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Energy Storage Materials · 2022 · IF 20.831

A bidirectional phase-transfer catalyst for Li-O2 batteries with high discharge capacity and low charge potential

Yiqiao Wang,Siyuan Pan,Yong Guo,Shichao Wu,Quan-Hong Yang

Li-O 2 batteries require catalysts to solve the problem of sluggish oxygen-related reaction kinetics. However, the solid catalysts and redox mediators are intrinsically deficient due to poor solid contacts and shuttle problems, respectively. Here, we report lithium phthalimide-N-oxyl (LiPINO) as a phase transfer catalyst (PTC) for promoting Li 2 O 2 formation and its reversible decomposition through the solution-phase reactions. The interaction between LiPINO and oxygen species in the electrolyte enables the high dissolution and stability of oxygen species, the fast charge transfer at liquid-solid interfaces and superior kinetics, and the suppressed side reactions. The efficient bidirectional catalytic activity and high stability of LiPINO capacitate batteries with a highly improved discharge capacity (11400 mAh g −1 ), a largely lowered charge potential (3.14 V) and an extended cycle life (more than 200 cycles) both in O 2 and air. Our understanding of the phase-transfer catalysis towards the Li-O 2 electrochemistry and the discovery of the PTC with superior activity and stability provide deep insights into the design of the most reliable catalysts for Li-O 2 batteries.

研究领域: 电化学 · 能源材料 · 物理化学 · 电池技术 · 催化化学
✓ 已验证 DOI 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2019 · IF 9.518

A shriveled rectangular carbon tube with the concave surface for high-performance enzymatic glucose/O2 biofuel cells

Zepeng Kang,Yi-Heng P. Job Zhang,Zhiguang Zhu

In this study, a novel carbon tube was prepared by carbonizing a rectangular polypyrrole (RPPy) tube at a high temperature for the construction of enzymatic biofuel cells with high performance. SEM and TEM images clearly showed that the initial PPy presented a rectangular tube shape, while the carbonized PPy became a shriveled rectangular tube with a concave surface, which might be beneficial for enzyme immobilization and electrochemical applications. The glucose oxidase (GOx)- or laccase (Lac)-modified electrodes based on carbonized RPPy exhibited excellent bioelectrochemical performance. In addition, a biofuel cell (GOx, glucose/O 2 , Lac) was assembled, and the open-circuit voltage reached 1.16 V. The maximum power density was measured to 0.350 mW cm −2 , which correlated to the gravimetric power density of 0.265 mW mg −1 (per mg of GOx) at 0.85 V. The constant-current discharge method was used to further evaluate the continuous discharge capacity. The discharge time reached 49.9 h at a discharge current of 0.2 mA before the voltage was lower than 0.8 V. Furthermore, three of the fabricated biofuel cells in series were able to continually light up a white light-emitting diode (LED) whose turn-on voltage was ca. 2.4 V for more than 48 h. This study suggests that carbonized conducting polymers may become a useful electrode material for the development of enzymatic biofuel cells.

研究领域: 生物化学 · 材料科学 · 能源科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Enhancement of cottonseed oil refining wastewater treatment by zero valent iron under sunlight irradiation and O2 bubbling

Chunzhen Fan,Suqing Wu,Xiangyong Zheng,Ke Bei,Shengbing He,Min Zhao

This study is the first to apply a zero-valent iron (ZVI) system in the treatment of cottonseed oil (CTO) refining wastewater. The results indicated that the ZVI system can effectively degrade and mineralize CTO in the wastewater, whereas sunlight irradiation and O 2 bubbling can considerably enhance CTO degradation, removing 93.5% of CTO and 69.0% of chemical oxygen demand within 180 min. In addition, a low concentration (0.1 mM) of S O 4 2 - and Cl − in the wastewater improved CTO degradation, whereas a high concentration (>1 mM) of these anions considerably inhibited the degradation process. However, N O 3 - at all concentrations hindered CTO degradation. Furthermore, OH and O 2 - were the main active species for CTO degradation in the ZVI system under dark conditions. However, in addition to these two species, photogenerated hole (h + ) played a key role in CTO degradation under sunlight irradiation. This observation might be derived from the photocatalytic effect due to photoexcitation of the iron corrosion product, γ-FeOOH. Our findings show that the ZVI system assisted by sunlight irradiation and O 2 bubbling is feasible for CTO-refining wastewater treatment and can guide the real wastewater treatment project.

