PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2020
·Vol. 38
·期 4
·5475-5484
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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
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化学动力学
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能源工程
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燃料科学
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高压物理
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·740-751
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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
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电化学
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能源存储
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高影响因子
JOURNAL OF POLYMER SCIENCE
·
2026
·
IF 3.9
Jialong Yang,Guangqun Zhai
The effect of H 2 O 2 and H 2 O 2 -ascorbic acid (Vc) pairs on defunctionalization of 2-cyano-2-propyl dithiobenzoate (CPDB) and CPDB-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization of methyl methacrylate (MMA) in dimethyl sulfoxide (DMSO) is investigated. The stability of CPDB toward H 2 O 2 is monitored by UV–vis absorption spectroscopy. CPDB is partially defunctionalized by H 2 O 2 alone and more seriously by H 2 O 2 -Vc pairs at 40°C, due to the oxidation by H 2 O 2 and the stepwise addition of DMSO-derived H 3 C· radicals. MMA greatly inhibits the defunctionalization of dithiobenzoate moieties, as both HO· and H 3 C· radicals incur oligomeric MMA-terminated alkyl radicals, which conserve the dithiobenzoate moieties of CPDB. H 2 O 2 -Vc-initiated CPDB-mediated RAFT polymerization is undertaken at 30°C and 40°C. Conversion is measured by gas chromatography, and molecular weight (MW) of PMMA is determined by gel-permeation chromatography. The processes manifest a moderately controlled fashion under optimal conditions. The products at low conversion display a multi-component composition, with high-MW PMMA consisting of 90% at least. MW of PMMA increases almost linearly with the yield and maintains a narrow distribution, but higher than the corresponding theoretical MW, owing to the partial defunctionalization of CPDB. Mass spectroscopy reveals that the irreversible termination of the intermediate radicals is the primary factor. Graphical H 2 O 2 initiated reversible addition-fragmentation chain transfer (RAFT) polymerization in dimethyl sulfoxide (DMSO) with 2-cyano-2-propyl dithiobenzoate (CPDB) as both the reducing agent and CTA. The defunctionalization of CPDB by H 2 O 2 in DMSO was observed, but methyl methacrylate significantly inhibited the defunctionalization. The CPDB-mediated RAFT polymerization was fulfilled with H 2 O 2 or H 2 O 2 -Vc pairs as the initiator. MS attributed the defunctionalization to the formation and the irreversible termination of lower-activity intermediate radicals.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Fangjie Liu,Zaifu Gong,HaiZhao Li,Wuhui Li,Yuliang Liu,Qingjie Wang
Proposes a functional modularization strategy to fabricate BZCY-GDC-LCO electrodes. • Exhibits low polarization resistance (0.141 Ω·cm 2 ) with 216 h stable operation. • Single cell delivers 0.757 W·cm −2 (FC) and 1.182 A·cm −2 at 1.3 V (EC) at 650 °C. Efficient triple-conduction (H + /O 2− /e − ) is vital for high-performance reversible protonic ceramic cells (R-PCCs), yet the underlying transport mechanisms and their specific impacts on electrode kinetics remain elusive. In this work, we employ a “functional modularization” strategy to engineer a BaZr 0.1 Ce 0.7 Y 0.2 O 3−δ -Gd 0.1 Ce 0.9 O 1.95 -LaCoO 3 (BZCY-GDC-LCO) triple-phase composite air electrode using commercially available precursors. The synergistic effects and individual roles of the conducting species in optimizing electrochemical kinetics were systematically investigated. The optimized BZCY-GDC-LCO electrode (1:1:1 mass ratio) exhibits excellent chemical compatibility, high oxygen vacancy concentration, and a well-distributed triple-phase boundary. Consequently, it achieves a low polarization resistance of 0.141 Ω·cm 2 at 650 °C and demonstrates robust long-term stability over 216 h of operation. Single-cell tests deliver a peak power density of 0.757 W·cm −2 in fuel cell mode and a current density of 1.182 A·cm −2 at 1.3 V in electrolysis mode at 650 °C. Kinetic analysis reveals oxygen adsorption/dissociation as the rate-determining step, while excessive steam partial pressure inhibits oxygen transport via surface site passivation. This work provides a scalable design strategy for high-performance R-PCC air electrodes, demonstrating that superior performance and favorable techno-economic feasibility can be achieved using conventional materials. Download: Download high-res image (166KB) Download: Download full-size image
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Yu Zhong,Xiaojuan Chen,Xinyang Zhang,Lei Qin
The capacity and lifespan of superoxide-based potassium–oxygen batteries (POBs) are limited by the failure of the potassium (K) anode due to oxygen crossover. The high-concentration potassium bis(trifluoromethanesulfonyl)imide (KTFSI)/dimethoxyethane recipe enables efficient anode passivation, but its high viscosity and elevated cost necessitate the use of a highly fluorinated ether co-solvent. In this study, we elucidate the indeterminate role of fluoroether in constructing the anode passivation layer. The fluoroether participates with TFSI − anions to form a robust solid electrolyte interphase (SEI) that effectively mitigates oxygen crossover. Moreover, the fluoroether shows a Janus effect that excessive addition triggers severe K corrosion, while an optimal amount leads to a desirable SEI on the K surface. This SEI acts both as an oxygen permeation barrier and as an efficient K + -conductive channel. With a more stable environment for the K anode, a POB utilizing the KTFSI-based electrolyte delivers over 200 cycles (above 800 h) with low round-trip overpotentials and high average coulombic efficiency (98.1%) as opposed to one using the potassium hexafluorophosphate-based electrolyte that fails early. Spectroscopic analyses and theoretical simulations were utilized to elucidate the molecular-scale interactions in the electrolyte components. This study provides fundamental insights and practical strategies for the development of long-life POBs.
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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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Chang Ge,Yijie Yang,Qizheng Cai,Zheng Fang,Heng Dai,Man Tong,Songhu Yuan
Surface water–groundwater interaction zones are recognized as hotspots for reactive oxygen species (ROS) production. Entrapped gas bubbles formed due to water table fluctuations are important sinks and sources of dissolved oxygen (DO), whereas their influence on ROS production remains unknown. Here, we use column experiments to simulate surface water–groundwater interactions and quantitatively investigate the role of entrapped gas bubbles in the spatiotemporal distributions of DO and H2O2. During surface water recharge, gas bubbles act as O2 sinks, which uptake O2 from DO in the infiltrated surface water and thus restrict O2 penetration and the resultant H2O2 production. For subsequent groundwater discharge, the O2 stored in gas bubbles serves as a DO source for groundwater, which promotes H2O2 production. Cycles of groundwater discharge and surface water recharge experiments support the fact that the restriction and promotion effects induced by gas bubbles persist across recharge–discharge cycles. Reactive transport modeling reveals that the peak concentration and distribution area of H2O2 during surface water recharge decrease with the increase in the degree of gas saturation, but they increase during groundwater discharge. These findings highlight the previously overlooked dual roles of entrapped gas bubbles in ROS production and distribution under fluctuating hydrological regimes.
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PubMed
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
FUEL
·
2024
·
IF 6.7
Xue Lu,Jingfang Li,Liye Liang,Guangming Li
Deep desulfurization with high-efficiency is imperia for environmental demands with increasing stringent standard of sulfur content in fuels. To develop high efficiency heterogeneous catalyst for aerobic oxidative desulfurization (AODS) of fuel, an Anderson-type CoMo 6 -2NH 2 (POM) as active site, which was considered to be very effective in catalyzing the activation of O 2 , was successfully anchored on the sub-stoichiometric ECOF as a carrier by Schiff-base condensation reaction between –NH 2 groups in CoMo 6 -2NH 2 and –CHO groups in ECOF. The anchoring of CoMo 6 -2NH 2 on ECOF by covalent bond resulted in the heterogenization of CoMo 6 -2NH 2 enabled CoMo 6 -2NH 2 @ECOF to be recyclable during the AODS process. When CoMo 6 -2NH 2 @ECOF was applied as catalyst for AODS of fuel with surfactant (OTAC) under O 2 , it exhibited excellent catalytic activity with almost 100 % removal rates under 95 °C for 6 h. Moreover, the catalyst can be recycled 7 times without significant loss of catalytic activity. Further, the structure-activity relationship was investigated and the reaction mechanism of AODS of fuel was verified by ESR, XPS analysis and selective quenching experiments.
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高影响因子
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
·
2020
·
IF 0.936
Liang WANG,Zhang-Quan PENG
Development of lithium-oxygen (Li-O 2 ) batteries is hindered by large overpotentials, low energy efficiency and unsatisfactory cycling life, which are predominately caused by the oxygen evolution reaction (OER) involving sluggish oxidation of lithium peroxide (Li 2 O 2 ). Herein, a highly-efficient soluble redox mediator (RM) of N , N’ -Diphenyl- p -phenylenediamine (DPPD) is introduced to catalyze the oxygen evolution reaction for Li-O 2 batteries. During charging process, DPPD is electrochemically oxidized into DPPD + , which can chemically decompose Li 2 O 2 on the cathode with a much-reduced overpotential. The in-situ differential electrochemical mass spectrometry confirms that the charging process is dominated by Li 2 O 2 decomposition. With the assistance of DPPD, Li-O 2 cells can achieve lower charging potential, improved cycling stability, and prolonged lifespan (294 cycles) which is three times longer than that of tetrathiafulvalene counterpart. This work presents a credible and viable opportunity for long lifespan Li-O 2 batteries.
研究领域:
电化学
·
能源材料科学
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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
SusMat
·
2021
·Vol. 1
·期 3
·448-457
·
IF 0
Zhaomin Chen,Xiaoqing Gu,Yutong Guo,Xin Wang,Mingwang Shao,Bin Dong,Zhenhui Kang
Electrochemical cell can overcome the inherent intermittence of the renewable energy sources, thus showing great potentials in applications ranging from electrical energy storage to future smart grid. However, the current electrochemical cells could not achieve the “total green” feature by fully utilizing the clean and abundant O 2 /H 2 O redox couples due to the enormous overpotentials for both oxygen reduction reaction (ORR) and oxygen release reaction (OER). Herein, we report a “total green” electrochemical composite film cell based on carbon dots (CDots), which can realize both ORR and OER in the acid environment. The in-air voltage generation (0.95 V, with a maximum power of 5.3 μW) relies on the multiple-electron-transfer redox chemical reaction between the two active components inside the composite film, that is, ORR/OER of CDots and the redox reaction of polyaniline (PANI) on the electrode and the resulting proton concentration gradient. Interestingly, the cell can be self-recovered at low load, recharged by adding H 2 O 2 , or electrocharged at high load. We anticipate that current study may open up new opportunities for designing and developing total-green energy storage and conversion systems for diverse applications.
研究领域:
材料科学
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能源技术
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环境科学
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