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1.
J Am Chem Soc ; 146(15): 10217-10233, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38563421

RESUMO

Although immunotherapy is relatively effective in treating hematological malignancies, their efficacy against solid tumors is still suboptimal or even noneffective presently. Compared to hematological cancers, solid tumors exhibit strikingly different immunosuppressive microenvironment, severely deteriorating the efficacy of immunotherapy: (1) chemical features such as hypoxia and mild acidity suppress the activity of immune cells, (2) the pro-tumorigenic domestication of immune cells in the microenvironment within the solid tumors further undermines the effectiveness of immunotherapy, and (3) the dense physical barrier of solid tumor tissues prevents the effective intratumoral infiltration and contact killing of active immune cells. Therefore, we believe that reversing the immunosuppressive microenvironment are of critical priority for the immunotherapy against solid tumors. Due to their unique morphologies, structures, and compositions, nanomedicines have become powerful tools for achieving this goal. In this Perspective, we will first briefly introduce the immunosuppressive microenvironment of solid tumors and then summarize the most recent progresses in nanomedicine-based immunotherapy for solid tumors by remodeling tumor immune-microenvironment in a comprehensive manner. It is highly expected that this Perspective will aid in advancing immunotherapy against solid tumors, and we are highly optimistic on the future development in this burgeoning field.


Assuntos
Nanomedicina , Neoplasias , Humanos , Microambiente Tumoral , Neoplasias/terapia , Imunoterapia , Carcinogênese , Imunossupressores/farmacologia
2.
J Am Chem Soc ; 146(25): 17201-17210, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38874405

RESUMO

As one of the most lethal cardiovascular diseases, aortic dissection (AD) is initiated by overexpression of reactive oxygen species (ROS) in the aorta that damages the vascular structure and finally leads to massive hemorrhage and sudden death. Current drugs used in clinics for AD treatment fail to efficiently scavenge ROS to a large extent, presenting undesirable therapeutic effect. In this work, a nanocatalytic antioxidation concept has been proposed to elevate the therapeutic efficacy of AD by constructing a cobalt nanocatalyst with a biomimetic structure that can scavenge pathological ROS in an efficient and sustainable manner. Theoretical calculations demonstrate that the antioxidation reaction is catalyzed by the redox transition between hydroxocobalt(III) and oxo-hydroxocobalt(V) accompanied by inner-sphere proton-coupled two-electron transfer, forming a nonassociated activation catalytic cycle. The efficient antioxidation action of the biomimetic nanocatalyst in the AD region effectively alleviates oxidative stress, which further modulates the aortic inflammatory microenvironment by promoting phenotype transition of macrophages. Consequently, vascular smooth muscle cells are also protected from inflammation in the meantime, suppressing AD progression. This study provides a nanocatalytic antioxidation approach for the efficient treatment of AD and other cardiovascular diseases.


Assuntos
Antioxidantes , Dissecção Aórtica , Cobalto , Catálise , Cobalto/química , Cobalto/farmacologia , Dissecção Aórtica/tratamento farmacológico , Dissecção Aórtica/patologia , Antioxidantes/química , Antioxidantes/farmacologia , Animais , Materiais Biomiméticos/química , Materiais Biomiméticos/farmacologia , Materiais Biomiméticos/síntese química , Camundongos , Espécies Reativas de Oxigênio/metabolismo , Humanos , Estresse Oxidativo/efeitos dos fármacos , Nanopartículas Metálicas/química
3.
J Am Chem Soc ; 146(5): 3186-3199, 2024 02 07.
Artigo em Inglês | MEDLINE | ID: mdl-38266487

