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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Enhancing the dioxygen activation for arsenic removal by Cu0 nano-shell-decorated nZVI: Synergistic effects and mechanisms

Longqian Xu,Kaili Yan,Yunfeng Mao,Deli Wu

Using copper and/or iron based nanomaterial to activate dioxygen to produce free radicals is an alternative and environmental friendly technique, but the low conversion efficiency of oxygen and the rate-limiting step of superoxide radical generation limit current application. In present work, Cu 0 nano-shell-decorated nZVI (CFNs) was synthesized and employed to enhance the activation of oxygen for the removal of arsenic at circumneutral pH. The adsorption and oxidation pathways of arsenic were investigated by determination of arsenic distribution and radical scavenger methods. The results showed that the removal of arsenic by CFNs involved the initial step of As III adsorption by ferrihydrite followed by the oxidation of As III by hydroxyl radical ( OH abs ) and superoxide radical ( O 2 − abs ) radicals. In the presence of oxygen, the removal capacity of CFNs was improved twice than that of conventional nZVI (i.e. 453 mg/g and 263 mg/g, respectively). We inferred that Cu I in-situ generated in heterogeneous catalysis was of increasing importance and the O 2 – abs produced from the activation of dioxygen was regarded as the key factor in the generation of H 2 O 2 at pH 7. The enhancement of Cu I generation mainly because of: (i) the facial loading of Cu 0 shell accelerated the generation of Cu I , (ii) reductive Fe 0 core contributed to the regeneration of Cu I , and (iii) the generation of ferrihydrite with high specific surface area favored the adsorption of oxygen. Hence, CFNs enhanced the electron transfer between Cu I /Fe II and O 2 , increased the utilization efficiency of oxidants and improved the effectiveness of the functional nanoparticles for environmental applications.

研究领域: 环境科学 · 纳米材料科学
✓ 已验证 DOI 高影响因子
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Journal of Environmental Sciences · 2020 · IF 4.302

Degradation of organic contaminants through the activation of oxygen using zero valent copper coupled with sodium tripolyphosphate under neutral conditions

Chengwu Zhang,Lishuang Xuan,Jingyi Zhang,Fang Yuan,Xianglong Kong,Chuanyu Qin

In this study, sodium tripolyphosphate (STPP) was used to promote the removal of organic pollutants in a zero-valent copper (ZVC)/O 2 system under neutral conditions for the first time. 20 mg/L p-nitrophenol (PNP) can be completely decomposed within 120 min in the ZVC/O 2 /STPP system. The PNP degradation process followed pseudo-first-order kinetics and the degradation rate of PNP gradually increased upon the decreasing ZVC particle size. The optimal pH of the reaction system was 5.0. Our mechanism investigation showed that Cu + generated by ZVC corrosion was the main reducing agent for the activation of O 2 to produce ROS . ·OH was identified as the only ROS formed during the degradation of PNP and its production pathway was the double-electron activation of O 2 (O 2 →H 2 O 2 →·OH). In this process, STPP did not only promote the release of Cu + through its complexation, but also promoted the production of ·OH by reducing the redox potential of Cu 2+ /Cu + . In addition, we could initiate and terminate the reaction by controlling the pH. At pH < 8.1, ZVC/O 2 /STPP could continuously degrade organic pollutants; at pH > 8.1, the reaction was terminated. STPP was recycled to continuously promote the corrosion of ZVC and O 2 activation as long as the pH was <8.1. This study provided a new and efficient way for O 2 activation and organic contaminants removal.

研究领域: 环境科学 · 化学
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ACS Applied Nano Materials · 2022 · IF 6.14

Triboelectric Plasma-Catalytic CO Oxidation of MnO2 Nanostructures Driven by Mechanical Energy at Room Temperature

Xue Shi,Bao Zhang,Liangliang Liu,Yifei Zhu,Xiaochen Xiang,Sumin Li,Ke Zhao,Wanyu Shang,Guangqin Gu,Junmeng Guo,Peng Cui,Gang Cheng,Zuliang Du

The simultaneous activation of surface lattice oxygen and dioxygen is key to transition metal oxide-based catalytic CO oxidation systems. However, the reaction is difficult at room temperature owing to the high metal–oxygen bond energy. This study presents a triboelectric plasma–transition metal oxide catalytic system driven by a triboelectric nanogenerator, which realizes CO oxidation reaction at room temperature and atmospheric pressure. Among the transition metal oxides evaluated, MnO2 nanostructures exhibited an optimal CO oxidation activity of 0.24 mmol·g–1·h–1 and a low energy consumption converted per mole CO of 6.0 × 103 kJ. For the activation of both surface lattice oxygen and dioxygen, multiple reaction pathways with barriers ranging from 0.37 to 2.43 eV have been revealed by X-ray photoelectron spectroscopy, electron paramagnetic resonance, and density functional theory simulation. These catalytic reaction phenomena have been explained by an extended Mars–van Krevelen mechanism, in which multiple pathways with various barriers were overcome by the electrons in the plasma with a uniform and broad distribution probability. This work provides an efficient strategy for the conversion and utilization of mechanical energy for chemical synthesis.

