SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hao Xu,Qian Ye,Jing Zhang,Qiansong Li,Meijing Wang,Peng Zhou,Guanyu Zhou,Qingguo Wang
In response to the inherent restriction of low Fe(II) regeneration in the Fenton process, this study demonstrated a mutual-promoting configuration, where oxygen functionalized g-C 3 N 4 (OCN) was applied in Fe(III)/H 2 O 2 system to utilize mild natural solar light (SL) for persistent Fe(II) generation. The constructed OCN/Fe(III)/H 2 O 2 /SL system exhibited strong adaptability to various pollutants, and it well outperformed the g-C 3 N 4 (GCN) modified system and the traditional Fenton system in pollutants degradation efficiency. Compared with GCN, OCN could significantly promote the Fe(II) generation under solar light (SL), leading to more efficient H 2 O 2 activation. The characterization analyses revealed the larger surface area and enhanced charge separation of OCN, which were considered to take main responsibility for its enhanced photoactivity. The complexation of Fe(III) with the carboxyl groups of OCN also benefited the Fe(II) generation. ·OH was detected as the dominant radical responsible for metronidazole (MNZ) degradation, and its production in the OCN modified system was about twice that in the GCN modified system and the Fenton system. Moreover, the precipitation of FeO x on the OCN surface benefited the charge separation of the OCN, so that the improved OCN enabled a slight enhancement of MNZ degradation in the reuse experiments. The intermediates of MNZ degradation were analyzed based on the results of LC-MS, which provided insight into MNZ degradation pathways. This work highlighted the concept of self-improving photocatalyst, the ingenious combination of photocatalysis and Fenton-like system formed a mutual-promoting situation where the OCN and the Fenton-like system could both be improved, which endowed the configuration great potential for green and economical oxidation in environmental remediation.
研究领域:
环境科学
·
光催化
·
水处理
·
高级氧化过程
✓ 已验证
DOI
PubMed
高影响因子
ACS Omega
·
2022
·
IF 4.132
Tao Chen,Yuanhong Min,Xiao Yang,Hao Gong,Xiaoying Tian,Li Liu,Yanhua Hou,Wensheng Fu
In recent years, the exploration of the nanozyme, an artificial enzyme with the structure and function of natural enzymes, has become a hot topic in this field. Although significant progress has been made, it is still a huge challenge to design nanozymes with multiple enzyme-like catalytic activities. In this work, we have successfully fabricated a colorimetric sensing platform to mimic peroxidase-like and oxidase-like activities by the CoS1.035 nanoparticles decorated N-doped carbon framework porous dodecahedrons (abbreviated to CoS1.035/N-C PDHs). And the catalytic mechanism of CoS1.035/N-C PDHs toward the peroxidase-like and oxidase-like activities is systematically explored. The results display that CoS1.035/N-C PDHs can catalyze the oxidation of the colorless substrate 3,3,′5,5′-tetramethylbenzidine (TMB) into blue oxidized TMB (ox-TMB) by disintegrating H2O2 or the physically/chemically absorbed O2 into different ROS species (·OH or O2·–) in the presence or absence of H2O2. Therefore, on the basis of the dual-enzyme mimic activities of CoS1.035/N-C PDHs, the bifunctional colorimetric sensing platform is established for H2O2 detection with a wide linear range of 0.5–120 μM and glutathione detection with a linear range of 1–60 μM, respectively. This work provides an efficient platform for dual-enzyme mimics, expanding the application prospect of Co-based chalcogenides as enzyme mimics in biosensing, medical diagnosis, and environment monitoring.
研究领域:
材料科学
·
生物化学
·
纳米技术
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhibin Yin,Qian Ji,Di Wu,Ziwei Li,Minfei Fan,Hongxin Zhang,Xiaolong Zhao,Aiguo Wu,Liang Cheng,Leyong Zeng
In order to achieve safe and high-efficient photodynamic therapy (PDT), it was a powerful strategy of constructing O2-generated nanozyme with intelligent “off/on” modulation and enhancement. Herein, a kind of H2O2-responsive nanozyme was developed for off/on modulation and enhancement of magnetic resonance (MR) imaging and PDT, in which great amounts of gold nanoclusters (AuNCs) were loaded into mesoporous silica to form nanoassembly, and manganese dioxide (MnO2) nanosheets were wrapped as switching shield shell (AuNCs@mSiO2@MnO2). In a neutral physiological environment, stable MnO2 shells eliminated singlet oxygen (1O2) generation to switch off PDT and MR imaging. However, in an acidic tumor microenvironment, the MnO2 shell reacted with H2O2, in which MnO2 degradation switched on MR imaging and PDT, and the generated O2 further enhanced PDT. H2O2-responsive MnO2 degradation brought about excellent MR imaging with a longitudinal relaxation rate of 25.31 mM–1 s–1, and simultaneously sufficient O2 generation guaranteed a 74% high 1O2 yield. Under the irradiation of a 635 nm laser, the viability of MDA-MB-435 cells was reduced to 4%, and the tumors completely disappeared, demonstrating strong PDT performance. Therefore, H2O2-responsive AuNCs@mSiO2@MnO2 nanozyme showed excellent off/on modulation and enhancement of MR imaging and PDT and was a promising intelligent nanoprobe for safe and high-efficiency theranostics.
研究领域:
纳米技术
·
生物医学工程
·
癌症研究
·
材料科学
·
诊疗学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-19
·
IF 10.6
Zhao Pan,Gong Liyang,Chang Le,Du Huiping,Geng Meijuan,Meng Siyu,Dai Liangliang
Chemodynamic therapy (CDT) is seriously limited by the inadequacy of exogenous catalytic ions and endogenous H 2 O 2 in tumors. Herein, a multifunction nano-bomb integrated with calcium peroxide (CaO 2 ) and β-lapachone as donors of H 2 O 2 and GSH-sensitive Fe-based coordination polymer as provider of catalytic ions was constructed for dual cascade-amplified tumor CDT. This hyaluronic acid (HA)-modified nano-bomb could be specially endocytosed by breast cancer cells through a targeting pathway, degraded and released cargoes in response to the GSH-rich cytoplasm. Furthermore, the released CaO 2 and β-lapachone could significantly self-generated sufficient H 2 O 2 , which could dual-cascade amplify CDT and induce severe oxidative to tumors via cooperating with the delivered iron ions from nano-bombs. Moreover, the unloaded iron and calcium ions could further accelerate tumor damage by overloading Ca 2+ and ferroptosis, as accompanied by good magnetic resonance imaging (MRI). In vitro and in vivo studies collectively reveal that this nano-bomb not only self-initiates double cascade-amplified CDT via self-generation of H 2 O 2 , but also efficiently activates ferroptosis and initiates Ca 2+ overloading, consequently significantly tumor growth suppression. This study offers a novel tumor-initiated nano-bomb for dual cascade-amplified CDT and bioimaging with activated ferroptosis and self-supplying H 2 O 2 .
研究领域:
纳米技术
·
癌症治疗
·
生物医学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Hongying Zhao,Ying Chen,Qiusheng Peng,Qingning Wang,Guohua Zhao
A novel bifunctional MOF(2Fe/Co)/CA cathode with a high surface possessing area, and good electrocatalytic and photocatalytic activity, was proposed for the solar photo–electro–Fenton (SPEF) process. The optimal nFe: nCo ratio was 2:1 for successfully introducing MOF(2Fe/Co) on the surface of CA, which is due to the specific interaction affinity of FeOOH between MOF(2Fe/Co) and CA. Continuous on–site generation of H 2 O 2 through an oxygen reduction reaction (ORR) was achieved over the CA cathode. The electron transfer number (n) of the ORR with CA was 2.5 in the selected potential range. Moreover, the addition of MOF can behave as the active sites for enhancing the ORR activity and hence can increase the yield of the H 2 O 2 . Simultaneously, the photoinduced electron (e cb − ) of MOF(2Fe/Co) efficiently in–situ decomposed H 2 O 2 to form hydroxyl radicals ( OH). The observation indicated that the e cb − is an efficient and new Fenton–like catalysts that is pH–independent. Efficient photo–electro–catalytic performance was exhibited when applied to degrade Rhodamine B (RhB) and dimethyl phthalate (DMP). Almost 100% RhB removal and 85% DMP removal were reached in 45 min and 120 min, respectively. The MOF(Fe/Co)/CA presented very low iron and cobalt leaching (<0.5 ppm) even in an acidic media, and it retained an efficient degradation efficiency in the wide pH range of 3–9.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2020
·
IF 5.339
Yue Wu,Shan Jiang,Zhifeng Fu
Based on the specific affinity behavior of teicoplanin towards Gram-positive (G + ) bacteria, teicoplanin-coated magnetic particles were employed to separate G + bacteria. Moreover, intracellular catalase released by catalase-positive bacteria led to catalyzed hydrolysis of H 2 O 2 and inhibition of chemiluminescent signal of luminol-H 2 O 2 system. By combining the separation capability of teicoplanin-coated magnetic particles and the inhibition of luminol chemiluminescence by catalase, a facile method was proposed for quantifying catalase-positive G + bacteria. In this proof-of-principle work, Staphylococcus aureus , Bacillus subtilis and Micrococcus luteus were adopted as model bacteria to evaluate its quantification performance. The three bacteria were quantified within the dynamic ranges of 5.0 × 10 2 –5.0 × 10 7 CFU mL −1 , 4.0 × 10 2 –4.0 × 10 7 CFU mL −1 and 2.0 × 10 2 –2.0 × 10 7 CFU mL −1 , with detection limits of 156 CFU mL −1 , 86 CFU mL −1 and 44 CFU mL −1 , respectively. Gram-negative bacteria and catalase-negative G + bacteria both displayed minor interference. The results for quantifying bacteria in milk, human urine and physiological saline samples demonstrated its reliability for real application. It provided a promising technique tool for food safety, medical diagnosis as well as drug quality control.
研究领域:
微生物学
·
分析化学
·
生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DESALINATION
·
2024
·
IF 8.3
Miaomiao Ye,Xingyuan Wang,Wen Jin,Yueqian Yan,Tuqiao Zhang,Xiaowei Liu
Seawater desalination based on air-water interfacial solar heating has attracted significant attention in recent years. However, the “high temperature, high salinity, sunlight irradiation and enrichment of photosensitive substances” environment formed at the evaporator surface unavoidably enhances the photochemical reaction, which in the next step may lead to the production of active species and by-products. In this work, H 2 O 2 , as an important reactive oxygen species and a transit substance for reactive oxygen species such as ·OH, 1 O 2 , and ·O 2 − , was monitored during solar evaporation. The average H 2 O 2 concentration at the evaporator surface was 2.24 mg·L −1 with a maximum concentration of 5.0 mg·L −1 , which is significantly higher than the average H 2 O 2 concentration in the ocean. The effects of the nitrate ions, halogen ions, iron ions, dissolved organic matter, and solar intensity on the generation of H 2 O 2 concentrations were explored. Finally, halogenated by-products were detected at the evaporator surface when phenol, a model pollutant, was present in the feedwater. This work fills the knowledge gap in understanding the generation of H 2 O 2 and the formation of halogenated by-products at the evaporator surface during solar evaporation.
研究领域:
环境科学
·
化学工程
·
水处理
·
太阳能
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jinyu Gu,Jinxin Xie,Shasha Li,Ge Song,Minghua Zhou
The oxygen-doped carbon nanotubes coated on the carbon felt acted as cathode to enhance the electro-peroxone (OCNT-EP) process. Owing to the introduction of oxygen-containing functional groups and defect sites, the OCNT modified cathode could achieve in-situ H 2 O 2 generation, activation, and catalytic ozonation in the EP process. The OCNT-EP showed a 2.3-folds apparent first-order rate constant ( k ) compared with the EP process using CNT cathode (CNT-EP) for atrazine (ATZ) degradation. According to the processes comparison, quenching experiments, electron paramagnetic resonance (EPR) analysis and determination of hydroxyl radical, it was proved that more . OH and 1 O 2 were generated by the in-situ H 2 O 2 activation and catalytic ozonation in the OCNT-EP process. Especially, this process improved pollutants degradation under acidic condition for the in-situ H 2 O 2 activation and catalytic ozonation, expanding the pH application range of the EP process with a lower energy consumption (0.10 kWh/g ATZ). What’ more, the OCNT modified cathode performed excellent stability with 20 cycle tests, and demonstrated all improved degradation rate (21.7%−78.0%) for various pollutants (carbamazepine, sulfamethazine, phenol and 2,4-dichlorophenol). Therefore, the OCNT-EP process could be considered as a promising and enhanced EP process for wastewater treatment.
研究领域:
环境工程
·
水处理
·
纳米技术
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
研究领域:
电催化
·
材料科学
·
能源化学
·
可持续化学
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Yan Gao,Chunqiao Jin,Xiaocai Li,Kaili Wu,Linna Gao,Xintian Lyu,Xianxi Zhang,Xiao Zhang,Xiliang Luo,Qingyun Liu
Porphyrins modified inorganic semiconductors as a platform in nanomaterials have been paid more attention, due to the fast electron transfer from synergistic effect. Two-Dimensional 5,10,15,20-tetra(4-carboxyphenyl)porphyrin-Co 9 S 8 nanocomposites (H 2 TCPP-Co 9 S 8 nanocomposites) were synthesized via a simple one-step hydrothermal method . A simple and highly sensitive method toward colorimetric biosensing of H 2 O 2 was developed by monitoring the color change of chromogenic substrate 3,3,5,5-tetramethylbenzidine (TMB) from colorless to blue. Notably, the H 2 TCPP-Co 9 S 8 nanocomposites were proved to possess the highly peroxidase-like activity, compared with that of pure Co 9 S 8 nanosheets . Unusually, ESR data verified that the catalytic mechanism of H 2 TCPP-Co 9 S 8 was firstly ascribed to production of superoxide radicals. The detection limit of H 2 O 2 was 8.19 μM and the linear range from 10 to 200 μM. Similarly, The detection limit of glutathione is as low as 0.194 μM with a linear range of 0.3–10 μM. Furthermore, this sensor has shown high selectivity to H 2 O 2 detection and was successfully applied in H 2 O 2 detection in contact lens fluid samples with satisfying results.
研究领域:
材料科学
·
纳米技术
·
分析化学
·
生物传感器
✓ 已验证
产品关联
DOI
高影响因子
BIOMACROMOLECULES
·
2022
·
IF 6.978
Xiaowen Xu,Yu Ran,Chengyuan Huang,Zongning Yin
Although “closed-loop” smart insulin delivery systems have been extensively investigated, the majority of them suffer from low insulin loading efficiency and slow glucose response. Here, we constructed a novel nanocomplex (NC), which was prepared by electrostatic interaction between negatively charged insulin prodrug nanoparticles (NPs) and positively charged polycaprolactone–polyethylenimine (PCL–PEI) micelles. The insulin prodrug was linked to acetalated dextran (AD) via borate ester bonds to form IAD NPs, and glucose oxidase (GOx) was encapsulated in PCL–PEI micelles. The NC was negatively charged with a high insulin grafting rate (0.473 mg/mg), and in vitro experiments revealed that IAD was sensitive to hyperglycemia and H2O2, whereas GOx significantly improved the response to glucose by altering the microenvironment to promote sustained insulin release. Furthermore, compared with free insulin and IAD NPs, subcutaneously injected NCs in diabetic rats had long-term hypoglycemic effects, showing excellent biocompatibility in vitro and in vivo, which had good potential in insulin self-regulation delivery.
研究领域:
药学
·
纳米技术
·
生物医学工程
·
糖尿病研究
✓ 已验证
DOI
PubMed
高影响因子
Theranostics
·
2024
·
IF 12.4
Muzi Li,Nan Wang,Ruiyuan Liu,Xinyue Zhang,Wei He,Wen Zhang,Jiaxin Li,Chen Peng,Yan Li
Background: Oral insulin delivery is considered a revolutionary alternative to daily subcutaneous injection. However, the oral bioavailability of insulin is very low due to the poor oral absorption into blood circulation. Methods: To promote penetration across the intestinal epithelium and achieve enhanced and safe glucose-responsive oral insulin delivery, pH and H 2 O 2 dual-sensitive nanoparticles (NPs) were constructed. The NPs were loaded of glucose oxidase (GOx) and insulin by pH and H 2 O 2 dual-sensitive amphiphilic polymer incorporated with phenylboronic ester-conjugated poly(2-hydroxyethyl methacrylate) and poly(carboxybetaine) (PCB). The dual-sensitive NPs were utilized for the treatment of type 1 diabetes mellitus (T1DM) after oral administration. Results: The dual-sensitive NPs could enhance the transport of insulin across the intestinal epithelium into blood facilitated by zwitterionic PCB. By virtue of the generated low pH and high H 2 O 2 with GOx in hyperglycemic environment, the pH and H 2 O 2 dual-sensitive NPs were disassembled to achieve rapid and sustained release of insulin. After oral administration of the dual-sensitive NPs in enteric capsules into T1DM mouse model, the oral bioavailability of insulin reached 20.24%, and the NPs achieved hypoglycemic effect for a few hours longer than subcutaneously injected insulin. Importantly, the pH and H 2 O 2 dual-sensitive NPs could ameliorate the local decline of pH and rise of H 2 O 2 to avoid the toxic side effect. Conclusion: Therefore, this work would provide a promising platform for the enhanced and safe treatment of diabetes mellitus.
研究领域:
药学
·
纳米技术
·
糖尿病研究
·
药物递送系统
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）