RESUMO

Atopic dermatitis (AD) is a prevalent chronic inflammatory skin disease that carries a significant global economic burden. Elevated levels of reactive oxygen species (ROS) have been recognized as contributing to AD exacerbation, making them a potential therapeutic target for AD treatment. Here, we introduce a dual-site biomimetic copper/zinc metal-organic framework (Cu/Zn-MOF) featuring four types of enzyme-like activities for AD treatment via suppressing the Fcγ receptor (FcγR)-mediated phagocytosis signal by mimicking the bimetallic sites of natural copper-zinc superoxide dismutase (CuZn-SOD). Interestingly, the neighboring Cu and Zn sites in both Cu/Zn-MOF and CuZn-SOD are at similar distances of ∼5.98 and ∼6.3 Šfrom each other, respectively, and additionally, both Cu and Zn sites are coordinated to nitrogen atoms in both structures, and the coordinating ligands to Cu and Zn are both imidazole rings. Cu/Zn-MOF exhibits remarkable SOD-like activity as well as its glutathione peroxidase (GPx)-, thiol peroxidase (TPx)-, and ascorbate peroxidase (APx)-like activities to continuously consume ROS and mitigate oxidative stress in keratinocytes. Animal experiments show that Cu/Zn-MOF outperforms halcinonide solution (a potent steroid medication) in terms of preventing mechanical injuries, reducing cutaneous water loss, and inhibiting inflammatory responses while presenting favorable biosafety. Mechanistically, Cu/Zn-MOF functions through an FcγR-mediated phagocytosis signal pathway, decreasing the continuous accumulation of ROS in AD and ultimately suppressing disease progression. These findings will provide an effective paradigm for AD therapy and contribute to the development of two-site bionics (TSB).


Assuntos
Dermatite Atópica , Estruturas Metalorgânicas , Humanos , Animais , Superóxido Dismutase/metabolismo , Cobre , Receptores de IgG , Zinco/metabolismo , Espécies Reativas de Oxigênio/metabolismo , Biomimética , Glutationa Peroxidase/metabolismo
4.
Chem Soc Rev ; 52(3): 973-1000, 2023 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-36597879

RESUMO

Lactate in tumors has long been considered "metabolic junk" derived from the glycolysis of cancer cells and utilized only as a biomarker of malignancy, but is presently believed to be a pivotal regulator of tumor development, maintenance and metastasis. Indeed, tumor lactate can be a "fuel" for energy supply and functions as a signaling molecule, which actively contributes to tumor progression, angiogenesis, immunosuppression, therapeutic resistance, etc., thus providing promising opportunities for cancer treatment. However, the current approaches for regulating lactate homeostasis with available agents are still challenging, which is mainly due to the short half-life, low bioavailability and poor specificity of these agents and their unsatisfactory therapeutic outcomes. In recent years, lactate modulation nanomedicines have emerged as a charming and efficient strategy for fighting cancer, which play important roles in optimizing the delivery of lactate-modulating agents for more precise and effective modulation and treatment. Integrating specific lactate-modulating functions in diverse therapeutic nanomedicines may overcome the intrinsic restrictions of different therapeutic modalities by remodeling the pathological microenvironment for achieving enhanced cancer therapy. In this review, the most recent advances in the engineering of functional nanomedicines that can modulate tumor lactate for cancer therapy are summarized and discussed, and the fundamental mechanisms by which lactate modulation benefits various therapeutics are elucidated. Finally, the challenges and perspectives of this emerging strategy in the anti-tumor field are highlighted.


Assuntos
Antineoplásicos , Neoplasias , Humanos , Antineoplásicos/farmacologia , Antineoplásicos/uso terapêutico , Ácido Láctico/uso terapêutico , Nanomedicina , Neoplasias/tratamento farmacológico , Neoplasias/patologia , Portadores de Fármacos/uso terapêutico , Microambiente Tumoral
5.
Nano Lett ; 23(17): 8355-8362, 2023 09 13.
Artigo em Inglês | MEDLINE | ID: mdl-37656434

