Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 84
Filtrar
1.
Bioresour Technol ; 408: 131177, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39097240

RESUMO

Biological degradation of PET plastic holds great potential for plastic recycling. However, the high costs associated with preparing free enzymes for degrading PET make it unfeasible for industrial applications. Hence, we developed various cell catalysts by surface-displaying PETase mutants and MHETase using autotransporters in E. coli and P. putida. The efficiency of surface display was enhanced through modifying the host, co-expressing molecular chaperones, and evoluting the autotransporter. In strain EC9F, PET degradation rate was boosted to 3.85 mM/d, 51-fold and 23-fold increase compared to free enzyme and initial strain ED1, respectively. The reusability of cell catalyst EC9F was demonstrated with over 38 % and 30 % of its initial activity retained after 22 cycles of BHET degradation and 3 cycles of PET degradation. The highest reported PET degradation rate of 4.95 mM/d was achieved by the dual-enzyme cascade catalytic system EC9F+EM2+R, a mixture of cell catalyst EC9F and EM2 with surfactant rhamnolipid.


Assuntos
Escherichia coli , Mutação , Escherichia coli/genética , Pseudomonas putida/enzimologia , Pseudomonas putida/genética , Polietilenotereftalatos/química , Polietilenotereftalatos/metabolismo , Catálise , Biocatálise , Biodegradação Ambiental
2.
J Colloid Interface Sci ; 678(Pt A): 378-392, 2024 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-39213991

RESUMO

Combination therapies have attracted significant attention because they address the limitations of monotherapy while improving overall efficacy. In this study, we designed a novel nanoplatform, named GOx@Fe-DMSN@PDA (GFDP), by integrating Fe2+ into dendritic mesoporous silica nanoparticles (DMSN) and selecting glucose oxidase (GOx) as the model drug loaded into the DMSN pores. Additionally, we coated the surface of the DMSN with polydopamine (PDA) to confer pH/near infrared (NIR) light-responsive controlled-release behavior and photothermal therapy (PTT). The introduction of Fe2+ into the DMSN framework greatly improved biodegradability and enhanced the peroxidase (POD)-like activity of GFDP. In addition, GOx could consume glucose and generate hydrogen peroxide (H2O2) within tumor cells to facilitate starvation therapy and enhance cascade catalysis. The PDA coating provided the DMSN with an intelligent response release ability, promoting efficient photothermal conversion and achieving the PTT effect. Cellular tests showed that under NIR light irradiation, GFDP exhibited a synergistic effect of PTT-enhanced starvation therapy and cascade catalysis, with a half-maximal inhibitory concentration (IC50) of 2.89 µg/mL, which was significantly lower than that of GFDP without NIR light irradiation (18.29 µg/mL). The in vivo anti-tumor effect indicated that GFDP could effectively accumulate at the tumor site for thermal imaging and showed remarkable synergistic therapeutic effects. In summary, GFDP is a promising nanoplatform for multi-modal combination therapy that integrates starvation therapy, PTT, and cascade catalysis.

3.
J Nanobiotechnology ; 22(1): 416, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-39014402

RESUMO

Reactive oxygen species (ROS)-associated anticancer approaches usually suffer from two limitations, i.e., insufficient ROS level and short ROS half-life. Nevertheless, no report has synchronously addressed both concerns yet. Herein, a multichannel actions-enabled nanotherapeutic platform using hollow manganese dioxide (H-MnO2) carriers to load chlorin e6 (Ce6) sonosensitizer and CO donor (e.g., Mn2(CO)10) has been constructed to maximumly elevate ROS level and trigger cascade catalysis to produce CO. Therein, intratumoral H2O2 and ultrasound as endogenous and exogeneous triggers stimulate H-MnO2 and Ce6 to produce •OH and 1O2, respectively. The further cascade reaction between ROS and Mn2(CO)10 proceeds to release CO, converting short-lived ROS into long-lived CO. Contributed by them, such a maximumly-elevated ROS accumulation and long-lived CO release successfully suppresses the progression, recurrence and metastasis of lung cancer with a prolonged survival rate. More significantly, proteomic and genomic investigations uncover that the CO-induced activation of AKT signaling pathway, NRF-2 phosphorylation and HMOX-1 overexpression induce mitochondrial dysfunction to boost anti-tumor consequences. Thus, this cascade catalysis strategy can behave as a general means to enrich ROS and trigger CO release against refractory cancers.


