JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Kaiquan He,Hong Tan,Shizhen Li,Pu Hu,Chaoqun Shang
The Li-S batteries possessing high theoretical energy density are promising for next-generation energy storage. However, the shuttle effect and slow conversion of lithium polysulfides seriously hinder the practical application. In this contribution, introducing metallic Cu to modify dual-phase TiO 2 (rutile/anatase) grown on N-doped carbon nanosheets (denoted as Cu/mTiO 2 -NC) can act as a buffer layer to confine the active S species in the cathode region effectively. The corresponding systematic experiments show that the Cu/mTiO 2 -NC provides sufficient surface affinity to adsorb and capture polysulfides and has a highly conductive C/N skeleton to achieve rapid electron migration. Moreover, the metallic Cu can react with polysulfides to further immobilize polysulfides. Thus, the Li-S batteries, with the aid of optimal Cu/mTiO 2 -NC, exhibit a desirable discharge capacity of 811 mA h g –1 after 100 cycles at 0.2 C, which is 50 % higher than that without Cu/mTiO 2 -NC. Moreover, the optimum Li-S batteries deliver a discharge capacity of 435.45 mA h g –1 after 600 cycles at 0.5 C, corresponding to attenuation per cycle of only 0.09 %.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Hardy Shuwanto,Hairus Abdullah,Dong-Hau Kuo,Noto Susanto Gultom
Y-doped Zn(O,S) nanocatalysts with different Y amounts have been fabricated, characterized, and applied for photocatalytic hydrogen evolution reaction (HER) and hydrogenation reaction (PHR) to reduce nitro groups and to cleave azo (N N) bond. The oxysulfide formation was confirmed by XRD, SAED, and DRS analyses. The best Y-doped Zn(O,S) could evolve hydrogen by 3,946 μmol g −1 h −1 in aqueous solution with ethanol as a hole scavenger reagent. The PHR of 5% Y-doped Zn(O,S) could hydrogenate 4-nitrophenol to 4-aminophenol and nitrobenzene to aniline in 120 and 90 min, respectively in a low-power UV light illuminated condition (16 W) as confirmed with UV–Vis spectroscopy. Besides of that, a sluggish cleavage of N N bond in azobenzene could be totally done to yield aniline within 30 min. Lastly, the detail mechanisms of HER and PHR including their molecular chemisorption phenomena were proposed and described with the steps of solvation , adsorption, pinning, and surface hydrogenation reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Tian Lan,Lecheng Lei,Bin Yang,Xingwang Zhang,Zhongjian Li
Kinetics of iron(II)- and manganese(II)-catalyzed oxidation of S(IV) in seawater were studied here to provide theoretical support for the flue gas desulfurization process (SFGD). Experiments were carried out with artificial seawater and acetic buffer. Results indicated that the reaction order with respect to dissolved oxygen is zero. However, the reaction order with respect to S(IV) is variable: second-order under uncatalyzed condition (4.0 ≤ pH ≤ 7.0); first-order under Fe(II)-catalyzed oxidation (2.5 ≤ pH ≤ 3.5); first-order (4.0 ≤ pH ≤ 5.0) and second-order (5.5 ≤ pH ≤ 5.9) under Mn(II)-catalyzed oxidation. The different S(IV) dependence could be attributed to different metal speciation at different pH values. Also, acetate is found to have significant inhibition effect on Mn(II)-catalyzed oxidation in high ion strength solution. The strong catalytic effect of Fe(II) and Mn(II) ions on S(IV) oxidation could lead to new ideas for the design of SFGD systems.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Feihu Mu,Shengpan Xu,Meixin Li,Yuqiu Yang,Xiaozhong Chu,Zhipeng Cheng,Xujing Guo,Jiming Xu,Benlin Dai,Chang-Ha Lee
Large amounts of carbon are stored primarily in dissolved organic matter (DOM), which plays an important indicator of lake eutrophication. However, removing DOM from eutrophic lakes remains a major challenge. Herein, a novel S-scheme flower-like microsphere BiVO 4 /nanosheet g-C 3 N 4 3D/2D heterojunction was successfully constructed using a two-step method for DOM degradation of real eutrophic lake water in the presence of peroxydisulfate (PDS). 1.0-BiVO 4 /g-C 3 N 4 /PDS exhibited highly efficient photocatalytic performance with an 87.8 % removal rate of DOM for 60 min, which was 5.3 and 8.9 times higher than BiVO 4 /PDS and g-C 3 N 4 /PDS, respectively. Sulfate radical (·SO 4 − ), hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) were mainly responsible for DOM degradation in the 1.0-BiVO 4 /g-C 3 N 4 /PDS system, and the transformation pathway of 1 O 2 was emphatically analyzed. In addition, the changes of fluorescence components in DOM were detected using synchronous fluorescence spectra, second derivative spectra, and two-dimensional correlated spectroscopy analysis. Humic-like fluorescence, fulvic-like fluorescence, and protein-like substances were removed higher than 85.30 %, 73.02 %, and 67.23 % by the 1.0-BiVO 4 /g-C 3 N 4 catalyst activating the PDS under visible light (VL), respectively. When the toxicity of catalytically treated eutrophic lake water was estimated by growth inhibition of Escherichia coli , the biotoxicity of DOM decreased continuously in the BiVO 4 /g-C 3 N 4 /PDS/VL coupling process. Theoretical calculations and photoelectrochemical tests suggested that the BiVO 4 /g-C 3 N 4 /PDS catalytic activity enhancement was attributed to the S-scheme mechanism and hybrid advanced oxidation process. It is expected that this work can provide new insight into DOM degradation in eutrophic lake water by the heterogeneous photocatalysis combined with the PDS activation system.