RESUMO

Oxidative stress and hypoxia are two key biochemical factors in the development of rheumatoid arthritis (RA). As both reactive oxygen species (ROS) and oxygen gas (O2) are oxygen-related chemicals, we suggest that a redox reaction converting ROS into O2 can mitigate oxidative stress and hypoxia concurrently, synergistically modulating the inflammatory microenvironment. In this work, ferrihydrite, a typical iron oxyhydroxide, is prepared in nanodimensions in which tetrahedrally coordinated Fe can form a composite catalytic center by coupling with an adjacent hydroxyl group, cooperatively facilitating H2O2 decomposition and O2 generation, presenting a high catalase-like activity. In the RA region, the nanomaterial catalyzes the conversion of excess H2O2 into O2, achieving both antioxidation and oxygenation favoring the alleviation of inflammation. Both cellular and in vivo experiments demonstrate the desirable efficacy of ferrihydrite nanoparticles for RA treatment. This work provides a methodology for the catalytic therapy of inflammatory diseases featuring both oxidative stress and hypoxia.


Assuntos
Artrite Reumatoide , Nanopartículas , Humanos , Antioxidantes/farmacologia , Antioxidantes/uso terapêutico , Espécies Reativas de Oxigênio , Peróxido de Hidrogênio , Artrite Reumatoide/tratamento farmacológico , Nanopartículas/uso terapêutico , Oxigênio , Hipóxia
6.
Nano Lett ; 23(10): 4683-4692, 2023 05 24.
Artigo em Inglês | MEDLINE | ID: mdl-36912868

RESUMO

The oral delivery of probiotics is commonly adopted for intestinal disease treatments in clinical settings; however, the probiotics suffer from a strong acidic attack in the gastric area and the low-efficiency intestinal colonization of naked probiotics. Coating living probiotics with synthetic materials has proven effective in enabling the adaption of bacteria to gastrointestinal environments, which, unfortunately, may shield the probiotics from initiating therapeutic responses. In this study, we report a copolymer-modified two-dimensional H-silicene nanomaterial (termed SiH@TPGS-PEI) that can facilitate probiotics to adapt to diverse gastrointestinal microenvironments on-demand. Briefly, SiH@TPGS-PEI electrostatically coated on the surface of probiotic bacteria helps to resist erosive destruction in the acidic stomach and spontaneously degrades by reacting with water to generate hydrogen, an anti-inflammatory gas in response to the neutral/weakly alkaline intestinal environment, thus exposing the probiotic bacteria for colitis amelioration. This strategy may shed new light on the development of intelligent self-adaptive materials.


Assuntos
Colite , Probióticos , Humanos , Intestinos , Bactérias , Probióticos/metabolismo , Probióticos/uso terapêutico
7.
Angew Chem Int Ed Engl ; 63(7): e202318585, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38108649

RESUMO

We report herein an electrocatalytic CO2 reduction-coupled sulfion oxidation system for the co-productions of valuable formate and sulfur at much enhanced atom utilization. Specifically, an organic ligand-assisted two-step reconstruction approach has been developed to fabricate the highly dispersed p-Bi nanosheets (p-Bi NSs) for cathodic CO2 reduction reaction (CO2 RR), and meanwhile porous Co-S nanosheets (Co-S NSs) was applied for anodic sulfion oxidation reaction (SOR). Significantly high Faradaic Efficiencies of about 90 % for formate production by CO2 RR in a wide potential range from -0.6 V to -1.1 V, and excellent SOR performances including an ultra-low onset potential of about 0.2 V and recycle capacity of S2- in the 0.1 M and 0.5 M S2- solutions, have been simultaneously achieved. In the meantime, both the structure transformation of the catalysts and the reaction pathways are explored and discussed in detail. A two-electrode CO2 RR||SOR electrolyzer equipped with above electrocatalysts has been established, which features as low as about 1.5 V to run the electrolyzer at 100 mA cm-2 , manifesting extremely lowered electricity consumption in comparison to conventional CO2 RR system. Moreover, a sulfur separation approach has been proposed by using CO2 , which is efficient, environmentally friendly and cost effective with value-added NaHCO3 be obtained as the byproduct.

