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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Visible-light-driven H2O2 production from O2 reduction with nitrogen vacancy-rich and porous graphitic carbon nitride

Yanbin Wang,Di Meng,Xu Zhao

Visible-light-driven H 2 O 2 production from O 2 reduction is an eco-friendly strategy and attracts increasing attentions. In this study, KOH modified graphitic carbon nitrides (CNKx) were constructed through the thermolysis of melamine-cyanuric acid supramolecular-complex in the presence of KOH. The BET specific surface area of CNK 0.2 with porous structure was 92 m 2  g −1 . The photocatalyst was characterized by XPS, ESR and element analysis and the analysis suggested that nitrogen vacancy was created in the framework of g-C 3 N 4 . Photoluminescence (PL) spectra indicated that the recombination of photogenerated electrons and holes was efficiently suppressed. ζ-potential revealed that more negative charge on the surface of CNK 0.2 , which promoted the adsorption of O 2 and accelerated the photocatalytic H 2 O 2 production. ESR experimental and radical quenching results illustrated that superoxide radical (O 2 - ) was the primary intermediate during the O 2 reduction process, suggesting the O 2 reduction pathway by CNK 0.2 was the sequential two-step single-electron reduction.

CAS / MDL: 3317-61-1
研究领域: 材料科学 · 环境科学 · 光催化
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Preparation and properties of (Ce0.2Zr0.2Ti0.2Sn0.2Y0.2-xCax)O2-δ (x=0∼0.2) high-entropy of compositionally-complex ceramics

Siyuan Li,Cuiwei Li,Huaiming Jia,Guangjin Chen,Kepi Chen,Linan An

In this paper, a series of (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Y 0.2- x Ca x )O 2-δ ( x  = 0∼0.2) high-entropy of compositionally-complex ceramics were prepared using solid-state reaction method. The results showed that the content of Ca 2+ had significant effects on the phase composition, microstructure and properties of the prepared materials. As Ca 2+ content increased, single-phase fluorite was easier to form. When x  ≤ 0.05, materials contained dual-phase of fluorite and pyrochlore structures. When x  ≥ 0.075, the prepared materials showed single-phase fluorite structure, which indicated that high-entropy fluorite ceramics (HEFCs) could be prepared under this condition. When Ca 2+ content increased from 0.075 to 0.2, grain size of HEFCs decreased, and relative density decreased from 95.7 % to 78.6 %. Thermal conductivity of these HEFCs varied from 1.87 W m −1  K −1 to 1.60 W m −1  K −1 , which was lower than 8YSZ. As Ca 2+ content increased, both size disorder and mass disorder increased too leading to low thermal conductivity. The results indicate that the prepared HEFCs are promising for thermal insulation applications.

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Frontiers in Bioengineering and Biotechnology · 2023 · IF 5.7

H2O2/O2 self-supply and Ca2+ overloading MOF-based nanoplatform for cascade-amplified chemodynamic and photodynamic therapy

Yujia Liang,Zhengmin Cai,Yamei Tang,Chenglin Su,Liye Xie,Yan Li,Xinqiang Liang

Introduction: Reactive oxygen species (ROS)-mediated therapies have typically been considered as noninvasive tumor treatments owing to their high selectivity and efficiency. However, the harsh tumor microenvironment severely impairs their efficiency. Methods: Herein, the biodegradable Cu-doped zeolitic imidazolate framework-8 (ZIF-8) was synthesized for loading photosensitizer Chlorin e6 (Ce6) and CaO 2 nanoparticles, followed by surface decoration by hyaluronic acid (HA), obtaining HA/CaO 2 -Ce6@Cu-ZIF nano platform. Results and Discussion: Once HA/CaO 2 -Ce6@Cu-ZIF targets tumor sites, the degradation of Ce6 and CaO 2 release from the HA/CaO 2 -Ce6@Cu-ZIF in response to the acid environment, while the Cu 2+ active sites on Cu-ZIF are exposed. The released CaO 2 decompose to generate hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), which alleviate the insufficiency of intracellular H 2 O 2 and hypoxia in tumor microenvironment (TME), effectively enhancing the production of hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) in Cu 2+ -mediated chemodynamic therapy (CDT) and Ce6-induced photodynamic therapy (PDT), respectively. Importantly, Ca 2+ originating from CaO 2 could further enhance oxidative stress and result in mitochondrial dysfunction induced by Ca 2+ overloading. Conclusion: Thus, the H 2 O 2 /O 2 self-supplying and Ca 2+ overloading ZIF-based nanoplatform for cascade-amplified CDT/PDT synergistic strategy is promising for highly efficient anticancer therapy.