Assuntos
Monóxido de Carbono , Neoplasias Pulmonares , Compostos de Manganês , Óxidos , Porfirinas , Espécies Reativas de Oxigênio , Espécies Reativas de Oxigênio/metabolismo , Neoplasias Pulmonares/metabolismo , Neoplasias Pulmonares/tratamento farmacológico , Humanos , Monóxido de Carbono/farmacologia , Monóxido de Carbono/metabolismo , Monóxido de Carbono/química , Animais , Compostos de Manganês/química , Compostos de Manganês/farmacologia , Óxidos/química , Óxidos/farmacologia , Camundongos , Porfirinas/química , Porfirinas/farmacologia , Clorofilídeos , Linhagem Celular Tumoral , Camundongos Endogâmicos BALB C , Peróxido de Hidrogênio/metabolismo , Camundongos Nus , Células A549
4.
Nano Lett ; 24(31): 9768-9775, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39057181

RESUMO

Excessive production of waste polyethylene terephthalate (PET) poses an ecological challenge, which necessitates developing technologies to extract the values from end-of-life PET. Upcycling has proven effective in addressing the low profitability of current recycling strategies, yet existing upcycling technologies operate under energy-intensive conditions. Here we report a cascade strategy to steer the transformation of PET waste into glycolate in an overall yield of 92.6% under ambient conditions. The cascade approach involves setting up a robust hydrolase with 95.6% PET depolymerization into ethylene glycol (EG) monomer within 12 h, followed by an electrochemical process initiated by a CO-tolerant Pd/Ni(OH)2 catalyst to convert the EG intermediate into glycolate with high Faradaic efficiency of 97.5%. Techno-economic analysis and life cycle assessment indicate that, compared with the widely adopted electrochemical technology that heavily relies on alkaline pretreatment for PET depolymerization, our designed enzymatic-electrochemical approach offers a cost-effective and low-carbon pathway to upgrade PET.


Assuntos
Técnicas Eletroquímicas , Polietilenotereftalatos , Polietilenotereftalatos/química , Catálise , Etilenoglicol/química , Poliésteres/química , Reciclagem , Hidrolases/química
5.
Biosens Bioelectron ; 262: 116553, 2024 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-39018977

RESUMO

A spatial-resolved and self-calibrated photoelectrochemical (PEC) biosensor has been fabricated by a multifunctional CeO2/CdS heterostructure, achieving portable and sensitive detection of carcinoembryonic antigen (CEA) using a homemade 3D printing device. The CeO2/CdS heterostructure with matched band structure is prepared to construct the dual-photoelectrodes to improve the PEC response of CeO2. In particular, as the photoactive nanomaterial, the CeO2 also plays the role of peroxidase mimetic nanozymes. Therefore, the catalytic performance of CeO2 with different morphologies (e.g., nano-cubes, nano-rods and nano-octahedra) have been studied, and CeO2 nano-cubes (c-CeO2) achieve the optimal catalytic activity. Upon introducing CEA, the sandwich-type immunocomplex is formed in the microplate using GOx-AuNPs-labeled second antibody as detection antibody. As a result, H2O2 can be produced from the catalytic oxidization of glucose substrate by GOx, which is further catalyzed by CeO2 to form •OH, thus in situ etching CdS and decreasing the photocurrents. The self-calibration is achieved by the dual-channel photoelectrodes on the homemade 3D printing device to obtain the photocurrents ratio, thus effectively normalizing the fluctuations of external factors to enhance the accuracy. This integrated biosensor with a detection limit as low as 0.057 ng mL-1 provides a promising way for ultrasensitive immunoassay in clinic application in complex environments.


Assuntos
Técnicas Biossensoriais , Compostos de Cádmio , Antígeno Carcinoembrionário , Cério , Técnicas Eletroquímicas , Impressão Tridimensional , Sulfetos , Técnicas Biossensoriais/instrumentação , Cério/química , Imunoensaio/instrumentação , Imunoensaio/métodos , Antígeno Carcinoembrionário/sangue , Compostos de Cádmio/química , Sulfetos/química , Humanos , Limite de Detecção , Ouro/química , Anticorpos Imobilizados/química , Nanopartículas Metálicas/química
6.
Adv Healthc Mater ; : e2401834, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38889805

