Nature Catalysis
·
2019
·Vol. 2
·期 11
·1035-1044
·
IF 0
Qiao Yu,Jiang Kezhu,Deng Han,Zhou Haoshen
Li–O 2 batteries have received considerable attention owing to their high theoretical gravimetric energy densities. However, the sluggish kinetic barrier between gaseous O 2 and solid products leads to severe polarized overpotenial. Besides, the gas-open cell architecture and cumbrous O 2 storage accessories bring additional burdens on practical application. Here, by pre-embedding Li 2 O nanoparticles into an iridium–graphene catalytic host, we confine the O 2 -free reversible Li 2 O/Li 2 O 2 interconversion within a sealed cell environment. After rationally controlling the depth of charge, the O 2 /superoxo-free charge capacity can be extended to 400 mAh g –1 (based on the entire cathodic loading mass), with only 0.12 V round-trip overpotential. Ultrastable rechargeability can be achieved for over 2,000 cycles with 99.5% coulombic efficiency. Moreover, matched with a silicon anode, the full-cell output gravimetric energy density can reach nearly 600 Wh kg –1 (based on the loading mass of both electrodes). This work shows that reversible oxide–peroxide conversion can be utilized for the development of high-energy-density sealed battery technologies.
研究领域:
材料科学
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电化学
·
能源存储
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DOI
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Chengwu Zhang,Chuipeng Kong,Paul G. Tratnyek,Chuanyu Qin
Tripolyphosphate (TPP) has many advantages as a ligand for the optimization of the Fe2+/O2 system in environmental remediation applications. However, the relationship between remediation performance and the Fe2+/TPP ratio in the system has not been previously described. In this study, we report that the degradation mechanism of p-nitrophenol (PNP) in Fe2+/O2 systems is regulated by the Fe2+/TPP ratio under neutral conditions. The results showed that although PNP was effectively degraded at different Fe2+/TPP ratios, the results of specific reactive oxygen species (ROS) scavenging experiments and the determination of PNP degradation products showed that the mechanism of PNP degradation varies with the Fe2+/TPP ratio. When CFe2+ ≥ CTPP, the initially formed O2•– is converted to •OH and the •OH degrades PNP by oxidation. However, when CFe2+ < CTPP, the O2•– persists long enough to degrade PNP by reduction. Density functional theory (DFT) calculations revealed that the main reactive species of Fe2+ in the system include [Fe(TPP)(H2O)3]− and [Fe(TPP)2]4–, whose content in the solution is the key to achieve system regulation. Consequently, by controlling the Fe2+/TPP ratio in the solution, the degradation pathways of PNP can be selected. Our study proposed a new strategy to regulate the oxidation/reduction removal of pollutants by simply varying the Fe2+/TPP ratio of the Fe2+/O2 system.
研究领域:
环境科学
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化学工程
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材料科学
·
计算化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yong Chen,Zhao Yang,Yunbo Liu,Yong Liu
In this paper, a novel Fenton-like system was constructed by a new catalyst (CNTs-Fe-Cu) combined with Al 0 -CNTs to in situ generate H 2 O 2 from activating O 2 for the degradation of sulfamerazine (SMR). The CNTs-Fe-Cu composite was prepared and characterized by XRD, SEM, EDS and BET methods. The results showed that H 2 O 2 could be generated in-situ by Al 0 -CNTs composite under oxygen aeration, which was then converted to OH and O 2 − radical by CNTs-Fe-Cu composite. The high removal efficiency of SMR could be obtained in Al 0 -CNTs/CNTs-Fe-Cu/O 2 system at a relatively broad range of pH. Furthermore, the removal efficiency of SMR and total organic carbon (TOC) was 85% and 60%, respectively under the following condition: initial pH = 5.8, T = 25 °C, O 2 flow rate = 400 mL/min, CNTs-Fe-Cu = 1 g/L, Al 0 -CNTs = 1 g/L, SMR = 50 mg/L, reaction time = 60 min. In addition, the intermediate products of SMR degradation were identified and the possible degradation pathways of SMR and the degradation mechanism of Al 0 -CNTs/CNTs-Fe-Cu/O 2 process were tentatively proposed.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Kailing Sun,Mingrui Liu,Siyan Yu,Huiyu Song,Jianhuang Zeng,Xiuhua Li,Shijun Liao
The Li–O 2 battery is one of the most promising next-generation energy storage systems due to its super-high theoretical energy density . However, its further development is impeded by the current cathode system, which exhibits low energy efficiency and poor cycling stability. Herein, we report a composite of vanadium nitride coated with nitrogen-doped carbon nanoribbons grown in situ on carbon paper (denoted as VN@C) as a novel binder-free cathode for Li–O 2 batteries. We find that the nitrogen-doped carbon coating can significantly improve the stability of VN and enhance the composite's ORR/OER activities. The Li–O 2 batteries with our optimal VN@C-850 cathodes achieve an initial discharge capacity of 8269 mA h g −1 , a discharge-charge voltage gap of 0.88 V, and considerable cycling stability for 183 cycles with a cut-off capacity of 1000 mA h g −1 , compared with 2027 mA h g −1 , 1.21 V, and 12 cycles with uncoated VN cathodes.