研究领域: 材料科学 · 催化化学 · 能源转换
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Advanced Healthcare Materials · 2024 ·Vol. 14 ·期 1 ·2402272 · IF 10

Genetically Engineered Bacteria as A Living Bioreactor for Monitoring and Elevating Hypoxia-Activated Prodrug Tumor Therapy

Hongwei Zhang,Linfu Chen,Qian Chen,Qiufang Chen,Jun Zhou

Tirapazamine (TPZ), an antitumor prodrug, can be activated in hypoxic environment. It specifically targets the hypoxic microenvironment of tumors and produces toxic free radicals. However, due to the tumor is not completely hypoxic, TPZ often fails to effectively treat the entire tumor tissue, resulting in suboptimal therapeutic outcomes. Herein, a low pathogenic Escherichia coli TOP10 is utilized to selectively colonize tumor tissues, disrupt blood vessels, and induce thrombus formation, leading to the expansion of hypoxic region and improving the therapeutic effect of TPZ. Additionally, a thermosensitive hydrogel is constructed by Pluronic F-127 (F127), which undergoes gelation in situ at the tumor site, resulting in sustained release of TPZ. To monitor the therapeutic process, it is genetically modified TOP10 by integrating the bioluminescent system luxCDABE (TOP10-Lux). The bioluminescent signal is associated with tumor hypoxia enhancement and thrombus formation, which is beneficial for therapeutic monitoring with bioluminescence imaging. In the murine colon cancer model, the TOP10-Lux combined with TPZ-loaded F127 hydrogel effectively suppressed tumor growth, and the treatment process is efficiently monitored. Together, this work employs genetically modified TOP10-Lux to enhance the therapeutic efficacy of TPZ and monitor the treatment process, providing an effective strategy for bacteria-based tumor-targeted chemotherapy and treatment monitoring.

研究领域: 肿瘤学 · 微生物治疗 · 分子影像学 · 药物递送 · 生物材料 · 转化医学 · 合成生物学
✓ 已验证 DOI 高影响因子
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Acta Biomaterialia · 2022 · IF 10.633

Genetically engineered bacteria-mediated multi-functional nanoparticles for synergistic tumor-targeting therapy

Yaotai Wang,Yu Tang,Yan Du,Li Lin,Zhong Zhang,Xia Ou,Sheng Chen,Qi Wang,Jianzhong Zou

Focused ultrasonic ablation surgery (FUAS) for tumor treatment has emerged as an effective non-invasive therapeutic approach, but its widespread clinical utilization is limited by its low therapeutic efficiency caused by inadequate tumor targeting, single imaging modality, and possible tumor recurrence following surgery. Therefore, this study aimed to develop a biological targeting synergistic system consisting of genetically engineered bacteria and multi-functional nanoparticles to overcome these limitations. Escherichia coli was genetically modified to carry an acoustic reporter gene encoding the formation of gas vesicles (GVs) and then target the tumor hypoxic environment in mice. After E. coli producing GVs (GVs- E. coli ) colonized the tumor target area, ultrasound imaging and collaborative FUAS were performed; multi-functional nanoparticles were then enriched in the tumor target area through electrostatic adsorption. Multi-functional cationic lipid nanoparticles containing IR780, perfluorohexane, and banoxantrone dihydrochloride (AQ4N) were coloaded in the tumor to realize targeted multimodal imaging and enhance the curative effect of FUAS. AQ4N was stimulated by the tumor hypoxic environment and synergistically cooperated with FUAS to kill tumor cells. In sum, synergistic tumor therapy involving multi-functional nanoparticles mediated by genetically engineered bacteria overcomes the limitations and improves the curative effect of existing FUAS. Statement of significance Inadequate tumor targeting, single image monitoring mode, and prone tumor recurrence following surgery remain significant challenges yet critical for tumor therapy. This study proposes a strategy for genetically engineered bacteria-mediated multifunctional nanoparticles for synergistic tumor therapy. The multifunctional genetically engineered biological targeting synergistic agent can accomplish tumor-targeting therapy, synergistic FUAS ablation, hypoxia-activated chemotherapy combined with FUAS ablation, and multiple-imaging guidance and monitoring all at the same time, thereby compensating for the shortcomings of FUAS treatment. This strategy could pave the way for the progress of tumor therapy.