RESUMO

Multiple enzyme-induced cascade catalysis has an indispensable role in the process of complex life activities, and is widely used to construct robust biosensors for analyzing various targets. The immobilized multi-enzyme cascade catalysis system is a novel biomimetic catalysis strategy that immobilizes various enzymes with different functions in stable carriers to simulate the synergistic catalysis of multiple enzymes in biological systems, which enables high stability of enzymes and efficiency enzymatic cascade catalysis. Nanozymes, a type of nanomaterial with intrinsic enzyme-like characteristics and excellent stabilities, are also widely applied instead of enzymes to construct immobilized cascade systems, achieving better catalytic performance and reaction stability. Due to good stability, reusability, and remarkably high efficiency, the immobilized multi-enzyme/nanozyme biomimetic cascade catalysis systems show distinct advantages in promoting signal transduction and amplification, thereby attracting vast research interest in biosensing applications. This review focuses on the research progress of the immobilized multi-enzyme/nanozyme biomimetic cascade catalysis systems in recent years. The construction approaches, factors affecting the efficiency, and applications for sensitive biosensing are discussed in detail. Further, their challenges and outlooks for future study are also provided.

7.
J Colloid Interface Sci ; 672: 512-519, 2024 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-38852353

RESUMO

Conversion of NO3- to NH3 proceeds stepwise in natural system under two different enzymes involving intermediate NO2-. Artificial electro-driven NO3- reduction also faces the obstacle of low faradaic efficiency due to insufficient utilization of this intermediate. Herein, we demonstrate a bimetallic COF-based electrocatalyst for the cascade catalysis of NO3--to-NO2--to-NH3 for the first time. TpBpy-Cu2Co4 exhibits a significantly improved performance, with an enhancement factor of 1.4-2 compared to monometallic TpBpy-M. The NH3 yield rate achieves 25.6 mg h-1 mgcat.-1 at -0.55 V vs RHE over TpBpy-Cu2Co4, together with excellent faradaic efficiency (93.4 %). This achievement demonstrates cascade catalysis between Co and Cu units, and their distinct roles are investigated through electrochemical experiments and theory calculations. In electrocatalytic process, Cu site facilities *NO3-to-*NO3H step, while the Co site significantly decreases the energy barrier of *NHOH-to-*NH. The present work provides a valuable inspiration in designing efficient catalysts for cascade reaction.

8.
J Agric Food Chem ; 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38836289

RESUMO

The bioderacemization of racemic phosphinothricin (D, L-PPT) is a promising route for the synthesis of l-phosphinothricin (L-PPT). However, the low activity and tolerance of wild-type enzymes restrict their industrial applications. Two stereocomplementary aminotransferases with high activity and substrate tolerance were identified in a metagenomic library, and a one-pot, two-stage artificial cascade biocatalytic system was developed to produce L-PPT through kinetic resolution and asymmetric amination. We observed that 500 mM D, L-PPT (100 g/L) could be converted into L-PPT with 94% final conversion and >99.9% enantiomeric excess (e.e.) within 24 h, with only 0.02 eq amino acceptor pyruvate and 1.2 eq amino donor l-aspartate required. The process could be scaled up to 10 L under sufficient oxygen and stirring. The superior catalytic performance of this system provides an eco-friendly and sustainable approach to the industrial deracemization of D, L-PPT to L-PPT.

9.
Biomater Adv ; 162: 213919, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38861801

RESUMO

Tumor microenvironment (TME)-responsive chemodynamic therapy (CDT) is severely hindered by insufficient intracellular H2O2 level that seriously deteriorates antitumor efficacy, albeit with its extensively experimental and theoretical research. Herein, we designed atomically dispersed FeCo dual active sites anchored in porous carbon polyhedra (termed FeCo/PCP), followed by loading with glucose oxidase (GOx) and anticancer doxorubicin (DOX), named FeCo/PCP-GOx-DOX, which converted glucose into toxic hydroxyl radicals. The loaded GOx can either decompose glucose to self-supply H2O2 or provide fewer nutrients to feed the tumor cells. The as-prepared nanozyme exhibited the enhanced in vitro cytotoxicity at high glucose by contrast with those at less or even free of glucose, suggesting sufficient accumulation of H2O2 and continual transformation to OH for CDT. Besides, the FeCo/PCP-GOx-DOX can subtly integrate starvation therapy, the FeCo/PCP-initiated CDT, and DOX-inducible chemotherapy (CT), greatly enhancing the therapeutic efficacy than each monotherapy.