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Siyuan Sun,Xiaoyun Zhang,Yang Sun,Fan Yang,Tianyu Bai,Cunhui Yu,Kexin Wei,Haojia Zhong,Qiang Wei,Yongfeng Li
Porous carbon coated manganese compounds nanoparticles (MnX, X = P, O or S) is a kind of potential catalysts for oxygen electrocatalysis due to the controllable d-band center, while the complex mechanism and performance difference is yet to reveal due to the lack of catalyst platform. Herein, the ORR catalytic activity and difference reason between manganese phosphide, oxide, and sulfide are tested and discussed via manganese compounds contained carbon-based catalyst platforms synthesis and Density functional theory (DFT). Manganese compounds nanoparticles active sites are uniformly distributed in porous carbon fibers/graphene composite, which guarantees the high mass transfer ability and conductive ability. Experiment results show that catalyst with Mn 2 P active sites exhibits best bifunctional catalytic activity for ORR/OER, which only need 0.89 V (vs. RHE) to achieve a half-wave potential (E 1/2 ) in ORR and 1.58 V (vs. RHE) to reach the overpotential at 10 mA cm −2 (E 10 ) in OER. Theoretical analysis shows that the d-band center of Mn in Mn 2 P is much closer to the Fermi level than MnS and MnO. The rate-determining process of Mn 2 P has the smallest energy barrier of 0.56 eV, indicating the best ORR activity. This work provides paves a solid way for the synthesis of carbon-based catalysts with manganese compounds active sites.
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高影响因子
ACS Nano
·
2023
·
IF 17.1
Bin Sun,KangKang Bao,Panpan Wang,Kai Liu,Hui Wu,Yang Jin
Due to their low self-discharge rate, no intermediate product dissolution in the cathode, and easy recycle of electrode materials, solid electrolyte-based molten lithium sulfur batteries can be one of the highly anticipated advanced electrochemical chemistry technologies for grid-scale energy storage. However, the actual energy density and reversibility of them still face severe challenges for low active materials loading and the inherent low conductivity of sulfur and its end-products. In this work, with the iodide modulation effect, small size (∼5 nm for the primary particles) and low relative crystallinity discharge end-products in the sulfur cathode can be formed, contributing to the immense specific capacity and reversibility. As validated by theoretical calculations, iodide ions in the homogeneous molten composite cathode display a profound comprehensive effect on the chemical reaction and cycling stability. As a result, high sulfur loading (over 80 mg cm–2) with a significant utilization rate can be achieved, corresponding to a single Li-S cell of 1.39 Ah and a volumetric energy density of 528.5 Wh L–1 based on the overall cell volume; simultaneously, a prominent cycling stability during 300 cycles along with an impressive reversibility is obtained.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Ting Huang,Qingbao Guan,Li Yuan,Guozheng Liang,Aijuan Gu
Developing a facile strategy to synthesize thermosetting all-aromatic liquid crystalline poly(esterimide)s (LCPEIs) at medium-low temperature and endowing LCPEIs with good processability and high thermal resistance are still two big challenges. Herein, a new solution polymerization based on direct esterification under 120 °C is developed, overcoming bottlenecks of traditional melt and solution polymerizations. Besides, two new reactive LCPEIs (LCPEI-1 and LCPEI-2) terminated with 3-ethynylaniline (3-EA) were synthesized, and their structures and properties were compared with two control samples without 3-EA end groups. LCPEI-1 and LCPEI-2 not only show good processing characteristics including low melting temperature (Tm = 200 °C), low melting viscosity, and good solubility in solvent, but their cured samples also have high glass transition temperature (Tg = 192 and 225 °C) and high storage modulus, whereas control samples, even treated with similar thermal history as curing procedure for LCPEI-1 and LCPEI-2, have poor performances. Cured-LCPEI-2 exhibits the highest Tg among polyesters with low Tm values (<250 °C) reported. The mechanism behind outstanding performances of LCPEIs is discussed.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 16
