Ca-SiO2 for high-performance ethanol steam reforming.

To enhance the catalytic performance of catalysts for the ethanol steam reforming (ESR) reaction, a facile reverse micelle strategy was adopted to prepare a core@shell Ni-Cu@Ca-SiO2 (Ni-Cu@CS) nanoreactor composed of an ultra-small Ni-Cu alloy (∼2.8 nm) encapsulated in Ca-functionalized SiO2 nanoparticles. Benefiting from its core@shell structural features and unique components, the Ni-Cu@CS nanoreactor exhibited superior activity (69.91% H2 selectivity and 99.99% ethanol conversion) and stability compared to reference samples. The regenerated Ni-Cu@CS nanoreactor showed high stability, maintaining 98.14% ethanol conversion and only 1.98 mg gcat-1 h-1 in carbon deposition. The high catalytic performance of Ni-Cu@CS is attributed to not only its encapsulated structure, which effectively prevented the sintering of neighboring Ni-Cu alloy nanoparticles, but also to its Ca-functionalized porous SiO2 shell, suppressing the carbon deposition. Moreover, its porous thin shell facilitated the mass transfer and diffusion of reactants and products. Thus, the Ni-Cu@CS nanoreactor is expected to become a new type of high-efficiency nanoreactor for the ESR reaction.

Paeonol prevents lipid metabolism dysfunction in palmitic acid-induced HepG2 injury through promoting SIRT1-FoxO1-ATG14-dependent autophagy.

This study aimed to investigate the effects of paeonol (Pae) on lipid metabolism in palmitic acid (PA)-induced injury of HepG2, and to evaluate the protective mechanisms. Lipid metabolism dysfunction of HepG2 cells was produced by administration of palmitic acid (PA). The cells were pretreated with different concentrations of Pae. MTT method was used to detect the cell survival; lipid metabolism was evaluated based on total cholesterol (TC), triglycerides (TG); Western blotting was used to detect the expression of Sirtuin 1 (SIRT1), autophagy related 14 (ATG14), microtubule-associated protein 1A/1B-light chain 3 (LC3) and p62 proteins; immunoprecipitation was used to detect the expression of acetylated FoxO1. After treatment for 24 h, the inhibitory concentration 50 (IC50) of PA in HepG2 cells was about 566.8 µM. Pae at the concentration range from 7.5 to 30 µM did not affect cell viability. Thus, 500 µM PA was used to model metabolism dysfunction and Pae at the concentration range was selected to investigate the protective effect. Compared with the normal control group, the cell survival rate decreased, the number of lipid droplets, and TC and TG levels increased in the model group. Compared with model group, the cell survival rate of Pae (7.5, 15, 30 µM) group increased, the number of lipid droplets and content of TC and TG decreased, the ratio of LC3-II/I increased and p62 expression decreased with pretreatment of Pae. Additionally, Pae pretreatment promoted SIRT1 and ATG14 expression, but reduced acetylated FoxO1 levels in PA-treated cells. Most importantly, autophagy inhibitor, as well as SIRT1 inhibitor blocked the effects of Pae on PA-induced cell injury and metabolism dysfunction, respectively. Pae prevents lipid metabolism dysfunction in PA-induced HepG2 injury by promoting SIRT1-FoxO1-ATG14-dependent autophagy.

Fabrication of Highly Dispersed Cu-Based Oxides as Desirable NH3-SCR Catalysts via Employing CNTs To Decorate the CuAl-Layered Double Hydroxides.

In this study, three kinds of CuAl-LDO/CNT (LDO, layered double oxide) catalysts were prepared by the assembly of CNTs and CuAl-LDH (LDH, layered double hydroxides) as well as subsequently structural topological transformation. The effects of the assembly method on the surface structure property and the DeNOx performance of the prepared samples were systematically investigated. It was found that three CuAl-LDO/CNT catalysts showed preferable NH3-SCR catalytic performance compared with CuAl-LDO where the catalyst CuAl-LDO/CNTs(I) exhibited optimum NOx conversion (>80%) and N2 selectivity (>90%) within 180-300 °C. Such fine catalytic performance can be attributed to the proper surface acidity and redox ability of the catalyst, which might be correlated with the high dispersion of Cu-based active centers caused by the induced nucleation and effective separation action of LDH by carbon nanotubes. In addition, the outstanding H2O and SO2 resistance of the CuAl-LDO/CNTs(I) catalyst was also obtained because of the synergistic effect between CuAl-LDO and CNTs, which could greatly promote the activation and decomposition of ammonium sulfate at lower temperatures.

Tunable preparation of highly dispersed Ni x Mn-LDO catalysts derived from Ni x Mn-LDHs precursors and application in low-temperature NH3-SCR reactions.

