Catalyzing Generation and Stabilization of Oxygen Vacancies on CeO_2−x Nanorods by Pt Nanoclusters as Nanozymes for Catalytic Therapy

Advanced Healthcare Materials, Journal Year: 2023, Volume and Issue: 12(31)

Published: Sept. 14, 2023

Abstract Although CeO 2 nanomaterials have been widely explored as nanozymes for catalytic therapy, they still suffer from relatively low activities. Herein, the catalyzing generation and stabilization of oxygen vacancies on nanorods by Pt nanoclusters via H gas reduction under mild temperature (350 °C) to obtain Pt/CeO 2− x , which can serve a highly efficient nanozyme cancer is reported. The deposited atomic layer deposition technique not only catalyst generate through hydrogen spillover effect, but also stabilize generated vacancies. Meanwhile, provide anchoring sites forming strong metal‐support interactions thus preventing their agglomerations. Importantly, reduced at 350 °C (Pt/CeO ‐350R) exhibits excellent enzyme‐mimicking activity reactive species (e.g., ·OH) compared other control samples, including temperatures, achieving performance tumor‐specific therapy efficiently eliminate cells in vitro ablate tumors vivo. ‐350R originates good activities vacancy‐rich nanoclusters.

Language: Английский

---

Atomic-level coordination structures meet graphitic carbon nitride (g-C3N4) for photocatalysis: Energy conversion and environmental remediation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 123683 - 123683

Published: Jan. 1, 2024

Language: Английский

---

Programmed Targeting Pyruvate Metabolism Therapy Amplified Single‐Atom Nanozyme‐Activated Pyroptosis for Immunotherapy

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(24)

Published: Feb. 7, 2024

Abstract Increasing cellular immunogenicity and reshaping the immune tumor microenvironment (TME) are crucial for antitumor immunotherapy. Herein, this work develops a novel single‐atom nanozyme pyroptosis initiator: UK5099 pyruvate oxidase (POx)‐co‐loaded Cu‐NS (Cu‐NS@UK@POx), that not only trigger through cascade biocatalysis to boost of cells, but also remodel immunosuppressive TME by targeting metabolism. By replacing N with weakly electronegative S, original spatial symmetry Cu‐N 4 electron distribution is changed enzyme‐catalyzed process effectively regulated. Compared spatially symmetric nanozymes (Cu‐N SA), S‐doped asymmetric (Cu‐NS SA) exhibit stronger activities, including peroxidase (POD), nicotinamide adenine dinucleotide (NADH) (NOx), L ‐cysteine (LCO), glutathione (GSHOx), which can cause enough reactive oxygen species (ROS) storms pyroptosis. Moreover, synergistic effect SA, UK5099, POx target metabolism, improves increases degree This study provides two‐pronged treatment strategy significantly activate immunotherapy effects via ROS storms, NADH/glutathione/ consumption, oxidation, lactic acid (LA)/ATP depletion, triggering regulating broad vision expanding

Language: Английский

---

Single-Atom Nanozymes: From Precisely Engineering to Extensive Applications

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(3), P. 347 - 357

Published: Feb. 3, 2024

ConspectusNanozymes are nanomaterials with intrinsic enzyme-like properties that can overcome the current limitations of natural enzymes, such as high preparation cost, instability, restricted application scenarios, etc. Since Fe3O4 nanoparticles (NPs) were shown to possess peroxidase (POD)-like activity in 2007, thousands reported mimic catalytic various types enzymes including catalase (CAT), haloperoxidase, superoxide dismutase (SOD), glucose oxidase, glutathione peroxidase, hydrolase, nuclease, nitroreductase, and others. Particularly, some nanozymes showed multienzyme-like activities regarding changes scenarios temperature, pH, Benefiting from their distinct physical-chemical characteristics properties, have been widely applied biomedical related fields vitro detections vivo therapeutic treatments. However, currently ambiguous structure–function correlations relatively inferior compared promote extensive efforts for modifications on development novel alternative nanozymes. The single-atom (SAzymes) present a unique way highly evolved enzyme active centers, because atomically dispersed sites, which leads atom utilization efficiency and, thus, potentially extraordinary activity. Also, abilities modify centers and/or tune interactions between metal supporting ligands provide precise engineer SAzymes at atomic levels. Given well-defined geometric electronic structures, thus serve exceptional templates deciphering relationships, is beneficial further improving performances.In this Account, we will review our recent other notable works developments effective mimics applications areas. We begin brief introduction why emergence SAzymes, artificial enzyme, tackles challenges facing. Next, focus systematic design, synthesis optimization especially impacts engineering environment an enzymologist perspective. For example, alternations first-shell ligand N P/S, SAzymes' CAT-like increased more than 4-fold. coordination numbers (x) Co–Nx(C) SAzyme significantly altered its oxidase (OXD)-like kinetics Then, discuss ways standardization specific kinetics. also wide ranges colorimetric biologicals, antibiosis treatments, cancer therapies. Finally, address future perspectives

