Near-Infrared-II-Activatable Self-Assembled Manganese Porphyrin-Gold Heterostructures for Photoacoustic Imaging-Guided Sonodynamic-Augmented Photothermal/Photodynamic Therapy

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 713 - 727

Published: Dec. 20, 2023

Porphyrins and their derivatives are widely used as photosensitizers sonosensitizers in tumor treatment. Nevertheless, poor water solubility low chemical stability reduce singlet oxygen (1O2) yield and, consequently, photodynamic therapy (PDT) sonodynamic (SDT) efficiency. Although strategies for porphyrin molecule assembly have been developed to augment 1O2 generation, there is scope further improving PDT SDT efficiencies. Herein, we synthesized ordered manganese (SM) nanoparticles with well-defined self-assembled metalloporphyrin networks that enabled efficient energy transfer enhanced photocatalytic sonocatalytic activity production. Subsequently, Au were grown situ on the SM surface by anchoring terminal alkynyl of form plasmonic SMA heterostructures, which showed excellent near-infrared-II (NIR-II) region absorption photothermal properties, facilitated electron–hole pair separation transfer. With modification hyaluronic acid (HA), SMAH heterostructure nanocomposites exhibited good actively targeted cancer cells. Under NIR-II light ultrasound (US) irradiation, generates hyperthermia, a large amount 1O2, inducing cell damage. Both vitro vivo studies confirmed effectively suppressed growth decreasing GSH levels SDT-augmented PDT/PTT. Moreover, utilizing strong window, can achieve photoacoustic imaging-guided combined This work provides paradigm enhancing metalloporphyrins improve synergistic therapeutic effect SDT/PDT/PTT.

Language: Английский

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Defect Engineering in Nanocatalysts: From Design and Synthesis to Applications

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: Feb. 13, 2024

Abstract Defect engineering is an emerging technology for tailoring nanomaterials' characteristics and catalytic performance in various applications. Recently, defect‐engineered nanoparticles have emerged as highly researched materials applications because of their exceptional redox reaction capabilities physicochemical optical properties. The properties nanomaterials can be readily adjusted by controlling the nature concentration defects within nanoparticles, avoiding need intricate design strategies. This review investigates defect nanocatalysts, including design, fabrication, Initially, categories strategies nanomaterial impacts on nanocatalysts' electronic surface properties, activity, selectivity, stability are summarized. Then, processes uses, gas sensing, hydrogen (H 2 ) evolutions, water splitting, reductions carbon dioxide (CO nitrogen to value‐aided products, pollutant degradation, biomedical (oncotherapy, antibacterial wound healing, biomolecular sensing) discussed. Finally, limitations prospective paths allowing logical optimization nanocatalytic long‐term efficient also examined. comprehensive gives unique insights into current state nanocatalysts inspires future research exploiting shortcomings improve customize performance.

Language: Английский

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Glutathione Induced In situ Synthesis of Cu Single‐Atom Nanozymes with Anaerobic Glycolysis Metabolism Interference for Boosting Cuproptosis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: Feb. 23, 2024

Abstract Single‐atom nanozyme (SAzyme) has sparked increasing interest for catalytic antitumor treatment due to their more tunable and diverse active sites than natural metalloenzymes in complex physiological conditions. However, it is usually a hard task precisely conduct catalysis at tumor after intravenous injection of those SAzyme with high reactivity. Moreover, the explorations SAzymes anticancer application are still its infancy need be developed. Herein, an situ synthesis strategy Cu was constructed convert adsorbed copper ions into isolated atoms anchored by oxygen (Cu−O 2 /Cu−O 4 ) via GSH‐responsive deformability supports. Our results suggest that activation process could further facilitate dissociation consumption glutathione, thereby leading deposition cytoplasm triggering cuproptosis. peroxidase‐like activity enabled intracellular reactive species production, resulting specifically disturbance metabolism pathway. Meanwhile, exposed glucose transporter (GLUT) inhibitor phloretin (Ph) can block glycose uptake boost cuproptosis efficacy. Overall, this effectively diminished off‐target effects SACs‐induced therapies introduced promising paradigm advancing cuproptosis‐associated therapies.