8.
Angew Chem Int Ed Engl ; 63(13): e202316606, 2024 03 22.
Artigo em Inglês | MEDLINE | ID: mdl-38212843

RESUMO

Immunotherapy has brought a new dawn for human being to defeat cancer. Although existing immunotherapy regimens (CAR-T, etc.) have made breakthroughs in the treatments of hematological cancer and few solid tumors such as melanoma, the therapeutic efficacy on most solid tumors is still far from being satisfactory. In recent years, the researches on tumor immunotherapy based on nanocatalytic materials are under rapid development, and significant progresses have been made. Nanocatalytic medicine has been demonstrated to be capable of overcoming the limitations of current clinicnal treatments by using toxic chemodrugs, and exhibits highly attractive advantages over traditional therapies, such as the enhanced and sustained therapeutic efficacy based on the durable catalytic activity, remarkably reduced harmful side-effects without using traditional toxic chemodrugs, and so on. Most recently, nanocatalytic medicine has been introduced in the immune-regulation for disease treatments, especially, in the immunoactivation for tumor therapies. This article presents the most recent progresses in immune-response activations by nanocatalytic medicine-initiated chemical reactions for tumor immunotherapy, and elucidates the mechanism of nanocatalytic medicines in regulating anti-tumor immunity. By reviewing the current research progress in the emerging field, this review will further highlight the great potential and broad prospects of nanocatalysis-based anti-tumor immune-therapeutics.


Assuntos
Hipertermia Induzida , Melanoma , Neoplasias , Humanos , Neoplasias/tratamento farmacológico , Imunoterapia , Fototerapia
9.
Angew Chem Int Ed Engl ; : e202409419, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38975974

RESUMO

The local acidity at the anode surface during electrolysis is apparently stronger than that in bulk electrolyte due to the deprotonation from the reactant, which leads to the deteriorated electrocatalytic performances and product distributions. Here, an anode-electrolyte interfacial acidity regulation strategy has been proposed to inhibit local acidification at the surface of anode and enhance the electrocatalytic activity and selectivity of anodic reactions. As a proof of the concept, CeO2-x Lewis acid component has been employed as a supporter to load Au nanoparticles to accelerate the diffusion and enrichment of OH- toward the anode surface, so as to accelerate the electrocatalytic alcohol oxidation reaction. As the result, Au/CeO2-x exhibits much enhanced lactic acid selectivity of 81% and electrochemical activity of 693 mA·cm-2 current density in glycerol oxidation reaction compared to pure Au. Mechanism investigation reveals that the introduced Lewis acid promotes the mass transport and concentration of OH- on the anode surface, thus promoting the generation of lactic acid through the simultaneous enhancements of Faradaic and non-Faradaic processes. Attractively, the proposed strategy can be used for the electro-oxidation performance enhancements of a variety of alcohols, which thereby provides a new perspective for efficient alcohol electro-oxidations and the corresponding electrocatalyst design.

10.
Angew Chem Int Ed Engl ; : e202411502, 2024 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-39072890

RESUMO

Plastic pollution, an increasingly serious global problem, can be addressed through the full lifecycle management of plastics, including plastics recycling as one of the most promising approaches. System design, catalyst development, and product separation are the keys in improving the economics of electrocatalytic plastics recycling. Here, a membrane-free co-production system was devised to produce succinic acid (SA) at both anode and cathode respectively by the co-electrolysis of polybutylene succinate (PBS) waste plastics and biomass-derived maleic acid (MA) for the first time. To this end, Cr3+-Ni(OH)2 electrocatalyst featuring much enhanced 1,4-butanediol (BDO) oxidation reaction (BOR) activity has been synthesized and the role of doped Cr has been revealed as an "electron puller" to accelerate the rate-determining step (RDS) in the Ni2+/Ni3+ cycling. Impressively, an extra-high SA production rate of 3.02 g h-1 and ultra-high apparent Faraday efficiency towards SA (FEapparent=181.5%) have been obtained. A carbon dioxide-assisted sequential precipitation approach has been developed to produce high-purity SA and byproduct NaHCO3 solids. Preliminary techno-economic analysis demonstrates that the reported system is economically profitable and promising for future industrial applications.