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FUEL · 2023 · IF 7.4

“On-off”controlled H2 evolution and O2 evolution upon NH3BH3 hydrolysis resp·H2O2 decomposition on Pt/ZIF-67

Qi Rong,Wenkai Huang,Fuhua Xu,Yanlan Wang,Changlong Wang,Xiang Liu

In spite of significant developments are accomplished in the exploration of H 2 and O 2 evolution upon water electrolysis/photolysis, this remains a challenge to design and develop ideal catalytic systems for this reaction and to isolate H 2 from H 2 -O 2 mixture with membranes. Herein, a series of ZIF-67-supported transition metal nanoparticles (TMNPs/ZIF-67), including Pt, Ir, Pd, Rh, Au and Ag, via immobilization of ultrafine TMNPs at the surface of ZIF-67, have been designed and developed for the selective H 2 generation from NH 3 BH 3 hydrolysis and O 2 evolution upon H 2 O 2 decomposition. In particular, the optimized nanocatalyst Pt/ZIF-67 presents the super-high catalytic property in the both H 2 evolution upon NH 3 BH 3 hydrolysis (689 mol(H 2 )·mol Pt -1 ·min −1 ) and O 2 evolution upon H 2 O 2 decomposition (979 mol(O 2 )·mol Pt -1 ·min −1) at 30 °C. Importantly, the selective “on–off” control for demand-based H 2 generation from NH 3 BH 3 hydrolysis was successfully realized by Zn 2+ /EDTA-2Na system. This highly efficient Pt/ZIF-67 proposed a new method for the promising potential application of ammonia borane and hydrogen peroxide as an economic and safe H 2 resp. O 2 carrier for fuel cell.

CAS / MDL: 13774-81-7 13454-96-1
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2023 · IF 5.8

Multifunctional barrier membranes promote bone regeneration by scavenging H2O2, generating O2, eliminating inflammation, and regulating immune response

Shuo Liu,Huiqi Yang,Liguo Zhang,Alberto Bianco,Baojin Ma,Shaohua Ge

The injured bone microenvironment is typically characterized by high-level reactive oxygen species (ROS, mainly H 2 O 2 ) and low content of oxygen. The former can cause cell apoptosis, induce immune imbalance and inflammation, inhibit osteogenic differentiation, and delay bone repair . In this work, barrier membranes made of a combination of hydroxyapatite nanowires (HAp NWs) and polylactic acid (PLA) loaded with manganese dioxide nanosheets (NSs) ( [email protected] ) were prepared to guide bone regeneration (GBR). Due to the catalytic function of MnO 2 , [email protected] membranes are able to effectively decompose H 2 O 2 to generate O 2 . In vitro experiments demonstrated [email protected] membranes inhibited the apoptotic process caused by high level of H 2 O 2 , decreased intracellular oxidative stress , suppressed inflammation-related gene/protein expression, and inhibited macrophage M1 polarization. The nanostructured HAp stimulated osteogenic differentiation, and the loading of MnO 2 NSs played a synergistic effect. In addition, the barrier function of PLA could hamper the epithelium overgrowth, providing the development space for periodontal regeneration. By scavenging H 2 O 2 , generating O 2 , eliminating inflammation, and regulating immune response, [email protected] membranes efficiently promoted bone regeneration. Our results confirmed that composite membranes have great potential for application in GBR, and provide a reference for future design of bone repair materials.

CAS / MDL: 7722-64-7
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Oxygen-rich hierarchical activated coke-based gas diffusion electrode enables highly efficient H2O2 synthesis via O2 electroreduction

Wei Zhou,Liang Xie,Yan Wang,Yani Ding,Xiaoxiao Meng,Fei Sun,Jihui Gao,Guangbo Zhao

Large-scale application of H 2 O 2 production through 2-electron oxygen reduction reaction (2eORR) greatly depends on the cost of electrode materials and configuration. In this work, engineered coal-derived oxygen-rich hierarchical activated coke (AC), which is low-cost and highly tunable in porosity and surface chemistry, was used as catalyst to fabricate gas diffusion electrodes (GDEs) for efficient H 2 O 2 production. Results showed that Fenton’s reagents treatment could significantly increase the contents of C O and –COOH on AC, leading to an increased hydrophilicity. However, the higher O contents do not necessarily enhance the selectivity of AC towards 2eORR (i.e., F-5-AC, F-10-AC), especially that F-20-AC exhibited a complete 4e pathway. GDEs were then fabricated with AC and oxidized AC as catalyst, key fabrication parameters including the PTFE binder and AC particle size, and operating parameters such as current intensity, electrolyte pH, and O 2 flow rate were optimized. Up to 747 mg/L H 2 O 2 were generated within 90 min. Results showed that oxidized AC exhibited a decreased H 2 O 2 yield, due to the flooding of GDEs caused by super-hydrophilicity property. Finally, DFT calculations were employed to reveal the synergistic effect of different O groups considering the fact of high O contents on AC.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