A series of Ni x Mn bimixed metal oxides (Ni x Mn-LDO) were prepared via calcining Ni x Mn layered double hydroxides (Ni x Mn-LDHs) precursors at 400 °C and applied as catalysts in the selective catalytic reduction (SCR) of NO x with NH3. The DeNO x performance of catalysts was optimized by adjusting the Ni/Mn molar ratios of Ni x Mn-LDO precursors, in which Ni5Mn-LDO exhibited above 90% NO x conversion and N2 selectivity at a temperature zone of 180-360 °C. Besides, Ni5Mn-LDO possessed considerable SO2 & H2O resistance and outstanding stability. Multiple characterization techniques were used to analyze the physicochemical properties of the catalysts. The analysis results indicated that all catalysts had the same active species Ni6MnO8, while their particle sizes showed significant differences. Notably, the uniform distribution of active species particles in the Ni5Mn-LDO catalyst provided the rich surface acidity and suitable redox ability which were the primary causes for its desirable DeNO x property.

Paeonol Attenuated Inflammatory Response of Endothelial Cells via Stimulating Monocytes-Derived Exosomal MicroRNA-223.

Introduction: Paeonol, an active compound isolated from the radix of Cortex Moutan, has been shown to have anti-atherosclerosis effects by regulating blood cells' function and protecting vascular cells injury. Besides, emerging evidences has proven that exosomes might play a pivotal role in intercellular communication by transmiting proteins and microRNAs from cell to cell. However, the relationship between monocytes-derived exosomal microRNA-223 and vascular inflammation injury along with paeonol' effects are still not clear. Objective: Our study aimed to explain whether paeonol's protective effect on inflammatory response is related to the regulation of exosomal microRNA-223 in the VECs. Methods: ApoE-/- mice were fed with high fat diet to replicate the AS model. HE staining and immunohistochemistry was used to detect inflammatory response of aorta. The expression of IL-1ß and IL-6 were detected by ELISA. Western blot was used to detect the expression of STAT3, pSTAT3, ICAM-1 and VCAM-1. qRT-PCR was used to detect miR-223 expression. Exosomes were extracted from THP-1 cells by differential centrifugation and observed by transmission electron microscope. Observation of exosomes uptake into HUVECs was realized by laser microscopy. miR-223 target gene was detected by double luciferase gene report test. Results: In vivo experiments confirmed that paeonol restricted atherosclerosis development and increased miR-223 expression, inhibited STAT3 pathway in ApoE-/- mice. In vitro, miR-223 showed robust presence in THP-1 cells and undetectable in HUVECs. And we had observed that miR-223 could be internalized from THP-1 cells into HUVECs taking exosomes as a carrier. Paeonol obviously increased miR-223 expression in co-cultured HUVECs and exosomes in concentration dependent manner, compared to LPS group. In addition, paeonol relieved inflammatory secretion, adhesion and STAT3 expression in HUVECs, which could be inverted after miR-223 inhibitor transfection into THP-1 cells. Conclusion: Paeonol could increase the expression of miR-223 in THP-1 derived exosomes and in HUVECs after uptake of exosomes, whereas decrease the expression of STAT3, p-STAT3 in HUVECs. Ultimately paeonol decreased the expression of IL-1ß, IL-6, ICAM-1, VCAM-1 in HUVECs and alleviated adhesion of THP-1 cells to HUVECs.

Synthesis and catalytic performance of hierarchically structured MOR zeolites by a dual-functional templating approach.

Novel hierarchical MOR zeolites have been successfully synthesized via a one-step dual-functional templating strategy utilizing gemini organic surfactant (C18-2-8) through hydrothermal process. After a period of ∼96 h for crystallization, the hierarchy MOR zeolite with a larger BET (412.0 m2/g), abundant intracrystalline mesopores (average mesopore size distribution of 4.55 nm), and more accessible acid sites can be synthesized. The XRD study revealed a long range structural ordering of mesoporous and a good crystallinity of microporous structure. The results indicated that the surfactant acted as a dual-functional template for generating both micropores and mesopores simultaneously. Compared with conventional MOR zeolite, hierarchically structured MOR zeolite not only has higher activity and stability, but also can avoid side-reaction taking place in ethanol dehydration reactions. This hierarchical micro/mesostructured mordenite zeolite may be a candidate for practical industrial applications especially in those reactions where bulky molecules are involved.

Cascade upgrading of γ-valerolactone to biofuels.

Cascade upgrading of γ-valerolactone (GVL), produced from renewable cellulosic biomass, with selective conversion to biofuels pentyl valerate (PV) and pentane in one pot using a bifunctional Pd/HY catalyst is described. Excellent catalytic performance (over 99% conversion of GVL, 60.6% yield of PV and 22.9% yield of pentane) was achieved in one step. These biofuels can be targeted for gasoline and jet fuel applications.