11.
Angew Chem Int Ed Engl ; 63(11): e202400206, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38253953

RESUMO

During the electrocatalytic NO3 - reduction reaction (NO3 - RR) under neutral condition, the activation of H2 O to generate H* and the inhibition of inter-H* species binding, are critically important but remain challenging for suppressing the non-desirable hydrogen evolution reaction (HER). Here, a Mn-doped Co(OH)2 (named as Mn-Co(OH)2 ) has been synthesized by in situ reconstruction in the electrolyte, which is able to dissociate H2 O molecules but inhibits the binding of H* species between each other owing to the increased interatomic spacing by the Mn-doping. The Mn-Co(OH)2 electrocatalyst offers a faradaic efficiency (FE) of as high as 98.9±1.7% at -0.6 V vs. the reversible hydrogen electrode (RHE) and an energy efficiency (EE) of 49.90±1.03% for NH3 production by NO3 - RR, which are among the highest of the recently reported state-of-the-art catalysts in neutral electrolyte. Moreover, negligible degradation at -200 mA cm-2 has been found for at least 500 h, which is the longest catalytic durations ever reported. This work paves a novel approach for the design and synthesis of efficient NO3 - RR electrocatalysts.

12.
Angew Chem Int Ed Engl ; 63(6): e202316858, 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38095801

RESUMO

Nanocatalytic tumor therapy based on Fenton nanocatalysts has attracted considerable attention because of its therapeutic specificity, enhanced outcomes, and high biocompatibility. Nevertheless, the rate-determining step in Fenton chemistry, which involves the transition of a high-valence metallic center (FeIII ) to a Fenton-active low-valence metallic center (FeII ), has hindered advances in nanocatalyst-based therapeutics. In this study, we constructed mesoporous single iron atomic nanocatalysts (mSAFe NCs) by employing catechols from dopamine to coordinate and isolate single iron atoms. The catechols also serve as reductive ligands, generating a field-effect-based cocatalytic system that instantly reduces FeIII species to FeII species within the mSAFe NCs. This self-motivated cocatalytic strategy enabled by mSAFe NCs accelerates the kinetics of the Fenton catalytic reaction, resulting in remarkable performance for nanocatalytic tumor therapy both in vitro and in vivo.


Assuntos
Compostos Férricos , Neoplasias , Humanos , Ferro , Neoplasias/tratamento farmacológico , Compostos Ferrosos , Catecóis , Peróxido de Hidrogênio , Catálise
13.
J Am Chem Soc ; 145(10): 5803-5815, 2023 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-36848658

RESUMO

The antioxidant system, signed with reduced glutathione (GSH) overexpression, is the key weapon for tumor to resist the attack by reactive oxygen species (ROS). Counteracting the ROS depletion by GSH is an effective strategy to guarantee the antitumor efficacy of nanocatalytic therapy. However, simply reducing the concentration of GSH does not sufficiently improve tumor response to nanocatalytic therapy intervention. Herein, a well-dispersed MnOOH nanocatalyst is developed to catalyze GSH autoxidation and peroxidase-like reaction concurrently and respectively to promote GSH depletion and H2O2 decomposition to produce abundant ROS such as hydroxyl radical (·OH), thereby generating a highly effective superadditive catalytic therapeutic efficacy. Such a therapeutic strategy that transforms endogenous "antioxidant" into "oxidant" may open a new avenue for the development of antitumor nanocatalytic medicine. Moreover, the released Mn2+ can activate and sensitize the cGAS-STING pathway to the damaged intratumoral DNA double-strands induced by the produced ROS to further promote macrophage maturation and M1-polarization, which will boost the innate immunotherapeutic efficacy. Resultantly, the developed simple MnOOH nanocatalytic medicine capable of simultaneously catalyzing GSH depletion and ROS generation, and mediating innate immune activation, holds great potential in the treatment of malignant tumors.