Language: Английский

---

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

---

Bioorthogonal Cu Single‐atom Nanozyme for Synergistic Nanocatalytic Therapy, Photothermal Therapy, Cuproptosis, and Immunotherapy

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 24, 2024

Single-atom nanozymes (SAzymes) with atomically dispersed active sites are potential substitutes for natural enzymes. A systematic study of its multiple functions can in-depth understand SAzymes's nature, which remains elusive. Here, we develop a novel ultrafast synthesis sputtered SAzymes by in situ bombarding-embedding technique. Using this method, copper (Cu) (CuSA) is developed unreported unique planar Cu-C

Language: Английский

---

Microfluidic Synthesis of CuH Nanoparticles for Antitumor Therapy through Hydrogen-Enhanced Apoptosis and Cuproptosis

ACS Nano, Journal Year: 2024, Volume and Issue: 18(12), P. 9031 - 9042

Published: March 12, 2024

Cuproptosis has drawn enormous attention in antitumor material fields; however, the responsive activation of cuproptosis against tumors using nanomaterials with high atom utilization is still challenging. Herein, a copper-based nanoplatform consisting acid-degradable copper hydride (CuH) nanoparticles was developed via microfluidic synthesis. After coating tumor-targeting hyaluronic acid (HA), denoted as HA-CuH-PVP (HCP) shows conspicuous damage toward tumor cells by generating Cu+ and hydrogen (H2) simultaneously. can induce apoptosis relying on Fenton-like reactions lead to causing mitochondrial protein aggregation. Besides, existence H2 enhance both cell death types dysfunction intracellular redox homeostatic disorders. In vivo experimental results further exhibit desirable potential HCP for killing inhibiting lung metastases, which will broaden horizons designing materials triggering better efficacy.

Language: Английский

---

Electron Lock Manipulates the Catalytic Selectivity of Nanozyme

ACS Nano, Journal Year: 2024, Volume and Issue: 18(4), P. 3814 - 3825

Published: Jan. 17, 2024

Nanomaterials with enzyme-mimicking functions, termed nanozymes, offer attractive opportunities for biocatalysis and biomedicine. However, manipulating nanozyme selectivity poses an insurmountable hurdle. Here, we propose the concept of energy-governed electron lock that controls transfer between substrates to achieve manipulation enzyme-like catalysis. An can be constructed opened, via modulating nanozyme's energy match barrier enzymatic reactions. iron-doped carbon dot (FeCD) easy-to-regulate is selected as a proof concept. Through regulating conduction band which dominates energy, activatable oxidase selective peroxidase (POD) substrate affinity 123-fold higher than natural horseradish (HRP) achieved. Furthermore, while maintaining selectivity, FeCDs exhibit catalytic kinetics comparable HRP upon transforming photons into electrons. Superior efficient catalysis, undetectable biotoxicity energize potent targeted drugs on antibiotic-resistant bacterial abscesses. provides robust strategy manipulate toward advanced nanozymes.

Language: Английский

---

Perspectives for the Role of Single-Atom Nanozymes in Assisting Food Safety Inspection and Food Nutrition Evaluation

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(5), P. 1813 - 1824

Published: Jan. 25, 2024

Single-atom nanozymes (SAzymes) have been greatly developed for rapid detection, owing to their rich active sites and excellent catalytic activity. Although several reviews concentrating on SAzymes reported, they mainly focused advanced synthesis, sensing mechanisms, biomedical applications. To date, few elaborate the promising applications of in food safety inspection nutrition evaluation. In this paper, we systematically reviewed enzyme-like activity mechanism, addition recent research advances domain evaluation past years. Furthermore, current challenges hampering practical assay are summarized analyzed, possible areas focusing SAzyme-based sensors testing also proposed.

Language: Английский

---

NIR-II Light-Driven Genetically Engineered Exosome Nanocatalysts for Efficient Phototherapy against Glioblastoma

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15251 - 15263

Published: May 23, 2024

Glioblastoma (GBM) poses a significant therapeutic challenge due to its invasive nature and limited drug penetration through the blood–brain barrier (BBB). In response, here we present an innovative biomimetic approach involving development of genetically engineered exosome nanocatalysts (Mn@Bi2Se3@RGE-Exos) for efficient GBM therapy via improving BBB enzyme-like catalytic activities. Interestingly, photothermally activatable multiple reactivity is observed in such nanosystem. Upon NIR-II light irradiation, Mn@Bi2Se3@RGE-Exos are capable converting hydrogen peroxide into hydroxyl radicals, oxygen, superoxide providing peroxidase (POD), oxidase (OXD), catalase (CAT)-like nanocatalytic cascade. This consequently leads strong oxidative stresses damage cells. vitro, vivo, proteomic analysis further reveal potential disruption cellular homeostasis, enhancement immunological induction cancer cell ferroptosis, showcasing great promise anticancer efficacy against with favorable biosafety profile. Overall, success this study provides feasible strategy future design clinical stimuli-responsive medicine, especially context challenging brain cancers like GBM.

Language: Английский

---