Assuntos
Doxorrubicina , Glucose Oxidase , Peróxido de Hidrogênio , Peróxido de Hidrogênio/metabolismo , Peróxido de Hidrogênio/química , Doxorrubicina/farmacologia , Doxorrubicina/química , Doxorrubicina/uso terapêutico , Glucose Oxidase/metabolismo , Glucose Oxidase/química , Humanos , Animais , Microambiente Tumoral/efeitos dos fármacos , Camundongos , Antineoplásicos/farmacologia , Antineoplásicos/química , Antineoplásicos/uso terapêutico , Linhagem Celular Tumoral , Neoplasias/tratamento farmacológico , Glucose/metabolismo , Domínio Catalítico
10.
Acta Biomater ; 182: 245-259, 2024 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-38729545

RESUMO

Diabetic wound healing is a great clinical challenge due to the microenvironment of hyperglycemia and high pH value, bacterial infection and persistent inflammation. Here, we develop a cascade nanoreactor hydrogel (Arg@Zn-MOF-GOx Gel, AZG-Gel) with arginine (Arg) loaded Zinc metal organic framework (Zn-MOF) and glucose oxidase (GOx) based on chondroitin sulfate (CS) and Pluronic (F127) to accelerate diabetic infected wound healing. GOx in AZG-Gel was triggered by hyperglycemic environment to reduce local glucose and pH, and simultaneously produced hydrogen peroxide (H2O2) to enable Arg-to release nitric oxide (NO) for inflammation regulation, providing a suitable microenvironment for wound healing. Zinc ions (Zn2+) released from acid-responsive Zn-MOF significantly inhibited the proliferation and biofilm formation of S.aureus and E.coli. AZG-Gel significantly accelerated diabetic infected wound healing by down-regulating pro-inflammatory tumor necrosis factor (TNF)-α and interleukin (IL)-6, up-regulating anti-inflammatory factor IL-4, promoting angiogenesis and collagen deposition in vivo. Collectively, our nanoreactor cascade strategy combining "endogenous improvement (reducing glucose and pH)" with "exogenous resistance (anti-bacterial and anti-inflammatory)" provides a new idea for promoting diabetic infected wound healing by addressing both symptoms and root causes. STATEMENT OF SIGNIFICANCE: A cascade nanoreactor (AZG-Gel) is constructed to solve three key problems in diabetic wound healing, namely, hyperglycemia and high pH microenvironment, bacterial infection and persistent inflammation. Local glucose and pH levels are reduced by GOx to provide a suitable microenvironment for wound healing. The release of Zn2+ significantly inhibits bacterial proliferation and biofilm formation, and NO reduces wound inflammation and promotes angiogenesis. The pH change when AZG-Gel is applied to wounds is expected to enable the visualization of wound healing to guide the treatment of diabetic wound. Our strategy of "endogenous improvement (reducing glucose and pH)" combined with "exogenous resistance (anti-bacterial and anti-inflammatory)" provides a new way for promoting diabetic wound healing.


Assuntos
Glucose Oxidase , Estruturas Metalorgânicas , Óxido Nítrico , Cicatrização , Zinco , Cicatrização/efeitos dos fármacos , Animais , Zinco/química , Zinco/farmacologia , Óxido Nítrico/metabolismo , Estruturas Metalorgânicas/farmacologia , Estruturas Metalorgânicas/química , Glucose Oxidase/farmacologia , Glucose Oxidase/metabolismo , Diabetes Mellitus Experimental/patologia , Microambiente Celular/efeitos dos fármacos , Camundongos , Hidrogéis/química , Hidrogéis/farmacologia , Masculino , Staphylococcus aureus/efeitos dos fármacos , Biofilmes/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Antibacterianos/farmacologia , Antibacterianos/química , Arginina/farmacologia , Arginina/química
11.
Int J Biol Macromol ; 268(Pt 1): 131870, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38670199