Language: Английский

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De Novo Designed Ru(II) Metallacycle as a Microenvironment‐Adaptive Sonosensitizer and Sonocatalyst for Multidrug‐Resistant Biofilms Eradication

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 8, 2024

Abstract Albeit sonodynamic therapy (SDT) has achieved encouraging progress in microbial sterilization, the scarcity of guidelines for designing highly effective sonosensitizers and intricate biofilm microenvironment (BME), substantially hamper therapeutic efficacy against infections. To address bottlenecks, we innovatively design a Ru(II) metallacycle‐based sonosensitizer/sonocatalyst (named Ru‐A3‐TTD ) to enhance potency sonotherapy by employing molecular engineering strategies tailored BME. Our approach involves augmenting ’s production ultrasonic‐triggered reactive oxygen species (ROS), surpassing performance commercial sonosensitizers, through straightforward but potent π‐expansion approach. Within BME, synergistically amplifies sonotherapeutic via triple‐modulated approaches: (i) alleviation hypoxia, leading increased ROS generation, (ii) disruption antioxidant defense system, which shields from glutathione consumption, (iii) enhanced penetration, enabling deep sites. Notably, sono‐catalytically oxidizes NADPH, critical coenzyme involved defenses. Consequently, demonstrates superior eradication multidrug‐resistant Escherichia coli compared conventional clinical antibiotics, both vitro vivo. our knowledge, this study represents pioneering instance supramolecular sonosensitizer/sonocatalyst. It provides valuable insights into structure‐activity relationship paves promising pathway treatment

Language: Английский

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A Distinctive Insight into Inorganic Sonosensitizers: Design Principles and Application Domains

Small, Journal Year: 2024, Volume and Issue: 20(25)

Published: Jan. 15, 2024

Abstract Sonodynamic therapy (SDT) as a promising non‐invasive anti‐tumor means features the preferable penetration depth, which nevertheless, usually can't work without sonosensitizers. Sonosensitizers produce reactive oxygen species (ROS) in presence of ultrasound to directly kill tumor cells, and concurrently activate immunity especially after integration with microenvironment (TME)‐engineered nanobiotechnologies combined therapy. Current sonosensitizers are classified into organic inorganic ones, current most reviews only cover highlighted their applications. However, there have few specific that focus on including design principles, regulation, etc. In this review, first according rationales rather than composition, action underlying chemistry highlighted. Afterward, what how TME is regulated based sonosensitizers‐based SDT nanoplatform an emphasis targets‐engineered elucidated. Additionally, applications non‐cancer diseases also outlined. Finally, setbacks challenges, proposed potential solutions future directions pointed out. This review provides comprehensive detailed horizon sonosensitizers, will arouse more attentions SDT.

Language: Английский

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Near‐Infrared Light‐Triggered MXene Nanocomposite for Tumor‐Specific Mild Photothermal‐Enhanced Chemodynamic Therapy

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 20, 2024

Abstract Mild photothermal therapy (PTT) is an emerging and elegant approach with minimal adverse effects, demonstrating itself as effective treatment for cancer. However, potential challenges may arise from the overexpression of heat shock protein 90 (HSP90) reliance on monotherapy. Here, a near‐infrared (NIR) light‐triggered MXene nanocomposite (FA@MXene/CuO 2 /GA) developed to synergistically combine mild PTT chemodynamic (CDT) remarkably tumor eradication without any notable tissue damage. Under irradiation NIR light, effectively enhances by suppressing HSP90 expression through release gambogic acid (GA) due excellent performance Ti 3 C nanosheets well tumor‐targeting ability biocompatibility surface‐modified FA‐PEG‐SH. The copper‐based catalyst CuO in this system releases Cu 2+ acid‐triggered manner within microenvironment, activating Fenton‐like reaction generate hydroxyl radicals, simultaneous production H O serves alleviate deficiency endogenous tumor. Overall, current work showcases remarkable synergistic anticancer effect CDT, also proposes new avenues research utilizing nanomaterials treatment.