α-Fe2O3 nanospindles as an efficient catalyst for optical and magnetic fields co-assisted Li-O2 cells

Daming Yang,Guiru Sun,Xinru Wang,Fengyang Li,Ze Gao,Pingli Zhang,Wei Lu,Ming Feng

The photo-assisted lithium-oxygen (Li-O 2 ) cell is widely concerned due to its low overpotential. However, rapid recombination rate of photogenerated electrons and holes remains a fundamental challenge for photo-assisted Li-O 2 cells. Herein, we design an optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles. We employed PL spectrum and I-t curve confirm that under the magnetic field, the photogenerated electrons and holes are driven via the opposite Lorentz forces in photo-assisted Li-O 2 cells, which is beneficial to accelerating the formation and decomposition of Li 2 O 2 . The optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles achieves an ultra-high discharge platform of 3.47 V and a low charge platform of 3.57 V, as well as a surprising energy efficiency of 97.2%. In addition, the optical and magnetic fields co-assisted Li-O 2 cell can stably cycle for over 25 cycles. This study offers a reference for improving the electrochemical kinetics of photo-assisted Li-O 2 cell by introducing magnetic field, which opens up a new avenue for the development of high-performance Li-O 2 cells.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2023 · IF 4.5

Co nanoparticles embedded into leaf-like porous carbon as a promising cathode catalyst for Li-O2 batteries

Chaoyang Sun,Fenglong Xiao,Di Wu,Gang Lian,Deliang Cui,Qilong Wang,Haohai Yu

Rechargeable Li-O 2 batteries show great potential due to their superior high energy density. However, the practical application is still limited by the sluggish kinetics, resulting in poor cycling performance and high overpotentials. Herein, highly dispersed Co nanoparticles embedded into porous N -doped carbon matrix (DCo-NC) with carbon nanotubes is explored through the pyrolysis of a bimetallic leaf-shaped ZnCo-ZIFs. The evaporation of Zn species and porous carbon matrix derived from ZIFs prevents the Co nanoparticles aggregation, exposes more Co-N active sites and provides abundant pores. They facilitate Li + and electron transfer, prevent Co nanoparticles from deactivation and provide enough space for Li 2 O 2 , thereby accelerating oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) kinetics. Accordingly, the Li-O 2 batteries with DCo-NC cathode exhibit reduced overpotential, high discharge capacity (10,490 mA h g −1 at 100 mA g −1 current density) and improved cycling performance (258 cycles at 500 mA g −1 with a limited capacity of 500 mA h g −1 , 103 cycles at 500 mA g −1 with a limited capacity of 1000 mA h g −1 ).

CAS / MDL: 10026-22-9 693-98-1
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Small · 2022 ·Vol. 18 ·期 23 ·2200548 · IF 15.153

Au3+-Functionalized UiO-67 Metal-Organic Framework Nanoparticles: O2•− and •OH Generating Nanozymes and Their Antibacterial Functions

Meng-Meng Pan,Yu Ouyang,Yong-Li Song,Lu-Qin Si,Ming Jiang,Xu Yu,Li Xu,Itamar Willner

The synthesis and characterization of Au 3+ -modified UiO-67 metal-organic framework nanoparticles, Au 3+ -NMOFs, are described. The Au 3+ -NMOFs reveal dual oxidase-like and peroxidase-like activities and act as an active catalyst for the catalyzed generation of O 2 •− under aerobic conditions or •OH in the presence of H 2 O 2 . The two reactive oxygen species (ROS) agents O 2 •− and •OH are cooperatively formed by Au 3+ -NMOFs under aerobic conditions, and in the presence of H 2 O 2. The Au 3+ -NMOFs are applied as an effective catalyst for the generation ROS agents for antibacterial and wound healing applications. Effective antibacterial cell death and inhibition of cell proliferation of Staphylococcus aureus ( S. aureus ) and Escherichia coli ( E . coli ) bacterial colonies are demonstrated in the presence of the Au 3+ -NMOFs. In addition, in vivo experiments demonstrate effective wound healing of mice wounds infected by S. aureus , treated by the Au 3+ -NMOFs.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Multifunctional hydrogel platform for biofilm scavenging and O2 generating with photothermal effect on diabetic chronic wound healing

Qian Wang,Weiwang Qiu,Mengna Li,Na Li,Xiaoran Li,Xiaohong Qin,Xueli Wang,Jianyong Yu,Faxue Li,Liqian Huang,Dequn Wu

