ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Rouyan Guo,Congcong Dang,Yiping Liu,Guangqi Zhang,Lingti Kong,Liancheng Zhao,Liming Gao
Developing an efficient and highly catalytic cathode is crucial to the advancement of rechargeable Li-O 2 batteries for utilizing their high theoretical energy density. However, due to the sluggish kinetics of the oxygen-involved reactions, the problems of short lifespan and large overpotential prevent their widely practical applications. Thus, cathodes are designed to enhance the adsorption capacity for oxygen and modulate the electron mobility for Li-O 2 batteries. Herein, NiAl layered double hydroxide (LDH)@Cu 2 S heterostructure with extremely large specific surface area and numerous exposed active sites is designed, combining snowflake-shaped Cu 2 S and dispersed two-dimensional layered NiAl LDH. Excitingly, NiAl LDH@Cu 2 S cathode exhibited a large specific discharge capacity of 14,519 mAh g -1 at a current density of 100 mA g -1 and prolonged cycle life up to 275 cycles at 300 mA g -1 with a cut-off capacity of 600 mAh g -1 , accompanied by a low discharge overpotential of 0.14 V at the first cycle. Theoretical calculations demonstrated that the excellent electrochemical performance stems from the optimized adsorption energy of the NiAl LDH@Cu 2 S structure for reactants and intermediate products, which reduces the energy barrier of discharge/recharge process. Therefore, benefited from the modulation of electron mobility and the promoted adsorption of oxygen, NiAl LDH@Cu 2 S heterojunction can display remarkable cycle stability and reversibility as the cathode catalyst, suggesting great application prospects for enhanced Li-O 2 batteries.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yandong Sun,Weiguang Han,Fangyuan Zhang,Hui Li,Ziqi Zhang,Xue Zhang,Boxiong Shen,Sheng-Qi Guo,Tianyi Ma
The generation of singlet oxygen ( 1 O 2 ) based on photocatalytic activation O 2 is considered to have important application prospects in purifying refractory organic pollutants in water. However, the uncertain dual pathway transformation of activated O 2 severely limits the generation of 1 O 2 . In this work, we show a robust BiOCl with dual defects (adjacent I-substitution defect and Cl vacancy) in halogen layer for the selective activation of O 2 to generate 1 O 2 . Combining experiments and theoretical calculations, we confirm that dual defects are beneficial in optimizing band structures, improving carrier separation efficiency, and promoting O 2 adsorption and activation. More importantly, it is confirmed that dual defects can directionally convert O 2 into 1 O 2 by increasing the thermodynamic conversion energy barrier of non- 1 O 2 conversion pathways and serving as a necessary site for 1 O 2 generation with dual functions of oxidation and reduction. Applying dual defect modified BiOCl to the removal of refractory aromatic pollutants in water, it is found that it has efficient and stable photocatalytic degradation efficiency and broad environmental adaptability. This work not only provides in-depth insights into the mechanism of photocatalytic activation of O 2 to selective produce 1 O 2 , but also lays the foundation for further development of highly active photocatalysts for environmental remediation and energy conversion.
研究领域:
环境科学
·
材料科学
·
化学
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PROGRESS IN ORGANIC COATINGS
·
2025
·
IF 7.3
Xinglei Cui,Zhonglian Li,Yizhuo Wang,Long Li,Zhi Fang
The weather resistance capability of insulating materials, i.e. surface performance including hydrophobicity, mechanical and electrical strength under diverse weather conditions, is considered of critical importance for high-voltage devices working outdoors. In this study, atmospheric pressure plasma jet with Ar/Hexamethyldisiloxane (HMDSO) assisted by γ-Aminopropyltriethoxysilane (APTES) and oxygen (O 2 ) addition is employed to deposit a robust insulating film with good weather resistance capability on the surface of Polymethylmethacrylate (PMMA). The gas flow rates of Si-containing precursors (HMDSO/APTES) and auxiliary gas (O 2 ) are varied to elucidate the correlation between precursor ratio and film performances. The mechanism for robust film deposition is explored by investigating reactions of active particles deduced from discharge characteristics, surface physical morphology and chemical composition variations. The results indicate that APTES plays a pivotal role in the enhancement of the film mechanical strength, while O 2 can further improve both mechanical and electrical performances. A robust superhydrophobic film is deposited, inhibiting the reduction in water contact angle by 81.6 % after the tape peel test compared with the film deposited by Ar/HMDSO system, and the flashover voltage is increased by 38.2 % with the optimal HMDSO/APTES/O 2 ratio of 7:5:1. The simultaneous improvements of the film hydrophobic, mechanical and electrical performances are contributed by crosslinking of silicone deposits and the introduction of -NH₂ groups. The weather resistance capability of the insulating material is effectively enhanced, providing guidance for outdoor insulation applications.