RESUMO

As one of the most important industrial enzymes, α-amylase is widely used in food processing, such as starch sugar and fermentation, bringing high added value to industry of more than a trillion dollars. We developed a multi-enzyme system (Glu&Gox@Cu-MOF-74) prepared by embedding α-glucosidase (Glu) and glucose oxidase (Gox) into the biomimetic metal-organic framework Cu-MOF-74 using in situ encapsulation within 15 min at room temperature for efficient and sensitive detection of α-amylase activity. Benefitting from the remarkable peroxidase-mimicking property and rigid skeleton of Cu-MOF-74, the biocatalytic platform exhibited excellent cascade activity and tolerance in various extremely harsh environments compared to natural enzymes. On this basis, a cascade biocatalytic platform was constructed for the detection of α-amylase activity with wide linear range (5-100 U/L) and low limit of detection (1.45 U/L). The colorimetric cascade scheme is important for the sensitive and selective determination of α-amylase in complex fermentation samples, and the detection time is short (∼0.5 h). This work provides new ideas for the detection of α-amylase based on the cascade amplification method.


Assuntos
Glucose Oxidase , Estruturas Metalorgânicas , alfa-Amilases , alfa-Amilases/análise , alfa-Amilases/metabolismo , alfa-Amilases/química , Estruturas Metalorgânicas/química , Glucose Oxidase/química , Glucose Oxidase/metabolismo , Técnicas Biossensoriais/métodos , Colorimetria/métodos , alfa-Glucosidases/metabolismo , alfa-Glucosidases/análise , Biocatálise , Cobre/química , Cobre/análise , Enzimas Imobilizadas/química , Enzimas Imobilizadas/metabolismo , Limite de Detecção
12.
Biosens Bioelectron ; 248: 115965, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38176253

RESUMO

A fast and accurate method for ultrasensitive monitoring of substrate is significant for cascade molecular detection. Here, we synthesize a glucose oxidase (GOx) microgel with iron coordination (Fe/GOx microgel). The microgel is cross-linked by chitosan and iron ion coordination which construct a tubular structure. Powder X-ray diffraction and Brunauer-Emmett-Teller results confirm the tubular crystal structure with a high specific surface area is formed in the microgel. The tubular structure offers a stable channel for intermediate transport which ensures the stabilization for the intermediate transport, and high specific surface area enhances the interaction between substrates and catalysts. As a result, the sensitivity of the Fe/GOx microgel is 175.5 µA mM-1 cm-2 and the lowest detection limit is 4.42 µM. In addition, the nanoscale Fe/GOx microgel also has the characteristics of reusability and maintains its activity after five times of catalysis. The generation of free radicals during the catalytic process can be detected by light detection and electrochemical signal detection within different detection limits. Therefore, Fe/GOx microgel provides a new platform and catalyst for the precise detection of cascade catalysis.


Assuntos
Técnicas Biossensoriais , Microgéis , Sistemas Automatizados de Assistência Junto ao Leito , Limite de Detecção , Técnicas Biossensoriais/métodos , Ferro/química , Glucose Oxidase/química , Glucose
13.
Angew Chem Int Ed Engl ; 63(12): e202315777, 2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38233351

RESUMO

Electrochemical CO2 reduction can convert CO2 to value-added chemicals, but its selectivity toward C3+ products are very limited. One possible solution is to run the reactions in hybrid processes by coupling electrocatalysis with other catalytic routes. In this contribution, we report the cascade electrocatalytic and thermocatalytic reduction of CO2 to propionaldehyde. Using Cu(OH)2 nanowires as the precatalyst, CO2 /H2 O is reduced to concentrated C2 H4 , CO, and H2 gases in a zero-gap membrane electrode assembly (MEA) reactor. The thermochemical hydroformylation reaction is separately investigated with a series of rhodium-phosphine complexes. The best candidate is identified to be the one with the 1,4-bis(diphenylphosphino)butane diphosphine ligand, which exhibits a propionaldehyde turnover number of 1148 under a mild temperature and close-to-atmospheric pressure. By coupling and optimizing the upstream CO2 electroreduction and downstream hydroformylation reaction, we achieve a propionaldehyde selectivity of ~38 % and a total C3 oxygenate selectivity of 44 % based on reduced CO2 . These values represent a more than seven times improvement over the best prior electrochemical system alone or over two times improvement over other hybrid systems.

14.
Chemistry ; 30(10): e202302959, 2024 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-38012090

RESUMO

A two-enzyme cascade system containing ω-transaminase (ω-TA) and L-threonine aldolase (L-ThA) was reported for the synthesis of 3-Phenylserine starting from benzylamine, and PLP was utilized as the only cofactor in these both two enzymes reaction system. Based on the transamination results, benzylamine was optimized as an advantageous amino donor as confirmed by MD simulation results. This cascade reaction system could not only facilitate the in situ removal of the co-product benzaldehyde, enhancing the economic viability of the reaction, but also establish a novel pathway for synthesizing high-value phenyl-serine derivatives. In our study, nearly 95 % of benzylamine was converted, yielding over 54 % of 3-Phenylserine under the optimized conditions cascade reaction.