研究领域: 生物医学工程 · 癌症治疗 · 纳米技术 · 分子生物学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF NANOBIOTECHNOLOGY · 2023 ·Vol. 21 ·期 1 ·1-23 · IF 10.2

NIR diagnostic imaging of triple-negative breast cancer and its lymph node metastasis for high-efficiency hypoxia-activated multimodal therapy

Pan Yi,Liu Longcai,He Yichen,Ye Luyi,Zhao Xin,Hu Zhiming,Mou Xiaozhou,Cai Yu

Background Triple-negative breast cancer (TNBC) possesses special biological behavior and clinicopathological characteristics, which is highly invasive and propensity to metastasize to lymph nodes, leading to a worse prognosis than other types of breast cancer. Thus, the development of an effective therapeutic method is significant to improve the survival rate of TNBC patients. Results In this work, a liposome-based theranostic nanosystem (ILA@Lip) was successfully prepared by simultaneously encapsulating IR 780 as the photosensitizer and lenvatinib as an anti-angiogenic agent, together with banoxantrone (AQ4N) molecule as the hypoxia-activated prodrug. The ILA@Lip can be applied for the near-infrared (NIR) fluorescence diagnostic imaging of TNBC and its lymph node metastasis for multimodal therapy. Lenvatinib in ILA@Lip can inhibit angiogenesis by cutting oxygen supply, thereby leading to enhanced hypoxia levels. Meanwhile, large amounts of reactive oxygen species (ROS) were produced while IR 780 was irradiated by an 808 nm laser, which also rapidly exhausted oxygen in tumor cells to worsen tumor hypoxia. Through creating an extremely hypoxic in TNBC, the conversion of non-toxic AQ4N to toxic AQ4 was much more efficiency for hypoxia-activated chemotherapy. Cytotoxicity assay of ILA@Lip indicated excellent biocompatibility with normal cells and tissues, but showed high toxicity in hypoxic breast cancer cells. Also, the in vivo tumors treated by the ILA@Lip with laser irradiation were admirably suppressed in both subcutaneous tumor model and orthotopic tumor models. Conclusion Utilizing ILA@Lip is a profound strategy to create an extremely hypoxic tumor microenvironment for higher therapeutic efficacy of hypoxia-activated chemotherapy, which realized collective suppression of tumor growth and has promising potential for clinical translation.

研究领域: 肿瘤学 · 生物医学工程 · 药学 · 诊断成像
✓ 已验证 DOI 高影响因子
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Biomaterials Science · 2022 ·Vol. 10 ·期 9 ·2358-2369 · IF 7.59

Autocatalytic oncotherapy nanosystem with glucose depletion for the cascade amplification of hypoxia-activated chemotherapy and H2O2-dependent chemodynamic therapy

Yao Hu,Song Bai,Xingyu Fan,Fangfang Zhou,Botao Chen,Songwen Tan,Hui Xu,Anqiang Pan,Shuquan Liang,Yongju He

Employing hypoxia-activated prodrugs is an appealing oncotherapy strategy, but limited by insufficient tumor hypoxia. Moreover, a standalone prodrug fails to treat tumors satisfactorily due to tumor complexity. Herein, a nanosystem (TPZ@FeMSN-GOX) was established for triple synergetic cancer starvation therapy, hypoxia-activated chemotherapy and chemodynamic therapy (CDT). TPZ@FeMSN-GOX was prepared by synthesizing iron-doped mesoporous silica nanoparticles (FeMSNs) followed by surface conjugation with glucose oxidase (GOX), and then loading with hypoxia-activated prodrug tirapazamine (TPZ). When TPZ@FeMSN-GOX entered the tumor cells, GOX could not only exhaust glucose to starve cancer cells and concomitantly produce H2O2, but also consume O2 to aggravate the hypoxia environment and amplify TPZ-mediated chemotherapy. Meanwhile, the released Fe3+ was reduced to reactive Fe2+ by endogenous glutathione, which ultimately decomposed the produced H2O2 and endogenous H2O2 into highly toxic ˙OH, guaranteeing highly efficient CDT. Together, TPZ@FeMSN-GOX could effectively kill cancer cells and significantly inhibit tumor growth, providing a good paradigm for effective tumor treatment.

研究领域: 纳米技术 · 癌症治疗 · 药学 · 生物医学工程
✓ 已验证 DOI PubMed 高影响因子
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