研究领域:
材料科学
·
电气工程
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xiao Liu,Peng Zhang,Liangliang Liu,Jianwen Feng,Xiaofeng He,Xiaosheng Song,Qing Han,Hua Wang,Zhangquan Peng,Yong Zhao
Aprotic lithium–oxygen (Li–O2) batteries with an ultrahigh theoretical energy density have great potential in rechargeable power supply, while their application still faces several challenges, especially poor cycle stability. To solve the problems, one of the effective strategies is to inhibit the generation of the LiO2 intermediate produced via a surface-mediated oxygen reduction reaction (ORR) pathway, which is an important species inducing byproduct generation and low cell cyclic stability. Herein, a series of quinones and solid materials serve as the solution-mediated and surface-mediated ORR catalysts, and it was found that the generation of LiO2 and byproducts from solid catalysts was inhibited by quinones. Among the studied quinones, benzo[1,2-b:4,5-b′]dithiophene-4,8-dione, a quinone molecule with the advantage of a highly symmetrical planar and conjugated structure and without α-H, exhibits high redox potential, diffusion coefficient, and electrochemical stability, and consequently the best ORR activities and the capability to inhibit byproduct generation. It indicated that the increase of the solution-mediated ORR pathway plays an important role in restraining the discharging side reaction, substantially improving cell cycle stability and capacity. This study provides the theoretical and experimental basis for better understanding the ORR process of Li–O2 batteries.
研究领域:
材料科学
·
电化学
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高影响因子
PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2020
·Vol. 38
·期 4
·5475-5484
·
IF 5.627
Jianghui Luo,Qianjin Lin,Wenxiang Xia,Yizhuo He,Mei Mei,Lixin Lu,Yang Liu,Chun Zou
Pressurized oxy-fuel combustion has been attracting increasing attentions due to its improved efficiency and low cost. The present study reports ignition delay times (IDTs) of pyridine under O 2 /CO 2 atmospheres within a temperature range from 1202 to 1498 K at pressures from 2.2 to 10 bar for equivalence ratios of 0.5, 1.0, and 2.0. The experimental results were compared with the IDTs of pyridine under O 2 /Ar atmospheres from MacNamara et al.. The comparison results indicate that the IDTs of pyridine under O 2 /CO 2 atmospheres are evident longer than those under O 2 /Ar atmospheres even at low pressure. A modified kinetic model (HUST pyridine Model) was proposed based on our previous mechanism. HUST pyridine Model predicted well the IDTs under both O 2 /CO 2 and O 2 /Ar atmospheres obtained in shock tubes and the species profiles under both O 2 /CO 2 and O 2 /N 2 atmospheres obtained in plug flow reactors . HUST pyridine Model, Alzueta Model, and Pyridine LTO Model were evaluated. The results show that the performance of HUST pyridine Model is much better than Alzueta Model, and Pyridine LTO Model. The main reason is that the net reaction rate of C 5 H 5 N + O = C 5 H 4 N + OH in HUST pyridine Model is much faster than that in Aluzeta Model. The effect of CO 2 on the ignition of pyridine at elevated pressures has been analyzed in detail. The oxidation pathways of pyridine are also analyzed at different pressures.