Assuntos
Peróxido de Hidrogênio , Neoplasias , Humanos , Espécies Reativas de Oxigênio/metabolismo , Peróxido de Hidrogênio/farmacologia , Glutationa/metabolismo , Antioxidantes , Neoplasias/tratamento farmacológico , Imunoterapia , Catálise , Linhagem Celular Tumoral
14.
J Am Chem Soc ; 145(24): 13147-13160, 2023 06 21.
Artigo em Inglês | MEDLINE | ID: mdl-37262421

RESUMO

The immunotherapy of deep solid tumors in the human body, such as liver cancer, still faces great challenges, especially the inactivation and insufficient infiltration of immune cells in solid tumor microenvironment. Natural killer (NK) cells are gaining ever-increasing attention owing to their unique features and are expected to play an important role in the liver cancer immunotherapy. However, NK cells are severely insufficient and inactivated in solid liver tumor due to the highly immunosuppressive intratumor microenvironment, resulting in poor clinical therapeutic efficacy. Herein, we propose a mild magnetocaloric regulation approach using a magnetogenetic nanoplatform MNPs@PEI-FA/pDNA (MPFD), which is synthesized by loading a heat-inducible plasmid DNA (HSP70-IL-2-EGFP) on polyethyleneimine (PEI)- and folic acid (FA)-modified ZnCoFe2O4@ZnMnFe2O4 magnetic nanoparticles (MNPs) to promote the proliferation and activation of tumor-infiltrating NK cells under magnetic manipulation without the limitation of penetration depth for orthotopic liver cancer immunotherapy. The magnetothermally responsive MPFD serves as a magnetism-heat nanotransducer to induce the gene transcription of IL-2 cytokine in orthotopic liver tumor for NK cell proliferation and activation. Both in vitro and in vivo results demonstrate that the remote mild magnetocaloric regulation (∼40 °C) by MPFD initiates the HSP70 promoter to trigger the overexpression of IL-2 cytokine for subsequent secretion, leading to in situ expansion and activation of tumor-infiltrating NK cells through the IL-2/IL-2 receptor (IL-2R) pathways and the resulting prominent tumor inhibition. This work not only evidences the great potential of magnetogenetic nanoplatform but also reveals the underlying proliferation and activation mechanism of NK cells in liver cancer treatment by magnetogenetic nanoplatform.


Assuntos
Neoplasias Hepáticas , Neoplasias , Humanos , Interleucina-2 , Imunoterapia , Neoplasias Hepáticas/terapia , Citocinas , Proliferação de Células , Fenômenos Magnéticos , Microambiente Tumoral
15.
J Am Chem Soc ; 145(44): 24153-24165, 2023 11 08.
Artigo em Inglês | MEDLINE | ID: mdl-37897426