研究领域:
电化学
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能源材料
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纳米材料
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电化学储能
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先进电池技术
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Shiyi Li,Jie Zhang,Bei Liu,Wanchao Hu,Changli Lü
Solar-driven photocatalytic H 2 O 2 production presents a sustainable alternative to the industrial anthraquinone process. An in situ anthraquinone (AQ) functionalized metal–organic framework (UiO-66-F 4 ) with fluorinated linkers enables efficient concurrent synthesis of H 2 O 2 and value-added benzaldehyde (BzH) in a two-phase system. The AQ-modified F-MOF achieves exceptional H 2 O 2 production rates of 118.1mmol g -1 h −1 under visible light and 328.2mmol g -1 h −1 under simulated sunlight, along with high BzH selectivity (∼95%). Fluorinated linkers and AQ act synergistically to enhance the built-in electric field, promote charge separation, and facilitate oxygen adsorption and activation. RDE and RRDE studies verify a highly selective two-electron oxygen reduction pathway (94% H 2 O 2 selectivity) and reveal a non-traditional mechanism involving energy transfer to form electrophilic 1 O 2 , which is subsequently reduced to •O 2 – by electron and protonated to H 2 O 2 . Both experimental and theoretical results demonstrate that the 1 O 2 mediated pathway proceeds with a lower free energy barrier compared to the molecular oxygen route. Meanwhile, the incorporation of AQ reduces the oxygen adsorption energy and provides additional adsorption sites, further enhancing photocatalytic H 2 O 2 production. EPR spectroscopy corroborates the interconversion between 1 O 2 and •O 2 – during the reaction. This work offers mechanistic insight into the coexistence and interconversion of reactive oxygen species, while demonstrating spontaneous separation and collection of both H 2 O 2 and high-value oxidation products in a two-phase system.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ruo-Yun Zhang,Kai Cheng,Xing Sun,Xiao-Quan Yang,Yong Li,Yong-Guo Hu,Xiao-Shuai Zhang,Bo Liu,Wei Chen,Yuan-Di Zhao,Dong-Sheng Huang
Colorectal cancer is one of the most common intestinal tumors, of which occurrence and development are closely related to immune escape activity in vivo . Then, how to comprehensively block immune escape remains a big challenge for immunotherapy. Thus, a biomimetic nanoprobe [email protected] /hybrid membrane/PA ( [email protected] ) is designed by coating Ce6 loaded ZIF-8 with a hybrid membrane composed of neutrophil membrane (Nm) & red blood cell membrane (Rm), accompanied by palmitoyl ascorbate (PA) to achieve reprogramming of immunosuppressive tumor microenvironment (TME) and enhancement of sonodynamics therapy (SDT) in hypoxic tumor. Cell and animal experiments indicate that, the [email protected] probe can specifically target tumor at the inflammatory site, and it can effectively reduce the adsorption of neutrophils, then inhibit the polarization toward immunosuppressive M2 macrophage phenotype. Immunofluorescence staining and ELISA experiments demonstrate that PA and Rm can generate O 2 and significantly improve the hypoxic environment, it enhances the polarization of anti-tumor M1 macrophages and regulate related cytokines, meanwhile improves the therapeutic effect of SDT. The survival rate of mice is elevated to 100% within 60 d. Overall, this O 2 self-generated biomimetic hybrid membrane nanoprobe can block immune escape from various aspects and obtain enhanced SDT effect, then increase the treatment efficiency of inflammatory tumor, significantly improve the prognosis and elevate the survival rate of mice, providing a new idea for the clinical diagnosis and treatment of colitis-associated tumors.