研究领域:
燃烧化学
·
化学动力学
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能源工程
·
燃料科学
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高压物理
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Nano Research
·
2018
·Vol. 12
·期 3
·517-523
·
IF 7.994
Liu Tie,Wang Leidanyang,Huang Tao,Yu Aishui
Design and fabrication of framework-structured porous precursors have been regarded as a prospective albeit challenging strategy to obtain bimetal/NC-enriched bifunctional elecrocatalysts. In this work, an effective bottom-up approach involving solution-based self-assembly and a post-annealing process was developed to confine (Co, Zn)-N-C active sites into N-enriched graphitic carbon nanocages. This novel architecture containing N-doped-C stabilized bimetallic nanoparticles derived from ZIF precursors was well-studied by a series of characterization and analysis techniques. Details were given that these well-dispersed (Co, Zn) nanoparticles were encapsulated into the pyridinic-N-dominated graphitic carbon nanocage with a total metal loading of approximately 7.4 at.%. This favorable hierarchical structure not only enhances the electron conductivity, but also owns a sufficient BET surface area facilitating the gas-liquid-solid triphase reaction and producing more space to store discharge products. Importantly, results infer that the interesting nanoframes manifests a satisfying ORR/OER activity and enhanced cell performance whether liquid or solid-state electrolytes are used. As such, our work rationalizes that this type of cage-shaped bimetal-N-C material is promising for high-performance Li-O 2 batteries.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源存储
·
功能材料
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·740-751
·
IF 12.732
Lichong Peng,Yaxin Sun,Shiquan Guo,Congju Li
Oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) involve proton coupled electron transfer reaction (PCET), resulting in sluggish redox kinetics. At present, the development of high-efficiency bifunctional oxygen electrocatalysts is still a puzzling challenge. Herein, we propose a scalable strategy for embedding and beading ZIF-derived hollow Co–Nx nanocube cage dispersion implanted with porous carbonized nanofibers (EH/PCNFs and BH/PCNFs) through electrospinning and annealing. The cobalt species prevent themselves from agglomerating during the annealing process through the “fence” effect of the non-volatile Zn species, thereby synergizing with ligand volatilization to facilitate the formation of Co–Nx nanocube cages. Benefiting from the ultralong interconnected multi-layered carbon nanofiber matrix, the hollow Co–Nx nanocube cages can change the charge density and electron distribution of the carbon nanofiber matrix, endowing the carbonized nanofiber carrier with special surface polarization and accelerating the electrocatalytic kinetics. Remarkably, the integrated Li–O2 batteries (LOBs) based on BH/PCNFs and EH/PCNFs electrodes exhibit significantly decreased charge/discharge polarization (0.79 V) and a long-term cyclability (147 cycles) under a cut off capacity of 500 mA h g−1 at 200 mA g−1. This work might be beneficial for the practically viable design and manufacture of dual-function oxygen electrocatalysts.
研究领域:
材料科学
·
电化学
·
能源存储
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Science China-Materials
·
2016
·Vol. 59
·期 8
·618-628
·
IF 0
Yi Ting-Feng,Han Xiao,Yang Shuang-Yuan,Zhu Yan-Rong
Layered Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 (0 ≤ x ≤ 0.08) cathode materials were successfully synthesized by a sol-gel method. X-ray diffraction and the refinement data indicate that all materials have typical α-NaFeO 2 structure with R -3 m space group, and the a -axis has almost no change, but there is a slight decrease in the c lattice parameter as well as the cell volume. Scanning electron microscopy and high resolution transmission electron microscopy prove that all the samples have uniform particle size of about 200–300 nm and smooth surface. The energy-dispersive X-ray spectroscopy mapping shows that aluminum has been homogeneously doped in the Li 1.2 Mn 0.56 Ni 0.16 Co 0.08 O 2 cathode material. The cyclic voltammetry and electrochemical impedance spectroscopy reveal that appropriate Al-doping contributes to the reversible lithium-ion insertion and extraction, and then reduces the electrochemical polarization and charge transfer resistance. Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) shows the lowest charge transfer resistance and the highest lithium-ion diffusion coefficient among all the samples. The Li-rich electrodes with low-level Al doping shows a much higher discharge capacity than the pristine one, especially the Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) sample, which exhibits greater rate capacity and better fast charge-discharge performance than the other samples. Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) also exhibits higher discharge capacity than the pristine one at each cycle at 55°C. These results clearly indicate that the high rate capacity together with a good high rate cycling performance and high-temperature performance of the low-Co Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x =0.05) is a promising alternative to next-generation lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