研究领域: 环境科学 · 污水处理
✓ 已验证 DOI PubMed 高影响因子
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RSC Advances · 2018 ·Vol. 8 ·期 71 ·40984-40988 · IF 2.936

Double-ratiometric fluorescence imaging of H2Se and O2˙− under hypoxia for exploring Na2SeO3-induced HepG2 cells' apoptosis

Xiaonan Gao,Wenfei Guo,Lihong Ge,Fanpeng Kong,Kehua Xu,Bo Tang

Sodium selenite (Na2SeO3), as an anti-tumor drug for inducing tumor cells' apoptosis, has been widely studied under normoxic conditions and has been shown to exhibit oxidative stress process-induced apoptosis. However, since the real tumor environment is hypoxic, the actual mechanism is still unclear. Hence, considering the main metabolite of Na2SeO3 in the metabolic process to be hydrogen selenide (H2Se) and also that it can be converted to superoxide anion (O2˙−) instantaneously in the presence of oxygen, a dual-ratiometric fluorescence imaging system for simultaneous monitoring of the changes of H2Se and O2˙− induced by Na2SeO3-guided tumor cell apoptosis under hypoxic conditions was constructed. Two molecular probes NIR-H2Se and dihydroethidium were used to detect H2Se and O2˙−, respectively, whereas Rhodamine 110 was used as the reference fluorophore. Notably, H2Se levels significantly increased under hypoxic conditions, but there was no change in the level of O2˙−, which is inconsistent with the results of the previous researches. Therefore, we hypothesize that the mechanism of Na2SeO3-induced apoptosis for tumor cells is caused by reductive stress; also, this method can be applied for the future study of other anti-cancer selenium compounds.

研究领域: 生物化学 · 医学影像学 · 肿瘤学
✓ 已验证 DOI 高影响因子
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA · 2024 ·Vol. 121 ·期 23 ·e2320012121 · IF 9.4

PVDF–HFP@Nafion-based quasisolid polymer electrolyte for high migration number in working rechargeable Na–O2 batteries

Xin He,Youxuan Ni,Wenjiao Ma,Qiu Zhang,Zhenkun Hao,Yunpeng Hou,Haixia Li,Zhenhua Yan,Kai Zhang,Jun Chen

Rechargeable sodium-oxygen (Na–O2) battery is deemed as a promising high-energy storage device due to the abundant sodium resources and high theoretical energy density (1,108 Wh kg–1). A series of quasisolid electrolytes are constantly being designed to restrain the dendrites growth, the volatile and leaking risks of liquid electrolytes due to the open system of Na–O2 batteries. However, the ticklish problem about low operating current density for quasisolid electrolytes still hasn’t been conquered. Herein, we report a rechargeable Na–O2 battery with polyvinylidene fluoride-hexafluoropropylene recombination Nafion (PVDF–HFP@Nafion) based quasisolid polymer electrolyte (QPE) and MXene-based Na anode with gradient sodiophilic structure (M-GSS/Na). QPE displays good flame resistance, locking liquid and hydrophobic properties. The introduction of Nafion can lead to a high Na+ migration number (tNa+ = 0.68) by blocking the motion of anion and promote the formation of NaF-rich solid electrolyte interphase, resulting in excellent cycling stability at relatively high current density under quasisolid environment. In the meantime, the M-GSS/Na anode exhibits excellent dendrite inhibition ability and cycling stability. Therefore, with the synergistic effect of QPE and M-GSS/Na, constructed Na–O2 batteries run more stably and exhibit a low potential gap (0.166 V) after an initial 80 cycles at 1,000 mA g–1 and 1,000 mAh g–1. This work provides the reference basis for building quasisolid state Na–O2 batteries with long-term cycling stability.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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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.