Language: Английский

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An Enzyme‐Engineered Coppery Nanozyme for High‐Efficiency Mild Photothermal/Chemodynamic/Starvation Therapy Through Self‐Reinforcing Cancer Energy Metabolism Regulation

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(22)

Published: Feb. 5, 2024

Abstract Photothermal therapy (PTT) has a great prospect in further improving tumor therapeutic outcomes, whereas its efficiency is restrained by low light penetration, excessive heat damage to normal tissues, up‐regulated shock proteins (HSPs), and limited effect of single treatment. Herein, an enzyme‐engineered coppery nanozyme based on dendritic mesoporous carbon nanosphere as the cornerstone load with glucose oxidase (GOx) followed modification hyaluronic acid constructed. Density functional theory calculations indicate that obtained exhibits peroxidase glutathione mimicking activities improve hydroxyl radicals (•OH) production. Furthermore, both generation •OH production GOx‐induced energy supply blockade can reduce HSPs expression enhance mild PTT (η = 34.9 %) upon irradiation 1064 nm laser, turn, accelerate catalytic processes for more •OH. Last but not least, introduction copper induce lipoylated protein dihydrolipoamide S‐acetyltransferase aggregation cause cellular cuproptosis. Due synergy multiple therapies, inhibition rate reach 93.4%. Overall, this work provides effective strategy potential treatment basis synergistic therapies.

Language: Английский

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Rodlike nanomaterials from organic diradicaloid with high photothermal conversion capability for tumor treatment

Aggregate, Journal Year: 2023, Volume and Issue: 4(5)

Published: May 25, 2023

Abstract Organic diradicaloids with unique open‐shell structures and properties have been widely used in organic electronics spintronics. However, their advantageous optical explored less the biomedical field. In this work, photothermal conversion behaviors of a boron‐containing diradicaloid (BOD) are reported. BOD can assemble 1,2‐distearoyl‐sn‐glycero‐3‐phosphoethanolamine‐poly(ethylene glycol) to form rodlike nanoparticles (BOD NPs). These as‐prepared NPs exhibit high capability robust stability. Notably, they possess morphological superiority, which guarantees effective therapy tumors. This work thus demonstrates promise as efficient agents for applications.

Language: Английский

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Tensile Strain‐Mediated Bimetallene Nanozyme for Enhanced Photothermal Tumor Catalytic Therapy

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)

Published: April 9, 2024

Abstract Nanozymes have demonstrated significant potential in combating malignant tumor proliferation through catalytic therapy. However, the therapeutic effect is often limited by insufficient performance. In this study, we propose utilization of strain engineering metallenes to fully expose active regions due their ultrathin nature. Here, present first report on a novel tensile strain‐mediated local amorphous RhRu (la‐RhRu) bimetallene with exceptional intrinsic photothermal and photo‐enhanced multiple enzyme‐like activities. Through geometric phase analysis, electron diffraction profile, X‐ray diffraction, it revealed that crystalline‐amorphous heterophase boundaries can generate approximately 2 % bimetallene. The structure in‐plane induce an amplified effect. Both experimental theoretical evidence support notion promotes Functioning as microenvironment (TME)‐responsive nanozyme, la‐RhRu exhibits remarkable efficacy both vitro vivo. This work highlights tremendous atomic‐scale strategy enhancing

Language: Английский

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Sulfur-Vacancy-Engineered Two-Dimensional Cu@SnS_2–x Nanosheets Constructed via Heterovalent Substitution for High-Efficiency Piezocatalytic Tumor Therapy

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(31), P. 21496 - 21508

Published: July 29, 2024

Ultrasound (US)-mediated piezocatalytic tumor therapy has attracted much attention due to its notable tissue-penetration capabilities, noninvasiveness, and low oxygen dependency. Nevertheless, the efficiency of is limited an inadequate piezoelectric response, separation electron–hole (e––h+) pairs, complex microenvironment (TME). Herein, ultrathin two-dimensional (2D) sulfur-vacancy-engineered (Sv-engineered) Cu@SnS2–x nanosheet (NS) with enhanced effect was constructed via heterovalent substitution strategy Sn4+ by Cu2+. The introduction Cu2+ ion not only causes changes in crystal structure increase polarization but also generates rich Sv decrease band gap from 2.16 1.62 eV inhibit e––h+ pairs recombination, collectively leading highly efficient generation reactive species under US irradiation. Moreover, shows US-enhanced TME-responsive Fenton-like catalytic activity glutathione depletion ability, further aggravating oxidative stress. Both vitro vivo results prove that Sv-engineered NSs can significantly kill cells achieve high-efficiency a biocompatible manner. Overall, this study provides new avenue for sonocatalytic broadens application 2D materials.

Language: Английский

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