锂离子电池
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
·
IF 5.7
Yulan Yu,Guanghui Feng,Yujun Jia,Hejun Li
In this work, AlN whisker-reinforced (Zr, Hf)O 2 coating was prepared on SiC coated carbon/carbon composites by sol-gel and plasma spraying methods. Its cyclic ablation resistance was evaluated using an oxyacetylene torch with a heat flux of 2.38 MW/m 2 . After ablation, the coating showed apparently decreased crack sizes and quantity as compared with the one without AlN whisker addition, pointing out its better crack tolerance. Moreover, the coating had a thinner oxidized region based on the linear ablation rate (−0.042 µm/s), greatly lower than that of pure oxide coating (−0.922 µm/s). After detailed observation and characterization, probable protection mechanism was proposed.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Qiuli Wang,Jiahao Meng,Lingling Huang,Feng Wu,Xue Yi,Guanghao Su,Ying Li,Zhenqing Hou,Zhongxiong Fan
How to efficiently synthesize toxic chemo-drugs in the hypoxia tumor microenvironment still faces a huge challenge. Herein, we have tailored engineered vehicle-free nanoreactors by coordination-driven co-assembly of photosensitizer indocyanine green (ICG), transition metal platinum (Pt), and nontoxic 1,5-dihydroxynaphthalene (DHN) to self-amplify O2 and cascade chemo-drug synthesis in tumor cells for self-reinforcing hypoxic oncotherapy. Once vehicle-free nanoreactors are internalized into tumor cells, they show a serious instability that results in rapid disassembly and on-demand drug release under the stimuli of acidic lysosome and laser radiation. Notably, the released Pt can efficiently decompose the endogenous hydrogen peroxide (H2O2) into O2 to alleviate tumor hypoxia, which is conducive to enhancing the photodynamic therapy (PDT) efficiency of the released ICG. Complementarily, a large amount of the 1O2 generated by PDT can efficiently oxidize the released nontoxic DHN into the highly toxic chemo-drug juglone. Therefore, such vehicle-free nanoreactors can achieve intracellular on-demand cascade chemo-drug synthesis and self-reinforce photo-chemotherapeutic efficacy on the hypoxic tumor. On the whole, such a simple, flexible, efficient, and nontoxic therapeutic strategy will broaden the study of on-demand chemo-drug synthesis and hypoxic oncotherapy.
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PubMed
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Yi Yuan,Wen-Long Wang,Zhi-Wei Wang,Jin Wang,Qian-Yuan Wu
Carbon nitride has been extensively used as a visible-light photocatalyst, but it has the disadvantages of a low specific surface area, rapid electron–hole recombination, and relatively low light absorbance. In this study, single-atom Ag was successfully anchored on ultrathin carbon nitride (UTCN) via thermal polymerization, the catalyst obtained is called AgUTCN. The Ag hardly changed the carbon nitride's layered and porous physical structure. AgUTCN exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants, eliminations of 85% were achieved by visible-light irradiation for 1 hr. Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 eV and suppressing electron–hole pair recombination. In addition, Ag doping facilitated O 2 adsorption on UTCN by decreasing the adsorption energy from −0.2 to −2.22 eV and favored the formation of O 2 ·− . Electron spin resonance and radical-quenching experiments showed that O 2 ·− was the major reactive species in the degradation of Acetaminophen (paracetamol, APAP).
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PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Yunbo Feng,Qian Wang,Shudong Sun,Weifeng Zhao,Changsheng Zhao
Artificial lung membranes as the core module of the extracorporeal membrane oxygenation technology (ECMO) execute the function of extracorporeal blood-gas barrier accomplishing CO 2 /O 2 exchange with blood. However, the unsatisfactory hemocompatibility and difficulty in functionalization are the prominent challenges faced by current artificial lung membrane materials. In this study, polyethersulfone (PES) composite membranes with self-anticoagulant property and high gas exchange efficient are fabricated by blending PES matrix with poly(vinylamine) (PVAm) modified carboxylic carbon nanotubes (mCNTs) and citrate-based poly(octamethylene-citrate) (POC) pre-polymers. The mCNTs construct specific gas transfer channels within the composite membranes to enhance the gas permeability, while the POC pre-polymers provide anticoagulant property based on the chelation to blood Ca 2+ and the inactivation effect to intrinsic coagulation factors. Importantly, directed by the actual ECMO gas exchange mode, we design a gas-liquid convectional circulation device that could evaluate gas exchange efficiency for the composite membranes under mimetic ECMO state. Therefore, this strategy not only proposes a new design method of advanced artificial lung membranes to solve the practical challenges in the current ECMO technology, but also establishes a scientific testing method to evaluate the gas exchange performance for new-type artificial lung membrane materials in the future.
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