Assuntos
Glicina Hidroximetiltransferase , Serina , Serina/análogos & derivados , Serina/metabolismo , Glicina Hidroximetiltransferase/metabolismo , Benzilaminas , Fosfato de Piridoxal
15.
Small ; 20(22): e2310597, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38143296

RESUMO

The electrochemical denitrification of nitrate (NO3 -) in actual wastewater to nitrogen (N2) is an effective approach to reversing the current imbalance of the nitrogen cycle and the eutrophication of water. However, electrostatic repulsion between NO3 - and the cathode results in the low efficiency of NO3 - reduction reaction (NO3RR). Here, density functional theory (DFT) calculations are used as a theoretical guide to design a Pd cluster-loaded multivalent Cu foam (Pd/Cu2O-CF) electrocatalyst, which achieves a splendid 97.8% NO3 - removal rate, 97.9% N2 selectivity, 695.5 mg N g-1 Pd h-1 reduction efficiency, and 60.0% Faradaic efficiency at -1.3 V versus SCE. The projected density of states (pDOS) indicates that NO3 - and Pd/Cu2O-CF are bonded via strong complexation between the O 2p (in NO3 -) and Cu 3d (in Cu2O) with the input of voltage, which reduces the electrostatic repulsion and enhances the enrichment of NO3 - on the cathode. In-situ characterizations demonstrate that Pd[H] can reduce Cu2O to Cu, and subsequently Cu reduces NO3 - to nitrite (NO2 -) accompanied by in situ reconfiguration of multivalent Cu foam. NO2 - is then transferred to the surface of Pd clusters by the cascade catalysis and accelerates the breaking of N─O bonds to form Pd─N, and eventually achieves the N≡N bond formation.

16.
Adv Healthc Mater ; 13(10): e2303476, 2024 04.
Artigo em Inglês | MEDLINE | ID: mdl-38161211

RESUMO

Chirality is common in nature, which determines the high enantioselectivity of living systems. Selecting suitable chiral configurations is of great meaning for nanostructures to function better in biological systems. In this study, chiral Co3O4-H2TPPS-Au (CoHAu) nanoassemblies are constructed to accelerate the production ∙OH by consuming D-glucose (D-Glu, widely spread in nature) based on their outstanding enantioselective cascade-catalytic abilities. In particular, D-CoHAu nanoassemblies are more effective in the catalytic conversion of D-Glu than L-CoHAu nanoassemblies. This phenomenon is due to the stronger binding affinity of D-CoHAu nanoassemblies indicated by the lower Km value. Moreover, D-CoHAu nanoassemblies display excellent consumption-ability of D-Glu and production of ∙OH in living cells, which can eliminate senescent cells effectively based on their intracellular enantioselective cascade-catalysis. This research establishes the foundation for bio-mimicking nanostructures with unique functionalities to regulate abnormal biological activities better.


Assuntos
Nanoestruturas , Estereoisomerismo , Catálise , Nanoestruturas/química , Senescência Celular
17.
J Nanobiotechnology ; 21(1): 400, 2023 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-37907972

RESUMO

Cancer has always posed a significant threat to human health, prompting extensive research into new treatment strategies due to the limitations of traditional therapies. Starvation therapy (ST) has garnered considerable attention by targeting the primary energy source, glucose, utilized by cancer cells for proliferation. Glucose oxidase (GOx), a catalyst facilitating glucose consumption, has emerged as a critical therapeutic agent for ST. However, mono ST alone struggles to completely suppress tumor growth, necessitating the development of synergistic therapy approaches. Metal catalysts possess enzyme-like functions and can serve as carriers, capable of combining with GOx to achieve diverse tumor treatments. However, ensuring enzyme activity preservation in normal tissue and activation specifically within tumors presents a crucial challenge. Nanodelivery systems offer the potential to enhance therapy effectiveness by improving the stability of therapeutic agents and enabling controlled release. This review primarily focuses on recent advances in the mechanism of GOx combined with metal catalysts for synergistic tumor therapy. Furthermore, it discusses various nanoparticles (NPs) constructs designed for synergistic therapy in different carrier categories. Finally, this review provides a summary of GOx-metal catalyst-based NPs (G-M) and offers insights into the challenges associated with G-M therapy, delivery design, and oxygen (O2) supply.