Diabetic wound treatment remains a major challenge due to the difficulties of eliminating bacterial biofilm and relieving wound hypoxia . To address these issues simultaneously, a multifunctional Dex-SA-AEMA/MnO 2 /PDA (DSAMP) hydrogel platform was developed with excellent biocompatibility and porous structure. The hydrogel could absorb the exudate, maintain humidity and permeate oxygen, which was prepared by encapsulating polydopamine (PDA) and manganese dioxide (MnO 2 ) into Dex-SA-AEMA (DSA) hydrogel by UV irradiation . With the addition of PDA , the DSAMP hydrogel was proved to eliminate the biofilm after NIR photodynamic therapy (PTT, 808 nm) irradiation at 54 °C. Furthermore, in order to mitigate hypoxia wound microenvironment, MnO 2 nanoparticles were added to convert the endogenous hydrogen peroxide (H 2 O 2 ) into oxygen (O 2 , 16 mg L −1 ). The diabetic wound in vivo treated by DSAMP hydrogel was completely healed on 14 days. It was revealed that the DSAMP hydrogel possessed a great potential as dressing for diabetic chronic wound healing.

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BIOELECTROCHEMISTRY · 2022 · IF 5.76

Involvement of O2·− release in zearalenone-induced hormesis of intestinal porcine enterocytes: An electrochemical sensor-based analysis

Yanjing Yun,Zhisong Lu,Xiaodan Jiao,Peng Xue,Wei Sun,Yan Qiao,Yang Liu

Relationship between mycotoxin-induced hormesis and reactive oxygen species (ROS) has not been systematically investigated due to the lack of an effective analysis method. To monitor cellular release and intracellular level of O 2 ·− , carboxymethyl cellulose-Mn 3 (PO 4 ) 2 nanocomposite was synthesized to fabricate an electrochemical biosensor, which selectively detects O 2 ·− over the range of 57.50 nM ∼ 2.95 μM (R 2  = 0.99) with the sensitivity of 78.67 μA μM −1 cm −2 and the detection limit of 8.47 nM. Transient exposure to zearalenone (ZEA) induces the enhancement on cell viability, immediate O 2 ·− release from cells, and reduction of intracellular O 2 ·− level. After post-treatment culture, intracellular O 2 ·− initially increases to a high level and then decreases to the normal level. Concurrently, the ZEA-induced hormesis disappears. Based on the findings, we propose a mechanism, involving the ROS release, increase of succinate dehydrogenase activity and recovery of intracellular ROS, to explain the occurrence and disappearance of hormesis in intestinal porcine enterocytes.

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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

PIM-1 mixed matrix membranes incorporated with magnetic responsive cobalt-based ionic liquid for O2/N2 separation

Hongyong Zhao,Ting Song,Xiaoli Ding,Ruyi Cai,Xiaoyao Tan,Yuzhong Zhang

Membrane technology for O 2 /N 2 separation is a mature industrial unit. Membranes with excellent permeation-separation performance are still one of the critical requirements. The cobalt-based compounds have been well known for their good affinity for O 2 , which can facilitate O 2 transfer and improve the O 2 /N 2 selectivity in membranes. The cobalt-based compounds, moreover, have a magnetic responsive effect, which can lead to a further improvement in O 2 /N 2 separation under a magnetic field. A class of PIM-1 mixed matrix membranes (MMMs), containing cobalt-based ionic liquid (CILs)@polyarylate (aromatic polyester) (PAR) (core-shell) composite nanospheres (CILs@PAR (c-s) CNPs), were prepared. Chemical compositions of CILs@PAR (core-shell) CNPs were determined by Fourier transform infrared spectroscopy (FTIR). Morphologies and structures of CILs@PAR (core-shell) CNPs were observed by transmission electron microscopy (TEM). Gas adsorption properties of CILs@PAR (core-shell) CNPs were tested. Thermal properties of the (CILs@PAR (c-s) CNPs)/PIM MMMs were investigated by simultaneous thermal analysis (TGA-DSC). Gas permeation-separation performances of the (CILs@PAR (c-s) CNPs)/PIM MMMs were also reported. Compared with the original PIM-1 membrane, the (CILs@PAR (c-s) CNPs)/PIM MMMs display higher O 2 /N 2 selectivity because of cobalt-based ionic liquid as O 2 carrier, coupled with a reduction in O 2 permeability. With increasing the content of the CILs@PAR (c-s) CNPs, the O 2 /N 2 selectivity increases, and the O 2 permeability decreases. It is also found that, as a magnetic field on the MMMs, the O 2 /N 2 selectivity further increases; and it increases more, as a higher content of CILs@PAR (c-s) CNPs. Therefore, the (CILs@PAR (c-s) CNPs)/PIM MMMs exhibit excellent O 2 /N 2 selectivity of ∼5 coupled with good O 2 permeability of ∼140 Barrer under a 180 mT magnetic field and show great potential for air separation.

CAS / MDL: 554-95-0
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