研究领域:
癌症研究
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纳米技术
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免疫治疗
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生物医学工程
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DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Jun-Min Zhang,Xiao-Wu Chen,Xiao You,Qing-Gang Li,Meng-Meng Wang,Xiang-Yu Zhang,Yan-Mei Kan,Yu-Dong Xue,Shao-Ming Dong
The effect of RE 2 O 3 (RE = La, Y, Er, Lu) on the oxidation behavior of RMI-SiC ceramics in air and wet oxygen atmospheres at 1400 °C were studied. The outward migration of RE 3+ cations reduces the oxidation resistance of SiC-RE ceramics in air, but improves the wet-oxidation resistance of SiC-RE ceramics due to the formation of denser RE 2 Si 2 O 7 layer. The outward migration rates of RE 3+ cations may be influenced jointly by the RE 3+ cation radius and the formation rate of RE 2 Si 2 O 7 . The higher mobility of Er 3+ and Y 3+ cations makes Y 2 O 3 and Er 2 O 3 promising modifier for enhancing the wet-oxidation resistance of RMI-SiC f /SiC composites, although the modified components need to be optimized and further analyzed in a more realistic service environment.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·
IF 2.8
Yan Jiaqi,Chen Gui,Lu Sihang,Wang Pin,Hu Zhengwu,Chen Wenkai,Yuan Ye
In this work, a stable bimetallic hydrotalcite-derived NiCu/MgAlO catalyst and O 2 as oxidant were used for the toluene oxidation to produce the valuable benzyl alcohol (PhCH 2 OH) and benzaldehyde (PhCHO) under solvent-free and additive-free conditions. This strategy gave 7.2% toluene conversion with 70.7% selectivity to PhCH 2 OH & PhCHO. Multiple characterizations showed that highly dispersed metallic Cu and Ni were anchored on the support surface and a chemical bonding interaction occurred between the metallic Ni and the MgAlO. The metal–support interaction contributed to the formation of active Ni 0 species and NiCu alloy with abundant oxygen defects, resulting in excellent catalytic activity and acceptable stability. A plausible reaction mechanism for the catalytic oxidation of toluene over NiCu/MgAlO catalyst has been proposed. The attractive feature of the present catalytic oxidation system compared to conventional methods was its ability to achieve high selectivity for the desired target product. The further advantage of NiCu/MgAlO catalyzed toluene oxidation was that the reaction temperature and time could be below 180 °C and 2 h, thereby minimizing energy consumption and reducing effluent wastewater, which has potential application prospects.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Jingbo Yang,Hongwei Mi,Shan Luo,Yongliang Li,Peixin Zhang,Libo Deng,Lingna Sun,Xiangzhong Ren
Flexible Li-O 2 batteries have attracted worldwide research interests and been considered to be potential alternatives for the next-generation flexible devices. Nitrogen-doped carbon nanofibers (N-CNFs) prepared by electrospinning are used as flexible substrate and an amorphous TiO 2 layer is coated by atomic layer deposition (ALD) and then decorated with Ru nanoparticles . The Ru/N-CNFs@TiO 2 composite is directly used as a free-standing electrode for Li-O 2 batteries and the electrode delivers a high specific capacity, improved round-trip efficiency and good cycling ability. The superior electrochemical performance can be attributed to the amorphous TiO 2 protecting layer and superior catalytic activity of Ru nanoparticles. Based on density functional theory (DFT) calculations from first principles, the carbon electrode after coating with TiO 2 is more stable during discharge/charge process. The analysis of Li 2 O 2 on three different interfaces (Li 2 O 2 /N-CNFs, Li 2 O 2 /TiO 2 , and Li 2 O 2 /Ru) indicates that the electron transport capacity was higher on Ru and TiO 2 compared with N-CNFs, therefore, Li 2 O 2 could be formed and decomposed more easily on the Ru/N-CNFs@TiO 2 cathode. This work paves a way to develop the free-standing cathode materials for the future development of high-performance flexible energy storage systems .
