SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Mengyan Duan,Long Cao,Ni Wang,Jianxin Liu,Lulu Zhang,Jiancheng Wang
Photocatalytic water splitting is hindered by flammable H 2 /O 2 cogeneration and energy-intensive post-separation. Herein, a Ru/WO 3 -MWCNTs ternary composite is designed to address these bottlenecks via a hydrogen spillover-based strategy: direct H* storage instead of gaseous H 2 generation to achieve H 2 /O 2 separation. Photogenerated H* from Ru active sites migrate through WO 3 , then is immobilized on MWCNTs as C H bonds for hydrogen storage, enabling exclusive O 2 release during photocatalysis. This composite exhibits an oxygen evolution rate (OER) of 645.28 μmol g −1 h −1 (outperforming binary counterparts) with no detectable gaseous H₂ during irradiation, alongside a stable H₂ storage capacity of 2.23 wt%. The stored hydrogen is thermally releasable, and the entire cycle of photocatalytic water splitting (hydrogen storage with O 2 evolution) and thermal H 2 release maintains excellent cyclic stability. This work establishes hydrogen storage-aided in-situ H 2 /O 2 separation as a universal strategy for addressing the core bottlenecks in photocatalytic water splitting.
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DOI
高影响因子
Nanomaterials
·
2026
·Vol. 16
·期 17
·1055
·
IF 4.8
Hang Yu,Wenjin Song,Runxin Huang,Jiale Liu,Yanshuo Du,Di Lu,Xianxian Shi,Yufang Chen
Lithium-oxygen (Li-O2) batteries are a compelling next-generation energy storage candidate owing to their ultrahigh theoretical specific energy, but their practical deployment is critically limited by sluggish cathodic oxygen reduction/evolution kinetics, severe polarization, and poor cyclability. Here, we design a composite catalyst consisting of ultrasmall iron clusters uniformly anchored on a three-dimensional nitrogen-doped carbon aerogel (Fe@NC). The material is synthesized via bidirectional freeze-drying followed by high-temperature reduction carbonization using chitosan, cellulose nanocrystals, and zinc acetate; sublimation of zinc during pyrolysis effectively suppresses iron aggregation, yielding highly dispersed Fe0 clusters of ~10 nm while preserving the aerogel’s hierarchical porous architecture rich in pyridinic and pyrrolic N species. Electrochemical tests show that Fe@NC delivers a deep-discharge specific capacity of 18,000 mAh/g, substantially outperforming pristine carbon aerogel and commercial Ketjen black, and maintains stable cycling over 280 cycles at 500 mAh/g. Microscopic and spectroscopic analyses confirm that Fe@NC promotes uniform, fine-particle Li2O2deposition without pore blockage and enables its complete reversible decomposition upon charging, effectively mitigating electrode passivation. This work demonstrates that the synergistic combination of carbon aerogel mass-transport benefits and iron cluster catalytic activity provides a viable, scalable route to high-performance Li-O2battery cathodes.
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Azhagar Samy,Raja Palani,Yi-Shiuan Wu,She-Huang Wu,Jeng-Kuei Chang,Arshid Numan,Rajan Jose,Chun-Chen Yang
Rechargeable lithium-oxygen (Li-O2) batteries are at the forefront of energy storage technology. Yet, they face critical challenges, including poor capacity, high overpotential at the oxygen cathode, inefficient lithium utilization, oxygen crossover, and the troublesome growth of lithium dendrites. This study provides an innovative solution using a graphene nanosheet (GNS) composite nickel ferrite (NiFe2O4) (NiFe2O4@GNS) catalyst and ZIF-8 particles decorated glass fiber (GF) (ZIF-8@GF) separator. Remarkably, the in situ grown ZIF-8@GF composite separator boosts higher ionic conductivity (∼2.87 × 10–3 S cm–1) and transport number (tLi+ ∼ 0.58). The modified catalyst and separator performed significantly better than the unmodified analogs in terms of specific capacity and cycling stability. In short, the device using the ZIF-8@GF separator and NiFe2O4@GNS catalyst goes up to 500 cycles without any charge polarization at 300 mA·g–1 and 500 mAh·g–1. In contrast, the corresponding cycle number for the cell with an unmodified separator even using the modified catalyst is ∼209 cycles with high charge polarization. These studies reveal that the modified separator effectively minimizes oxygen and I–/I3– redox crossover, captures anions, accelerates lithium-ion transport, and prevents the harmful intermediates (like O2– or LiO2), which can drastically degrade the organic electrolyte. Furthermore, the insulating characteristics of the ZIF-8@GF membrane deter direct electron transport to ZIF-8 nanoparticles during lithium peroxide formation, thus ensuring uninterrupted access to catalytic anion trapping sites.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
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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高影响因子
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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DOI
高影响因子
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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DOI
高影响因子
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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DOI
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
·
能源工程
·
燃料科学
·
高压物理
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DOI
高影响因子
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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DOI
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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DOI
高影响因子
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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DOI
Catalysis Science & Technology
·
2024
·
IF 4.4
Pengken Li,Hui Zhao,Rong Ji,Wenwen Chi,Xinyu Sun,Yuming Dong,Yongfa Zhu
A one-step two-electron oxygen reduction pathway is crucial for the stable and efficient photosynthesis of hydrogen peroxide. However, the lower oxygen adsorption and activation capacity significantly restrict the ability of the one-step two-electron oxygen reduction pathway. In this work, a covalent organic framework containing a diacetylene unit (COF-Tfp-BDDA) as an efficient oxygen reduction active site was designed for the photosynthesis of hydrogen peroxide. This work demonstrates that the introduction of the diacetylene unit efficiently improved the oxygen adsorption and activation capacity of the COF. Additionally, the introduction of a diacetylene unit effectively promoted charge separation. COF-Tfp-BDDA exhibited a superior rate of H2O2 preparation (880 μmol g−1 h−1) under visible light irradiation from pure water and oxygen, better than most COF-based photocatalysts. The catalyst exhibited a stable hydrogen peroxide photosynthesis efficiency above 100 hours in cycling experiments. Based on the experimental and DFT calculation results, the introduction of a diacetylene unit not only enhances the adsorption and activation of oxygen but also alters the reduction pathway of oxygen, leading to effective charge separation. These factors contribute to the efficient photosynthesis of hydrogen peroxide in pure water. This work provides a novel idea regarding the application of COFs in the field of solar energy conversion.
研究领域:
材料科学
·
光催化
·
太阳能转化
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）