RESUMO

Cancer stem cells (CSCs) within protumorigenic microlesions are a critical driver in the initiation and progression of early stage lung cancer, where immune cells provide an immunosuppressive niche to strengthen the CSC stemness. As the mutual interactions between CSCs and immune cells are increasingly recognized, regulating the immune cells to identify and effectively eliminate CSCs has recently become one of the most attractive therapeutic options, especially for abundant tumor-associated macrophages (TAMs). Herein, we developed a nebulized nanocatalytic medicine strategy in which iron-based nanoparticle-regulated TAMs effectively target CSC niches and trigger CSC ferroptosis in the early stage of lung cancer. Briefly, the iron-based nanoparticles can effectively accumulate in lung cancer microlesions (minimum 122 µm in diameter) through dextran-mediated TAM targeting by nebulization administration, and as a result, nanoparticle-internalized TAMs can play a predominant role of the iron factory in elevating the iron level surrounding CSC niches and destroying redox equilibrium through downregulating glucose-6-phosphate metabolite following their lysosomal degradation and iron metabolism. The altered microenvironment results in the enhanced sensitivity of CSCs to ferroptosis due to their high expression of the CD44 receptor mediating iron endocytosis. In an orthotopic mouse model of lung cancer, the initiation and progression of early lung cancer are significantly suppressed through ferroptosis-induced stemness reduction of CSCs by nebulization administration. This work presents a nebulized therapeutic strategy for early lung cancer through modulation of communications between TAMs and CSCs, which is expected to be a general approach for regulating primary microlesions and micrometastatic niches of lung cancer.


Assuntos
Ferroptose , Neoplasias Pulmonares , Camundongos , Animais , Neoplasias Pulmonares/patologia , Macrófagos/metabolismo , Células-Tronco Neoplásicas , Microambiente Tumoral
16.
J Am Chem Soc ; 145(24): 13249-13260, 2023 06 21.
Artigo em Inglês | MEDLINE | ID: mdl-37285166

RESUMO

Iodine, as a typical haloid element in group VIIA, has been extensively applied as antiseptics clinically, thanks to its effective and wide-spectrum antimicrobial activity against bacteria, fungi, and viruses. Nevertheless, current iodic sterilizing agents are still limited to topical applications such as instrument sterilization and treatments of skin or mucous membrane infection due to its unsatisfactory stability and biocompatibility. Here, we propose an emerging two-dimensional iodine nanomaterial (noted as iodinene) for the treatment of infection diseases in vivo. Iodinene nanosheets were fabricated by a facile and environmentally friendly approach via sonication-assisted liquid exfoliation, which present an intriguing layered structure and negligible toxicity. The as-synthesized iodinene would experience an in situ allotropic transformation spontaneously to release active HIO and I2 molecules by reacting with H2O2 in the infectious microenvironment. By the in situ production of active HIO and I2 molecules via allotropic transformation, iodinene presents enhanced antibacterial efficacy against Staphylococcus aureus, Escherichia coli, and Pseudomonas aeruginosa. In vivo outcome demonstrates the desirable antibacterial efficacy of iodinene in treating bacterial wound infection and pneumonia. This study thus offers an alternative to conventional sterilizing agents against hard-to-treat bacterial infections.


Assuntos
Anti-Infecciosos Locais , Infecções Bacterianas , Iodo , Humanos , Iodo/farmacologia , Peróxido de Hidrogênio , Antibiose , Antibacterianos/farmacologia , Antibacterianos/uso terapêutico , Antibacterianos/química , Bactérias
17.
Small ; 19(42): e2303061, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37340882

RESUMO

Developing anode catalysts with substantially enhanced activity for hydrogen oxidation reaction (HOR) and CO tolerance performance is of great importance for the commercial applications of proton exchange membrane fuel cells (PEMFCs). Herein, an excellent CO-tolerant catalyst (Pd-WO3 /C) has been fabricated by loading Pd nanoparticles on WO3 via an immersion-reduction route. A remarkably high power density of 1.33 W cm-2 at 80 °C is obtained by using the optimized 3Pd-WO3 /C as the anode catalyst of PEMFCs, and the moderately reduced power density (73% remained) in CO/H2 mixed gas can quickly recover after removal of CO-contamination from hydrogen fuel, which is not possible by using Pt/C or Pd/C as anode catalyst. The prominent HOR activity of 3Pd-WO3 /C is attributed to the optimized interfacial electron interaction, in which the activated H* adsorbed on Pd species can be effectively transferred to WO3 species through hydrogen spillover effect and then oxidized through the H species insert/output effect during the formation of Hx WO3 in acid electrolyte. More importantly, a novel synergetic catalytic mechanism about excellent CO tolerance is proposed, in which Pd and WO3 respectively absorbs/activates CO and H2 O, thus achieving the CO electrooxidation and re-exposure of Pd active sites for CO-tolerant HOR.