研究领域:
材料科学
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电化学
·
理论计算
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产品关联
DOI
高影响因子
BIOMEDICAL CHROMATOGRAPHY
·
2020
·Vol. 34
·期 8
·e4852
·
IF 1.728
Jing Wang,Yong Zhang,Meiqi Zhou,Meizhu Zheng,Jing Cui,Zhiqiang Liu,Chunming Liu,Shu Liu
Superoxide anion radical scavenger and xanthine oxidase inhibitor play an important role in the treatment of several relevant human diseases. In the present study, ultrafiltration liquid chromatography–mass spectrometry coupled to microplate reader was applied to screen and identify superoxide anion radical scavengers and xanthine oxidase inhibitors from total flavonoids of Ginkgo biloba leaves. As a result, four compounds (quercetin, apigenin, kaempferol and isorhamnetin) were screened as xanthine oxidase inhibitors by ultrafiltration LC–MS, and the 50% scavenging concentration values of the screened flavonoids were lower than those for allopurinol. Lineweaver–Burk plot results indicated that kaempferol was a competitive xanthine oxidase inhibitor; the other flavonoids were all anticompetitive inhibitors. Four flavonoids—rutin, quercetin, kaempferol and isorhamnetin—were screened as superoxide anion radical scavengers by LC–MS. The results demonstrate that the method for screening and evaluation of superoxide anion radical scavenger and xanthine oxidase inhibitor from a complex mixture system is feasible and efficient.
研究领域:
药理学
·
分析化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiayu Xiao,Luo Hai,Ke Yang,Yuze Luo,Zefeng Wang,Junqin Li,Chunlei Ou,Li Wang,Le Deng,Dinggeng He
Reactive oxygen species (ROS) such as hydroxyl radicals ( OH) and singlet oxygen ( 1 O 2 ) have emerged as promising therapeutic agents for combating biofilm-associated bacterial infections. However, the hypoxic microenvironments in the biofilms severely hinder the ROS production. Herein, we have rationally integrated copper peroxide (CP) and indocyanine green (ICG) into a polydopamine (PDA) nanoparticle to construct a versatile hybrid nanoplatform (PDA/CP/ICG), which can enhance ROS generation for highly efficient biofilm elimination by relieving hypoxic microenvironment. When the PDA/CP/ICG accumulates at the infection site or biofilm, the acidic microenvironment triggers the co-release of Cu 2+ and H 2 O 2 , and the former can catalyze the conversion of self-supplied H 2 O 2 into OH via a Fenton-like reaction and consume the overexpressed antioxidant glutathione (GSH) to further promote the oxidative stress. Moreover, with the help of an 808 nm laser, the hyperpyrexia caused by PDA induces the decomposition of CP into O 2 that is immediately converted by ICG into 1 O 2 . The PDA/CP/ICG shows satisfactory antibacterial and antibiofilm effect due to the self-amplified production of OH and 1 O 2 , and outstanding wound healing with good in vivo biosafety. Overall, this study provides a facile paradigm in ROS-based biofilm elimination, and the proposed hypoxia-irrelevant bactericidal nanoplatform has great potential for future biomedical applications.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Pei-Pei Luo,Xin-Ke Zhou,Yu Li,Tong-Bu Lu
Solar energy-driven direct CH4 conversion to liquid oxygenates provides a promising avenue toward green and sustainable CH4 industry, yet still confronts issues of low selectivity toward single oxygenate and use of noble-metal cocatalysts. Herein, for the first time, we report a defect-engineering strategy that rationally regulates the defective layer over TiO2 for selective aerobic photocatalytic CH4 conversion to HCHO without using noble-metal cocatalysts. (Photo)electrochemical and in situ EPR/Raman spectroscopic measurements reveal that an optimized oxygen-vacancy-rich surface disorder layer with a thickness of 1.37 nm can simultaneously promote the separation and migration of photogenerated charge carriers and enhance the activation of O2 and CH4, respectively, to •OH and •CH3 radicals, thereby synergistically boosting HCHO production in aerobic photocatalytic CH4 conversion. As a result, a HCHO production rate up to 3.16 mmol g–1 h–1 with 81.2% selectivity is achieved, outperforming those of the reported state-of-the-art photocatalytic systems. This work sheds light on the mechanism of O2-participated photocatalytic CH4 conversion on defective metal oxides and expands the application of defect engineering in designing low-cost and efficient photocatalysts.
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DOI
PubMed
高影响因子
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