✓ 已验证 产品关联 DOI 高影响因子
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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.

✓ 已验证 产品关联 DOI 高影响因子
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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
✓ 已验证 产品关联 DOI 高影响因子
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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.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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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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RSC Advances · 2019 ·Vol. 9 ·期 29 ·16288-16295 · IF 3.049

Metal–organic framework derived hollow porous CuO–CuCo2O4 dodecahedrons as a cathode catalyst for Li–O2 batteries

Shu-ying Zhen,Hai-tao Wu,Yan Wang,Na Li,Hao-sen Chen,Wei-li Song,Zhen-hua Wang,Wang Sun,Ke-ning Sun

Herein, hollow porous CuO–CuCo2O4 dodecahedrons are synthesized by using a simple self-sacrificial metal–organic framework (MOF) template, which resulted in dodecahedron morphology with hierarchically porous architecture. When evaluated as a cathodic electrocatalyst in lithium–oxygen batteries, the CuO–CuCo2O4 composite exhibits a significantly enhanced electrochemical performance, delivering an initial capacity of 6844 mA h g−1 with a remarkably decreased discharge/charge overpotential to 1.15 V (vs. Li/Li+) at a current density of 100 mA g−1 and showing excellent cyclic stability up to 111 charge/discharge cycles under a cut-off capacity of 1000 mA h g−1 at 400 mA g−1. The outstanding electrochemical performance of CuO–CuCo2O4 composite can be owing to the intrinsic catalytic activity, unique porous structure and the presence of substantial electrocatalytic sites. The ex situ XRD and SEM are also carried out to reveal the charge/discharge behavior and demonstrate the excellent reversibility of the CuO–CuCo2O4 based electrode.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Polymer Chemistry · 2018 ·Vol. 9 ·期 9 ·1095-1108 · IF 4.927

Thermoresponse and self-assembly of an ABC star quarterpolymer with O2 and redox dual-responsive Y junctions

Xiaoqi Zhao,Wentao Wu,Jian Zhang,Wenxue Dai,Youliang Zhao

Multicomponent miktoarm stars with multifunctional Y junctions may provide us with new insights into their physicochemical properties and prospective applications. Considering the unique role of a gas stimulus in smart materials and the promising gradient-type properties induced by combined stimuli, this study aims at the synthesis, thermoresponsive and self-assembly behaviors of an O2-, redox-, thermo-, and pH-responsive 3-miktoarm star quarterpolymer. A robust method involving controlled polymerization, amine–thiol–ene conjugation and hydrolysis was developed to achieve a poly(N-isopropylacrylamide-co-4-(2-(2,2,2-trifluoroethylcarbamoyl)ethylthio)-2-(acrylamido)-N-(2-hydroxyethyl)butanamide)-arm-poly(ε-caprolactone)-arm-poly(acrylic acid) star. Owing to the changes in amphiphilicity, chemical composition and mutual interactions, a single stimulus or various stimuli combinations could lead to switchable LCSTs and morphological transformations. Upon increasing pH, O2 treatment and oxidation, the copolymer solution was liable to exhibit enhanced LCST due to the improved hydrophilicity. The star quarterpolymer could self-assemble into multicompartment vesicles (pH 3.0), vesicles (pH 5.9) and small micelle/vesicle mixtures (pH 10) at ambient temperature. Upon thermo, redox and O2 stimuli, the assemblies formed at different pHs could be further converted into some other morphologies such as compound micelles and nanocapsules with hollow caves. Our research affords a general route to synthesize MMSs with tailored Y junctions, and the combination of the O2 stimulus with other stimuli may potentially expand the scope of multi-triggered properties and applications of star copolymers.

CAS / MDL: 814-68-6 6038-19-3
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