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DYES AND PIGMENTS · 2022 · IF 5.122

An intelligent photosensitizer that selectively kills Gram-positive pathogenic cocci while preventing harm to beneficial bacilli

Le Wang,Xiaohong Pan,Shuzhi Tang,Yaqi Wang,Haixing Shi,Huanhuan Wang,Wenzhen Liu,Zhuo Chen

The skin microbiota is an inseparable component of the skin barrier structure, which participates in the stabilization or impairment of the barrier function as well as the development of many skin diseases. In order to maintain the stability of skin bacteria community structure, people pay more and more attention to protecting probiotics, such as bacilli, and killing pathogens, such as Gram-positive cocci. We herein report a negatively charged photosensitizer TPA-3NBA with aggregation-induced emission (AIE) characteristics, which was synthesized by one-step reaction, can selectively and rapidly stain (within 0.5 min) and effectively kill Gram-positive cocci (killing 6.0 log 10 of Staphylococcus aureus at a concentration of 1 μM) without affecting bacilli under white light irradiation. This selective bacterial imaging makes it possible to quickly identify locally bacterial infection. Furthermore, the normal concentration of divalent ion (Ca 2+ ) in human body can significantly promote the absorption of TPA-3NBA by Gram-positive cocci, thus improving its antibacterial activity. To the best of our knowledge, this is the first photosensitizer to be reported with good performance in selective bacterial imaging and removal of Gram-positive pathogenic cocci, indicating its potential application prospect in targeted antimicrobial therapy.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

The combined effects of nanoplastics and dibutyl phthalate on Streptomyces coelicolor M145

Xiaomei Liu,Jingkang Ma,Saisai Guo,Qingying Shi,Jingchun Tang

The environmental and human health risks posed by nanoplastics have attracted considerable attention; however, research on the combined toxicity of nanoplastics and plasticizers is limited. This study analyzed the combined effects of nanoplastics and dibutyl phthalate (DBP) on Streptomyces coelicolor M145 (herein referred to as M145) and its mechanism. The results demonstrated that when the concentration of both nanoplastics and DBP was 1 mg/L, the co-addition was not toxic to M145. When the DBP concentration increased to 5 mg/L, the combined toxicity of 1 mg/L nanoplastics and 5 mg/L DBP reduced when compared to the 5 mg/L DBP treatment group. Similarly, the combined toxicity of 10 mg/L nanoplastics and 1 mg/L DBP on M145 was also lower than that of only 10 mg/L nanoplastics. The co-addition of 10 mg/L nanoplastics and 5 mg/L DBP resulted in the lowest survival rate (41.3%). The key reason for differences in cytotoxicity were variations in the agglomeration of nanoplastics and the adsorption of DBP on nanoplastics. The combination of 10 mg/L nanoplastics and 5 mg/L DBP maximized the production of antibiotics; actinorhodin and undecylprodigiosin yields were 3.5 and 1.8-fold higher than that of the control, respectively. This indicates that the excessive production of antibiotics may be a protective mechanism for bacteria. This study provides a new perspective for assessing the risk of co-exposure to nanoplastics and organic contaminants on microorganisms in nature.

CAS / MDL: 175606-05-0
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2022 · IF 7.129

Microbiology combined with metabonomics revealing the response of soil microorganisms and their metabolic functions exposed to phthalic acid esters

Changcai Wu,Yajie Ma,Dan Wang,Yongpan Shan,Xianpeng Song,Hongyan Hu,Xiangliang Ren,Xiaoyan Ma,Junyu Luo,Jinjie Cui,Yan Ma

As microplastics became the focus of global attention, the hazards of plastic plasticizers (PAEs) have gradually attracted people's attention. Agricultural soil is one of its hardest hit areas. However, current research of its impact on soil ecology only stops at the microorganism itself, and there is still lack of conclusion on the impact of soil metabolism. To this end, three most common PAEs (Dimethyl phthalate: DMP, Dibutyl phthalate: DBP and Bis (2-ethylhexyl) phthalate: DEHP) were selected and based on high-throughput sequencing and metabolomics platforms, the influence of PAEs residues on soil metabolic functions were revealed for the first time. PAEs did not significantly changed the alpha diversity of soil bacteria in the short term, but changed their community structure and interfered with the complexity of community symbiosis network. Metabolomics indicated that exposure to DBP can significantly change the soil metabolite profile. A total of 172 differential metabolites were found, of which 100 were up-regulated and 72 were down-regulated. DBP treatment interfered with 43 metabolic pathways including basic metabolic processes. In particular, it interfered with the metabolism of residual steroids and promoted the metabolism of various plasticizers. In addition, through differential labeling and collinear analysis, some bacteria with the degradation potential of PAEs, such as Gordonia , were excavated.

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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Surface Coating of Pulmonary siRNA Delivery Vectors Enabling Mucus Penetration, Cell Targeting, and Intracellular Radical Scavenging for Enhanced Acute Lung Injury Therapy

Jiaojiao Zhu,Man Guo,Yanhui Cui,Yingcai Meng,Jinsong Ding,Wenbin Zeng,Wenhu Zhou

Pulmonary delivery of anti-inflammatory siRNA presents a promising approach for localized therapy of acute lung injury (ALI), while polycationic vectors can be easily trapped by the negatively charged airway mucin glycoproteins and arbitrarily internalized by epithelial cells with nontargetability for immunological clearance. Herein, we report a material, the dopamine (DA)-grafted hyaluronic acid (HA–DA), coating on an anti-TNF-α vector to address these limitations. HA–DA was simply synthesized and facilely coated on poly(β-amino ester) (BP)-based siRNA vectors via electrostatic attraction. The resulting HA–DA/BP/siRNA displayed significantly enhanced mucus penetration, attributable to the charge screen effect of HA–DA and the bioadhesive nature of the grafting DA. After transmucosal delivery, the nanosystem could target diseased macrophages via CD44-mediated internalization and rapidly escape from endo/lysosomes through the proton sponge effect, resulting in effective TNF-α regulation. Meanwhile, DA modification endowed the coating material with robust antioxidative capability to scavenge a broad spectrum of reactive oxygen/nitrogen species (RONS), which protected the lung tissue from oxidative damage and synergized with anti-TNF-α to inhibit a cytokine storm. As a result, a remarkable amelioration of ALI was achieved in a lipopolysaccharide (LPS)-stimulated mice model. This study provides a multifunctional coating material to facilitate pulmonary drug delivery for the treatment of lung diseases.

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Nanoscale Advances · 2022 ·Vol. 4 ·期 5 ·1414-1421 · IF 5.598

Hollow carbon nanospheres embedded with stoichiometric γ-Fe2O3 and GdPO4: tuning the nanospheres for in vitro and in vivo size effect evaluation

Hui Zhang,Jianping Zhang,Yi Chen,Tianze Wu,Mingzhu Lu,Zhenxia Chen,Yu Jia,Yongtai Yang,Yun Ling,Yaming Zhou

The size modulation of hollow carbon nanospheres (HCSs) has attracted great interest in the contexts of cellular uptake, drug delivery and bioimaging. In this study, a facile fabrication method was specifically used to minimize all influencing factors except for the particle size. A series of nanoparticles of hollow carbon nanospheres embedded with magnetic resonance imaging (MRI) nanoagent γ-Fe2O3 and GdPO4 nanoparticles (Fe–Gd/HCS), were successfully prepared and applied to in vitro/vivo evaluation with well-defined sizes of ∼100 nm (Fe–Gd/HCS-S), ∼200 nm (Fe–Gd/HCS-M), and ∼300 nm (Fe–Gd/HCS-L), respectively. Then the in vitro size effect of Fe–Gd/HCS was systematically investigated by bio-TEM, CLSM, CCK-8 assay, and flow cytometry revealing that Fe–Gd/HCS could be internalized and the cellular uptake amounts increase with the decrease of size. Furthermore, the in vivo size-effect behavior of Fe–Gd/HCS (∼100 nm, ∼200 nm, ∼300 nm) was tracked by MRI technique, demonstrating that all Fe–Gd/HCS can distinguish the liver, in which Fe–Gd/HCS with the smallest particle size exhibited the best performance among these nanoparticles. By leveraging on these features, Fe–Gd/HCS-S (∼100 nm) was further chosen as a theranostic agent, preliminarily presenting its capability for multi-modal imaging and therapy.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Journal of Materials Chemistry B · 2022 ·Vol. 10 ·期 10 ·1553-1560 · IF 7.571

Highly efficient synergistic biocatalysis driven by stably loaded enzymes within hierarchically porous iron/cobalt metal–organic framework via biomimetic mineralization

Hao Shen,Haimei Shi,Yi Yang,Jiayi Song,Chuanfan Ding,Shaoning Yu

The integration of multimodal chemo-/bio-catalysis for efficient cascade reactions has long provided broad prospects in the field of biotechnology for ages. In this work, we describe the synthesis of a biomimetic multienzyme hybrid with hierarchically porous structure and outstanding catalytic activity via in situ encapsulation of natural enzymes in an iron–cobalt bimetallic metal–organic framework (Fe/Co-MOF, FCM). The combination of a single enzyme (glucose oxidase) or dual enzyme (β-galactosidase and glucose oxidase) with FCM resulted in remarkable synergistic biocatalysis ability; in contrast to simple biocatalyst mixtures in solution, the prepared multienzyme hybrid resulted in 3.2-fold and 2.1-fold improvements in activity for tandem reactions, respectively. The reinforced cascade bioactivity of the multienzyme hybrid benefitted from the synergistic effect between iron/cobalt in the FCM nanozyme, the opened substrate channel between enzymes/nanozymes, and the beneficial effect provided by the hierarchical MOF pores. The enlarged pores not only provided adequate space for immobilized proteins to diffuse and reorientate in FCM with low surface energy, but also reduced the intrinsic mass transfer obstacle to increase the diffusional efficiency of reactants/intermediates. In addition, on account of the shielding effect provided by FCM, the multienzyme hybrid exhibited enhanced tolerance towards severe circumstances and excellent reusability and has been successfully applied in small molecule detection, such as glucose and lactose. The current study highlights the superiority of synergistic bioreactors integrated with the MOF nanozyme and natural enzymes, suggesting great potential for applications in sustainable biomimetic catalysis.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Antioxidation of a proteoglycan from Ganoderma lucidum protects pancreatic β-cells against oxidative stress-induced apoptosis in vitro and in vivo

Yanna Pan,Shilin Yuan,Yilong Teng,Zeng Zhang,Yanming He,Ying Zhang,Haohui Liang,Xiao Wu,Jiaqi Li,Hongjie Yang,Ping Zhou

Oxidative stress is one of the major factors in induction of pancreatic β-cell apoptosis and diabetes. Here, we investigated systematically the roles of a proteoglycan (namely, FYGL ) from Ganoderma lucidum in protection and repair of pancreatic β-cells against oxidative stress-induced injury and apoptosis on molecular, cellular and animal basis. FYGL in vitro had antioxidant activity in terms of scavenging of free radicals and reduction power. FYGL improved cells viability, insulin secretion, redox indicator expressions, and mitochondrial membrane potential in H 2 O 2 -induced INS-1 cell via regulating the activations of apoptosis-related mitogen-activated protein kinases (MAPK) and nuclear factor kappa B (NF-κB) pathways as well as the insulin secretion-related pathway. Thrillingly in vivo , FYGL repaired the injured pancreas, reduced the pancreatic β-cells apoptosis, and improved insulin secretion because of regulating the balance of oxidation-reduction, therefore well managed blood glucose in db/db diabetic mice. These results demonstrated that FYGL is promising to be used as a novel natural remedy for protection of pancreatic β-cells against oxidative stress in diabetes treatment.

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BIOSENSORS & BIOELECTRONICS · 2022 · IF 12.545

Nano-channel confined biomimetic nanozyme/bioenzyme cascade reaction for long-lasting and intensive chemiluminescence

Yaxue Jia,Siqi Zhao,Qishu Qu,Li Yang

We present here a novel nano-channel confined biomimetic nanozyme/bioenzyme system, which is prepared by co-immobilizing polyoxometalates (vanadomolybdophosphoric heteropoly acid, PMoV 2 ) and glucose oxidase (GOx) in the nano-scale channel of core-shell mesoporous silica (CSMS) microspheres . The biomimetic dual-enzyme nanoreactors ( [email protected] 2 @GOx) is used for producing long-lasting chemiluminescence (CL) emission. With glucose and luminol in the reaction mixture, hydrogen peroxide (H 2 O 2 ) is formed in mesoporous channels by GOx catalysis and then is consumed immediately by PMoV 2 to induce CL emission. Confined in nano-size channels of CSMS materials, the biomimetic cascade reactions can induce a long-lasting CL emission with a flat period over 12 h. The proposed [email protected] 2 @GOx system has excellent reproducibility and storage stability, and has been applied for glucose sensing in human serum samples with satisfactory accuracy. Our study provides a new glow-type CL system based on nanozyme/bioenzyme cascade reactions confined in nano-scale channels of CSMS microspheres, and will also shed a light on potential application of functional polyoxometalates immobilized in mesoporous materials , which would be of great value in various fields including bioassays and heterogeneous catalysis.

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DALTON TRANSACTIONS · 2022 ·Vol. 51 ·期 8 ·3331-3340 · IF 4.569

Enhancement in the active site exposure in a porphyrin-based PIL/graphene composite catalyst for the highly efficient conversion of CO2

Xiao-Xuan Guo,Feng-Lei Zhang,Yaseen Muhammad,Dong-Liang Hu,Zhao-Tian Cai,Guo-Min Xiao

Poly(ionic liquid)s (PILs) have gained widespread attention in recent years due to their excellent properties similar to both ionic liquids and polymers. However, their further applications are limited because abundant and flexible ions easily block nanopores in the PIL catalysts, thus blocking the active sites and ultimately leading to decreased catalytic activity. This work reports the synthesis of a PIL/graphene composite catalyst (iPOP-ZnTPy@GNFs) based on an in situ surface preparation strategy, which effectively controlled the particle size and dispersion state of ionic liquids. The iPOP-ZnTPy@GNFs exhibited a larger surface area and more exposed active sites, which intensified the catalytic activity in the CO2 cycloaddition reaction with propylene oxide with almost double the reaction rate as compared to that of iPOP-ZnTPy-2 at 100 °C and S/C = 1000. As expected, the iPOP-ZnTPy@GNF catalyst efficiently converted epoxides to cyclic carbonates at room temperature or atmospheric pressure, which can significantly reduce the process cost. In addition, iPOP-ZnTPy@GNFs exhibited excellent broad substrate scope, catalytic diversity, and remarkable reusability. The reaction mechanism of CO2 cycloaddition was studied via density functional theory calculations and was validated by experimental findings. This work provides a feasible method for improving the utilization of active sites in PILs as a highly robust catalyst for CO2 cycloaddition and can be further extended to other types of catalytic reactions in practical applications.

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Nano Today · 2022 · IF 18.962

Reverse intratumor bacteria-induced gemcitabine resistance with carbon nanozymes for enhanced tumor catalytic-chemo therapy

Juqun Xi,Yanqiu Wang,Xuejiao Gao,Yaling Huang,Jie Chen,Yong Chen,Lei Fan,Lizeng Gao

Emerging evidence demonstrates that intratumor bacteria promote tumor resistance to gemcitabine chemotherapy. The underlying mechanism is relate to intratumor bacteria expressing a specific cytidine deaminase (CDD) which metabolizes gemcitabine into its inactive form. Therefore, to overcome tumor resistance to gemcitabine, the CDD activity of intratumor bacteria must be restricted during chemotherapy. Herein, we developed an antitumor strategy by utilizing the dual functions of nitrogen-doped carbon nanospheres (N-CSs), i.e., as nanoinhibitors of CDD to overcome bacteria-mediated gemcitabine resistance and as nanozymes to integrate tumor catalytic therapy with chemotherapy. We found that the nitrogen-doped graphitized structure of the N-CSs could competitively bind to the active center of CDD and thus prevented gemcitabine metabolism. In addition, nitrogen doping endowed the N-CSs with peroxidase-like activity that generates •OH radicals for tumor catalytic therapy. Furthermore, in mouse cancer models with intratumor bacteria, the N-CSs successfully reversed bacterial CDD-induced gemcitabine resistance and restored tumor susceptibility to gemcitabine. The synergistic effects of catalytic therapy and chemotherapy for tumor treatment were achieved by using single N-CSs with dual nanozymatic and nanoinhibitory functions. This work provides a promising approach to overcome tumor drug-resistance induced by intratumor bacteria and synergize gemcitabine chemotherapy with nanozyme-mediated catalytic therapy for tumor treatment.

CAS / MDL: 70-18-8 9002-96-4
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DRUG DELIVERY · 2022 · IF 6.819

Orally administered intelligent self-ablating nanoparticles: a new approach to improve drug cellular uptake and intestinal absorption

Yanzi Liang,Ruihuan Ding,Huihui Wang,Lanze Liu,Jibiao He,Yuping Tao,Zhenyu Zhao,Jie Zhang,Aiping Wang,Kaoxiang Sun,Youxin Li,Yanan Shi

Oral drug delivery to treat diabetes is being increasingly researched. The mucus and the epithelial cell layers hinder drug delivery. We designed a self-ablating nanoparticle to achieve smart oral delivery to overcome the gastrointestinal barrier. We used the zwitterionic dilauroyl phosphatidylcholine, which exhibits a high affinity toward Oligopeptide transporter 1, to modify poly(lactic-co-glycolic acid) nanoparticles and load hemagglutinin-2 peptide to facilitate its escape from lysosomes. Nanoparticles exhibit a core–shell structure, the lipid layer is degraded by the lysosomes when the nanoparticles are captured by lysosomes, then the inner core of the nanoparticles gets exposed. The results revealed that the self-ablating nanoparticles exhibited higher encapsulation ability than the self-assembled nanoparticles (77% vs 64%) and with better stability. Quantitative cellular uptake, cellular uptake mechanisms, and trans-monolayer cellular were studied, and the results revealed that the cellular uptake achieved using the self-ablating nanoparticles was higher than self-assembling nanoparticles, and the number of uptake pathways via which the self-ablating nanoparticles functioned were higher than the self-assembling nanoparticles. Intestinal mucus permeation, in vivo intestinal circulation, was studied, and the results revealed that the small self-assembling nanoparticles exhibit a good extent of intestinal uptake in the presence of mucus. In vitro flip-flop, intestinal circulation revealed that the uptake of the self-ablating nanoparticles was 1.20 times higher than the self-assembled nanoparticles. Pharmacokinetic study and the pharmacodynamic study showed that the bioavailability and hypoglycemic effect of self-ablating nanoparticles were better than self-assembled nanoparticles.

CAS / MDL: 18194-25-7 127641-86-5
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APPLIED ORGANOMETALLIC CHEMISTRY · 2022 ·Vol. 36 ·期 4 ·e6587 · IF 4.072

Synthesis, characterization, superoxide dismutase, and antimicrobial activities of Co (II) complexes with Schiff base ligand and their hybrid proteins

Dan Mo,Xun Song,Jiri Wu,Yogini Jaiswal,Yifu Guan,Yuzhen Zhang,Yunjun Shen,Hedong Bian

Metal complexes have been reported to possess excellent free radical scavenging and antimicrobial properties. In the present study, seven linear trinuclear complexes were synthesized based on bis Schiff base ligand and complexes 1 , 3 – 7 are reported for the first time. Their structure was characterized by IR spectroscopy and single crystal diffraction. BSA was used as carrier to hybridize the synthesized complexes to construct hybrid proteins. The interaction between metal complex and BSA was studied by UV–Vis spectrophotometry and fluorescence spectroscopy. Static quenching was the main mechanism identified for the interaction between metal complex and BSA. In the superoxide dismutase (SOD) activity test, IC 50 values of complexes and hybrid proteins range between 2.89 and 26.53 μM, with hybrid proteins demonstrating a stronger activity than the complexes. Among all the complexes studied, complex 5 exhibited the strongest inhibition against Candida albicans (MIC 12.5 μg ml −1 ) and Cryptococcus neoformans (MIC 6.5 μg ml −1 ).

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