Assuntos
Nanopartículas Metálicas , Nanopartículas , Neoplasias , Humanos , Glucose Oxidase , Sistemas de Liberação de Fármacos por Nanopartículas , Neoplasias/terapia , Metais , Glucose , Linhagem Celular Tumoral , Peróxido de Hidrogênio
18.
J Agric Food Chem ; 71(51): 20772-20781, 2023 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-37963219

RESUMO

l-Phenyllactic acid (l-PLA) is a small molecular organic acid that exhibits a powerful capacity for inhibition against foodborne pathogens. In this work, we developed a new cost-effective and environmentally friendly process for the biosynthesis of l-PLA. This strategy designed a novel whole-cell biotransformation system employing two heterologous enzymes, namely, phenylalanine dehydrogenase (PheDH) and l-hydroxyisocaproate dehydrogenase (l-HicDH). The novelty of this strategy lies in the first-time utilization of these two enzymes, which not only enables cascade catalysis for the production of l-PLA but also facilitates the regeneration of the coenzymes (NAD+/NADH) using only two enzymes rather than introducing more heterologous enzymes to the system. Consequently, this strategy can effectively simplify the biosynthesis process of l-PLA and minimize production costs. The initial l-PLA yield using this process achieved 2.53 ± 0.07 g/L. Furthermore, through meticulous optimization of the parameters for inducible enzyme expression and l-PLA biosynthesis, the l-PLA yield was successfully increased to 4.68 ± 0.04 g/L with a yield rate of 64.54 ± 0.29%. Moreover, this novel strategy is versatile in the biosynthesis of other organic acids, which can be achieved by easily modulating the combinations of substrates and enzymes.


Assuntos
Coenzimas , Regeneração , Biotransformação , Poliésteres
19.
Angew Chem Int Ed Engl ; 62(47): e202308827, 2023 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-37802975

RESUMO

Enzymatic catalysis with high efficiency allows them a great prospect in metabolite monitoring in living cells. However, complex tumor microenvironments, such as acidity, H2 O2 , and hypoxia, are bound to disturb catalytic reactions for misleading results. Here, we report a spatially compartmentalized artificial organelle to correct intratumoral glucose analysis, where the zeolitic imidazolate framework-8 immobilized glucose oxidase-horseradish peroxidase cascade core and catalase-directed shell act as signal transduction and guarding rooms respectively. The acid-digested core and stable shell provide appropriate spaces to boost biocatalytic efficiency with good tolerability. Notably, the endogenous H2 O2 is in situ decomposed to O2 by catalase, which not only overcomes the interference in signal output but also alleviates the hypoxic states to maximize glucose oxidation. The marked protective effect and biocompatibility render artificial organelles to correct the signal transduction for dynamic monitoring glucose in vitro and in vivo, achieving our goal of accurate intratumoral metabolite analysis.


Assuntos
Células Artificiais , Estruturas Metalorgânicas , Estruturas Metalorgânicas/metabolismo , Glucose/análise , Catalase/metabolismo , Oxirredução , Glucose Oxidase/metabolismo
20.
Adv Sci (Weinh) ; 10(31): e2304149, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37635202

RESUMO

CsPbX3 perovskite nanocrystal (NC) is considered as an excellent optical material and is widely applied in optoelectronics. However, its poor water stability impedes its study in enzyme-like activity, and further inhibits its application in biomimetic cascade catalysis. Herein, for the first time, the oxidase-like and ascorbate oxidase-like activities of an amphiphilic polymer capped CsPbX3 are demonstrated, and its catalytic mechanism is further explored. Furthermore, an all-nanozyme cascade system (multifunctional CsPbBr3 @Zr-metal organic framework (Zr-MOF) and Prussian blue as oxidase-like and peroxidase-like nanozyme) is constructed with a portable paper-based device for realizing the dual-mode (ratiometric fluorescence and colorimetric) detection of ascorbic acid in a point-of-care (POC) fashion. This is the first report on the utilization of all-inorganic CsPbX3 perovskite NC in biomimetic cascade catalysis, which opens a new avenue for POC clinical disease diagnosis.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA