MACROMOLECULES
·
2023
·
IF 5.5
Jie Cai,Xiyu Wang,Yuanyuan Liu,Caihui Luo,Xinhua Lu,Yuanli Cai
We herein report a site-specific polymerization-induced electrostatic self-assembly (PIESA) that enables the precision synthesis of highly charged salt-tolerant nanoreactors. Site-specific PIESA is achieved using an anionic aromatic–aliphatic sulfonate block copolymer in photoinitiated reversible addition-fragmentation chain transfter (photo-RAFT) polymerization of a cationic monomer in water at 25 °C. Preferential complexation of cationic growing chains to the aromatic sulfonate block results in not only site-specific molecular recognition but also unique salt-tolerant PIC nanoparticles. Neutral block incorporation leads to ultrafast reaction of very dilute monomer (2.0% w/w) and exclusive formation of more salt-tolerant smaller spheres or 4 nm fibril-structured 10 nm ultrathin lamellae. The ultrathin lamellae can induce a sequence-controllable ultrafast copolymerization of oppositely-charged dilute monomers with perfect shape/size preservation up to 100% conversions, and thus can be viewed as a nanoreactor. This work opened up an avenue for the precision synthesis of highly charged salt-tolerant PIC functional nanoparticles, providing a versatile platform for easy access to structural and functional complexity from simple mixtures.
研究领域:
聚合物化学
·
材料科学
·
纳米技术
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yang Li,Shouwei Zuo,Qiaohong Li,Huawei Huang,Xin Wu,Jing Zhang,Huabin Zhang,Jian Zhang
Hierarchical structures with a complex interior and a functional exterior are highly advantageous for energy-related electrocatalysis. Herein, a carbon-supported molybdenum carbide/sulfide heterostructure interior is covered with a defect-rich MoS 2 nanosheet exterior. The resulting hierarchical structure (C–MoCS x @MoS 2 ) is a promising nanoreactor for seawater splitting. X-ray absorption spectroscopy demonstrates that MoC and MoS 2 are chemically integrated into the C–MoCS x core, providing abundant C–Mo–S sites for hydrogen evolution. Experimental studies and theoretical calculations show that the defect-rich MoS 2 exterior exhibits a high capability for repelling salt deposition, allowing the penetration of low-saline water into the inner C–MoCS x to accelerate the water-splitting reaction. As expected, the obtained C–MoCS x @MoS 2 is remarkably active and exceptionally stable in natural seawater. This work opens new avenues for developing effective electrocatalysts for seawater splitting and other energy-related applications.
研究领域:
材料科学
·
能源化学
·
表面科学
✓ 已验证
DOI
高影响因子
Science Advances
·
2025
·Vol. 11
·期 11
·
IF 12.5
Fuyuan Zheng,Xufeng Wan,Yangming Zhang,Yan Yue,Qiaochu Li,Zhuang Zhang,Shuoyuan Li,Hong Xu,Qiang Su,Xiaoting Chen,Le Tong,Long Zhao,Jian Cao,Xin Tang,Xiao Yang,Jiagang Wu,Jian Li,Xiang Lv,Zongke Zhou,Duan Wang
Tracking and eradicating drug-resistant bacteria are critical for combating implant-associated infections, yet effective antibacterial therapies remain elusive. Herein, we propose an oxygen vacancy–rich (BiFe)0.9(BaTi)0.1O3−x nanoreactor as a piezoelectric sonosensitizer by spatiotemporal ultrasound–driven sono- and chemodynamic tandem catalysis to amplify antibacterial efficacy. The piezoelectric charge carriers under a built-in electric field synchronize the reaction of O2 and H2O, efficiently generating H2O2. The electron-rich oxygen vacancies modulate the local electronic structure of an Fe site. It facilitates reactive oxygen species generation by piezoelectric electrons and accelerates valence state cycles of Fe(III)/Fe(II) to achieve the sustained maintenance of hydroxyl radicals via H2O2/Fe(II)–catalyzed chemodynamic reactions, which lead to bacterial membrane damage. Transcriptomics analysis revealed that intracellular Fe overload induced by excessive Fe(II)-mediated dysregulation of the two-component system disrupts bacterial metabolism, triggering bacterial ferroptosis-like death. Thus, the porous titanium scaffold, engineered with a piezoelectric nanoreactor, demonstrates superior antibacterial efficacy under ultrasound and facilitates osteogenesis via piezoelectric immunomodulation–activated therapy.
研究领域:
生物医学工程
·
微生物学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Minerals
·
2018
·Vol. 8
·期 7
·296
·
IF 1.835
Jing Ouyang,Dawei Mu,Yi Zhang,Huaming Yang,Steven L. Suib
Barium carbonate (BaCO3) materials with the controllable morphology of nanoparticles were selectively loaded into the lumen halloysite nanotubes (abbreviated as Hal) by a urease assisted catalytic implementation strategy. The Hal mineral was pre-treated through leaching by hydrochloric acid (abbreviated as A-Hal), resulting in increased defect sites and zeta potential. The negatively charged urease was loaded inside the positively charged A-Hal lumen, and then through the decomposition of urea catalyzed by urease to produce carbonate ions and ammonia. When Ba2+diffused in, BaCO3particles were selectively synthesized in the lumen of A-Hal, the pore channels of A-Hal effectively controlled the growth and aggregation of BaCO3nanocrystals and their geometrical morphology. The obtained BaCO3/A-Hal-T was characterized by transmission electron microscopy, Fourier transformation infrared spectroscopy and X-ray diffraction, differential scanning calorimetry-thermogravimetry (DSC-TG). The BaCO3/A-Hal-T may provide a candidate for potential applications.Keywords:halloysite;urease;barium carbonate;selective decoration;nanoreactors
研究领域:
材料科学
·
生物催化
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Jiaqi Qiu,Jinjin Huang,Xiaokang Zhu,Yuting Min,Dongming Qi,Tao Chen
Fabrication of highly efficient and recyclable micellar nanoreactors for green organic transformation via self-assembly of catalyst-containing amphiphilic copolymers in water has made great progress. These methods commonly include synthesis and functionalized amphiphilic copolymers and then self-assembly. In this study, a straightforward, one-step strategy for the construction of DMAP-functionalized nanoreactors was developed via polymerization-induced self-assembly (PISA). Acrylate hydrophilic monomer and DMAP-functionalized monomer in the presence of hydrophilic macromolecular chain transfer reagent was polymerized through reversible addition-fragmentation chain transfer (RAFT) polymerization in situ in water, leading to simultaneous amphiphilic block copolymer formation and self-assembly. The diameters of the resulted micelles ranged from 20 to 100 nm depending on the type and amount of hydrophilic monomer, and solid content is up to 25%. The high catalytic activity of the micelles as homogeneous, also readily recyclable catalysts is demonstrated through acylation of a variety of alcohols and recovery by simple dialysis. The study offers an one-pot tandem RAFT-PISA process in water for fabricating highly efficient catalytic nanoreactor.
研究领域:
材料科学
·
化学工程
·
绿色化学
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Qianxi Zhou,Hao Zhang,Tianyu Zeng,Jiahua Yang,Qizhi Liang,Hai Shi,Yongmei Yin,Genxi Li
The dynamic variation of D-amino acids (D-AAs) in human saliva has great potential as the indicator for individual physiological states and disease progression; however, enantiospecific profiling of D-AAs is a great challenge. In this work, a nanoreactor based on mesoporous hydrogen-bonded organic framework (MHOF) has been fabricated for the enantiospecific profiling of D-AAs. The nanoreactor is prepared by using MHOFs as the scaffold to organize the biocatalytic cascade of D-AA oxidase (DAAO) and horseradish peroxidase (HRP). In the meanwhile, the large, stable, and robust transport channels of MHOFs allow the unimpeded transport of the involved biocatalytic substrates. Once D-AA substrates efficiently transport into MHOFs, the chromogenic reactions of 3,3′,5,5′-tetramethylbenzidine (TMB) and H 2 O 2 can be activated. So, using this MHOF nanoreactor, enantiospecific and visual detection of D-AAs can be achieved. Moreover, the stable nanoreactor can be operated in complex solution and utilized for the profiling of D-AA levels in saliva samples collected from gastric cancer patients, suggesting that D-AAs may be a powerful fingerprint for the diagnosis of gastric cancer. Therefore, the fabricated MHOF-based nanoreactor may provide an emerging tool for the enantiospecific profiling of D-AAs and supports the D-AA fingerprint as the indicator of gastric cancer diagnosis.
研究领域:
医学
·
生物化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2017
·Vol. 22
·期 2
·152
·
IF 2.861
Jiachen Ma,Luqing Zhang,Bing Geng,Umair Azhar,Anhou Xu,Shuxiang Zhang
In this work, a thermo-responsive and cross-linked fluoropolymer poly(2,2,2-Trifluoroethyl) methacrylate (PTFEMA) was successfully prepared by reversible addition-fragmentation chain transfer (RAFT) mediated aqueous polymerization with a thermo-responsive diblock poly(dimethylacrylamide-b-N-isopropylacrylamide) (PDMA-b-PNIPAM) that performed a dual function as both a nanoreactor and macro-RAFT agent. The cross-linked polymer particles proved to be in a spherical-like structure of about 50 nm in diameter and with a relatively narrow particle size distribution.1H-NMR and19F-NMR spectra showed that thermo-responsive diblock P(DMA-b-NIPAM) and cross-linked PTFEMA particles were successfully synthesized. Influence of the amount of ammonium persulfate (APS), the molar ratio of monomers to RAFT agent, influence of the amount of cross-linker on aqueous polymerization and thermo-responsive characterization of the particles are investigated. Monomer conversion increased from 44% to 94% with increasing the molar ratio of APS and P(DMA-b-NIPAM) from 1:9 to1:3. As the reaction proceeded, the particle size increased from 29 to 49 nm due to the consumption of TFEMA monomer. The size of cross-linked nanoparticles sharply decreased from 50.3 to 40.5 nm over the temperature range 14–44 °C, suggesting good temperature sensitivity for these nanoparticles.Keywords:RAFT polymerization;nanoreactor;aqueous polymerization;cross-linking;temperature sensitivity
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTENGCOMM
·
2011
·Vol. 14
·期 2
·700-707
·
IF 4.006
Kun Zhang,Dieqing Zhang,Jie Liu,Kuaixia Ren,Hui Luo,Yingjie Peng,Guisheng Li,Xibin Yu
Iodine-incorporated BiOCl (I–BiOCl) core–shell microspheres were for the first time fabricated using a one-step approach under atmospheric pressure. The morphology and compositional characteristics of the 3D hierarchitectures (HAs) of BiOCl were investigated by various techniques such as XRD, FESEM, TEM, EDS, XPS and PL. On the basis of observing the structure of BiOCl and iodine-containing BiOCl at different intervals of reaction time, a three-stage growth mechanism that involves an initial Ostwald ripening process followed by a self-assembly process is proposed. Meanwhile, iodine anions were utilized as both structure-directing agents for fabricating hollow, core–shell, solid structure and doped ions incorporated into the framework of the core–shell BiOCl spheres to extend the light adsorption edge to the visible light region. UV-vis spectra reveal that the band energies of the iodine anions-modified BiOCl (I–BiOCl) hierarchical hollow, core–shell, and solid samples (2.43 eV, 2.28 eV and 2.04 eV, respectively) exhibit obvious red-shifts with respect to that of the pure hollow BiOCl sample (3.23 eV). I–BiOCl without adding poly(vinylpyrrolidone) (PVP) was researched. This result demonstrated that the formation of the core–shell structure is induced by a synergetic effect by iodine and PVP. The specific surface area and porosity of the iodine anions-modified hierarchical BiOCl were also investigated by using nitrogen adsorption–desorption isotherms. The as-prepared I–BiOCl core–shell microspheres showed much higher photocatalytic activity than that of the reported TiO2−x−yNxFy(SC)-3 and Bi2WO6, which was evaluated by the degradation of phenol under visible light (λ > 420 nm) and Rhodamine-B (RhB) dye under visible light (λ > 420 nm) and sun-light irradiation.
研究领域:
材料科学
·
纳米技术
·
光催化化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yishi Lu,Ziyue Zu,Nan Zhong,Yang Li,Xuan Sha,Shangyu Lu,Jie Zhang,Hanyao Sun,Xi Luo,Ziqing Xu,Feiyun Wu,Yuxia Tang,Shouju Wang
Autophagy blockade has emerged as a promising strategy to enhance the antitumor efficacy of pancreatic ductal adenocarcinoma (PDAC). However, autophagy inhibition in PDAC may induce compensatory macropinocytosis to maintain cellular homeostasis by upregulating nuclear factor erythroid 2-related factor 2 (NRF2). In this study, lysosomal-activated nanoreactors loaded with the NRF2 inhibitor ML385 (CPZI-Ms) are developed to spatiotemporally block autophagy and inhibit macropinocytosis. The nanoreactors, which preferentially accumulate in lysosomes, undergo degradation in the acidic lysosomal environment, triggering a Fenton-like reaction between the released Cu 2 ⁺ ions and H₂O₂ to generate hydroxyl radicals. This results in lysosomal membrane permeabilization, which further leads to not only lysosomal autophagy blockade, but also the leakage of Cu 2 ⁺ and ML385 into the cytoplasm. Cu 2 ⁺ induces extensive oxidative stress throughout the whole cell, while ML385 suppresses compensatory macropinocytosis response activated by autophagy blocking. As a result, the Panc02 cells become a “besieged fortress”, with impaired autophagic clearance and restricted nutrient uptake. In vivo, CPZI-Ms effectively suppress tumor growth in Panc02-bearing mice, offering a promising nanoplatform for enhancing cancer cell killing. Taken together, the present work provides an innovative anti-tumor insight by spatiotemporally blocking autophagic flux and inhibiting compensatory macropinocytosis.
研究领域:
肿瘤学
·
药理学
·
纳米医学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shiyan Li,Xuwei Shang,Haiya Lou,Zixu Wang,Yihe Qiu,Shanshan Xiang,Fangying Yu,Hong Yuan
The immunosuppressive tumor environment, characterized by elevated redox levels, significantly impairs the effectiveness of oxidation and the immune response. Here, an electron-accepting-inspired glycopolymer-based nanoreactor (chitosan-grafted nitrobenzene nanoparticles) CNP employing hypoxia-activated group nitrobenzene was constructed to realize cascade bilateral regulation of ferroptosis and immune activation by intervening antioxidant systems. The as-prepared CNP could consume nicotinamide adenine dinucleotide phosphate (NADPH) in the hypoxia-response process, allowing it to be involved in the recycling of glutathione (GSH) and thioredoxin (Trx). This ultimately affects redox homeostasis, leading to reduced GSH levels, increased reactive oxygen species (ROS), and inhibition of (glutathione peroxidase 4) Gpx4. By taking advantage of the sensitivity difference between tumor cells and dendritic cells (DCs) to the ferroptosis inducer erastin (Er) based on varying xCT expression levels, we developed Er-loaded nanoparticles CNP/Er. These nanoparticles not only enhance ferroptosis in 4T1 cells through Gpx4 inhibition by CNP but also promote DC maturation by utilizing CNP’s hypoxia-responsive mechanism to increase ROS levels. The CNP/Er was believed to be an ideal candidate for bilateral regulation of ferroptosis and immune activation in one nanoreactor.
研究领域:
肿瘤学
·
生物材料学
·
免疫学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Chemistry Frontiers
·
2025
·
IF 6.4
Wenjing Yang,Yibing Ji,Lang Li,Chenhang Ding,Wurikaixi Aiyiti,Feilong Xiong,Cijun Shuai
The efficacy of reactive oxygen species (ROS)-related skin tumor therapies is significantly restricted by intracellular overexpressed glutathione (GSH) which is a free radical scavenger. Herein, a GSH-depleting and high ROS production nanoreactor (MFO@MIL) is constructed by in-situ loading manganese ferrite (MnFe2O4) onto the iron-based metal organic frameworks (MIL-101). The MFO@MIL is then incorporated into polycaprolactone (PCL) to prepare a porous skin scaffold, aiming to continuously release of MFO@MIL and simultaneously regulate intracellular reducibility and ROS yield to enhance anti-tumor efficacy. Particularly, the MnFe2O4 with GSH peroxidase-like ability can persistently deplete GSH to decrease the consumption of hydroxyl radical (•OH) generated by Fenton reaction between MIL-101 with hydrogen peroxide (H2O2). Meanwhile, the depletion process of MnFe2O4 will produce Mn2+, which collaborates with the MIL-101 to continuously catalyze H2O2 to produce •OH, remarkably increasing •OH yield and enhancing anti-tumor efficacy. Results showed that the depletion rate of GSH by the scaffold reached 84.4% within 24 hours. The •OH yield of the scaffold is significantly higher than that of the scaffold loaded with MIL-101 alone. Systematic cell experiments demonstrated the powerful anti-tumor efficacy of the scaffold. This study proposes a versatile strategy to significantly enhance ROS-based anti-tumor efficacy and potentially extend it to multiple tumors.
研究领域:
生物医学工程
·
肿瘤学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Rong Dai,Ziliang Zheng,Kai Shi,Xu Wu,Xia An,Xianmei Xie
Ethanol steam reforming (ESR) has drawn great attention for sustainable H 2 production. Design active and sinter resistant nanocatalysts are critical issues for ESR reaction. Herein, a core–shell structured Pt-Cu@Ni-SiO 2 nanocomposite for ESR reaction has been synthesized via a one-pot facile encapsulation strategy, which is featured by highly active and sintering resistance for ESR reaction. Structural and morphological characterizations revealed that each Pt-Cu@Ni-SiO 2 nanocomposite contained a 3 nm Pt-Cu core and multiple Ni nanoparticles with diameters of around 3 nm anchored on the SiO 2 shell. The Pt-Cu@Ni-SiO 2 nanoreactor exhibited higher ethanol conversion (99.99%) and H 2 selectivity (70.32%) and an excellent stability with no loss of activity after 50 h of reaction at 450 °C. The advantages were originated from the ultra-small size of metal nanoparticles and the unique core–shell structure provides a great opportunity to give full play to the catalytic activity of active sites thus guaranteed excellent catalytic activity. Compared with the supported Pt-Cu@Ni-SiO 2 catalyst, the Pt-Cu@Ni-SiO 2 nanoreactor exhibit good stability and sintering resistance due to the encapsulation of the metal nanoparticles and the enhanced metal-support interaction. Thus, it is supposed that this type of catalyst opens a new strategy for the design of the ESR catalyst.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）