18.
J Biomed Inform ; 143: 104391, 2023 07.
Artigo em Inglês | MEDLINE | ID: mdl-37196988

RESUMO

OBJECTIVE: This article summarizes our approach to extracting medication and corresponding attributes from clinical notes, which is the focus of track 1 of the 2022 National Natural Language Processing (NLP) Clinical Challenges(n2c2) shared task. METHODS: The dataset was prepared using Contextualized Medication Event Dataset (CMED), including 500 notes from 296 patients. Our system consisted of three components: medication named entity recognition (NER), event classification (EC), and context classification (CC). These three components were built using transformer models with slightly different architecture and input text engineering. A zero-shot learning solution for CC was also explored. RESULTS: Our best performance systems achieved micro-average F1 scores of 0.973, 0.911, and 0.909 for the NER, EC, and CC, respectively. CONCLUSION: In this study, we implemented a deep learning-based NLP system and demonstrated that our approach of (1) utilizing special tokens helps our model to distinguish multiple medications mentions in the same context; (2) aggregating multiple events of a single medication into multiple labels improves our model's performance.


Assuntos
Aprendizado Profundo , Humanos , Processamento de Linguagem Natural
19.
J Biomed Inform ; 142: 104343, 2023 06.
Artigo em Inglês | MEDLINE | ID: mdl-36935011

RESUMO

Clinical documentation in electronic health records contains crucial narratives and details about patients and their care. Natural language processing (NLP) can unlock the information conveyed in clinical notes and reports, and thus plays a critical role in real-world studies. The NLP Working Group at the Observational Health Data Sciences and Informatics (OHDSI) consortium was established to develop methods and tools to promote the use of textual data and NLP in real-world observational studies. In this paper, we describe a framework for representing and utilizing textual data in real-world evidence generation, including representations of information from clinical text in the Observational Medical Outcomes Partnership (OMOP) Common Data Model (CDM), the workflow and tools that were developed to extract, transform and load (ETL) data from clinical notes into tables in OMOP CDM, as well as current applications and specific use cases of the proposed OHDSI NLP solution at large consortia and individual institutions with English textual data. Challenges faced and lessons learned during the process are also discussed to provide valuable insights for researchers who are planning to implement NLP solutions in real-world studies.


Assuntos
Ciência de Dados , Informática Médica , Humanos , Registros Eletrônicos de Saúde , Processamento de Linguagem Natural , Narração
20.
J Nanobiotechnology ; 21(1): 319, 2023 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-37674191

RESUMO

Stimulating ion channels targeting in neuromodulation by external signals with the help of functionalized nanoparticles, which integrates the pioneering achievements in the fields of neurosciences and nanomaterials, has involved into a novel interdisciplinary field. The emerging technique developed in this field enable simple, remote, non-invasive, and spatiotemporally precise nerve regulations and disease therapeutics, beyond traditional treatment methods. In this paper, we define this emerging field as nano-neuromodulation and summarize the most recent developments of non-genetic nano-neuromodulation (non-genetic NNM) over the past decade based on the innovative design concepts of neuromodulation nanoparticle systems. These nanosystems, which feature diverse compositions, structures and synthesis approaches, could absorb certain exogenous stimuli like light, sound, electric or magnetic signals, and subsequently mediate mutual transformations between above signals, or chemical reactions, to regulate stimuli-sensitive ion channels and ion migrations which play vital roles in the nervous system. We will also discuss the obstacles and challenges in the future development of non-genetic NNM, and propose its future developments, to add the further progress of this promising field.


Assuntos
Nanopartículas , Nanoestruturas , Eletricidade
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