·5579-5589
·
IF 6.119
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu,Quanli Dong
Transition metal co-catalysts exhibit considerable potential in the photocatalytic water splitting process, but their limited activity and poor stability inhibit their extensive application, and therefore effective schemes are required to further enhance their co-catalytic performance. In this article, 2D/2D C3N4/CdS heterogeneous photocatalysts are first synthesized, and then CoNi alloyed NPs are selectively loaded on their CdS nanosheets by a convenient photodeposition method. The CoNi loading amount and Co/Ni ratio are adjusted by the photodeposition time and precursor Co2+/Ni2+ ratio, respectively. Meanwhile, Co–S bonds are formed between CdS and CoNi NPs. Their optimal hydrogen evolution rate can reach up to 2936.65 μmol g−1 h−1, which is higher than that of C3N4/CdS with Co, Ni or Pt as co-catalysts (i.e. 844.59, 2385.96 and 2486.66 μmol g−1 h−1), respectively. The enhanced photocatalytic performance should be due to the following three points: (1) the formation of the 2D/2D C3N4/CdS heterojunction; (2) the optimized Gibbs free energy of the CoNi co-catalysts; (3) the formation of Co–S bonds between CoNi and CdS. Our work provides a cost-effective scheme to exploit stable and efficient photocatalysts.
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高影响因子
Polymers
·
2019
·Vol. 11
·期 6
·1002
·
IF 3.164
Minghui Xiao,Na Zhang,Jie Zhuang,Yuchen Sun,Fang Ren,Wenwen Zhang,Zhaosheng Hou
The aim of this study is to offer a new class of degradable shape-memory poly(ether-ester-urethane)s (SMPEEUs) based on poly(ether-ester) (PECL) and well-defined aliphatic diurethane diisocyanate (HBH) for further biomedical application. The prepolymers of PECLs were synthesized through bulk ring-opening polymerization using ε-caprolactone as the monomer and poly(ethylene glycol) as the initiator. By chain extension of PECL with HBH, SMPEEUs with varying PEG content were prepared. The chemical structures of the prepolymers and products were characterized by GPC,1H NMR, and FT-IR, and the effect of PEG content on the physicochemical properties (especially the shape recovery properties) of SMPEEUs was studied. The microsphase-separated structures of the SMPEEUs were demonstrated by DSC and XRD. The SMPEEU films exhibited good tensile properties with the strain at a break of 483%–956% and an ultimate stress of 23.1–9.0 MPa. Hydrolytic degradation in vitro studies indicated that the time of the SMPEEU films becoming fragments was 4–12 weeks and the introduction of PEG facilitates the degradation rate of the films. The shape memory properties studies found that SMPEEU films with a PEG content of 23.4 wt % displayed excellent recovery properties with a recovery ratio of 99.8% and a recovery time of 3.9 s at body temperature. In addition, the relative growth rates of the SMPEEU films were greater than 75% after incubation for 72 h, indicating good cytocompatibility in vitro. The SMPEEUs, which possess not only satisfactory tensile properties, degradability, nontoxic degradation products, and cytocompatibility, but also excellent shape recovery properties at body temperature, promised to be an excellent candidate for medical device applications.Keywords:poly(ether-ester-urethane)s;poly(ethylene glycol);well-defined hard segments;degradability;shape memory behavior
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Yang Bai,Fuxiang Feng,Lei Tian,Yankun Xiong,Yong Yang,Qiang Guo,Yuan Liu
To advance the direct coal liquefaction (DCL) technology by a “Catalytic cycle of hydrogen donor solvents” pathway, it was important for the iron-based DCL catalyst to be pre-sulfurized under a suitable condition. In this report, the effect of liquid medium in the slurry bed pre-sulfurization process on iron-based catalyst was studied. Catalysts were pre-sulfurized under a variety of liquid mediums including alkanes, aromatics and heteroatom-containing compounds and the activity were evaluated according to their performance on hydrogenation of naphthalene . It was observed that, the nitrogen-containing medium give rise to the significant negative influence on the catalytic activity (with only 2.5 %-15.3 % of naphthalene conversions). Multiple spectroscopic and microscopic analyses of catalysts exhibited that the decrease of S vacancies was mainly responsible for the low activity. It was due to the promotion effect on Fe 1-x S crystallization and troilite generation. S vacancies of the iron-based catalysts was considered as Lewis acid sites to catalyze the hydrogenation reaction. The new findings from this work is beneficial for the development and optimization of pre-sulfurization technology .
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高影响因子
EUROPEAN JOURNAL OF PHARMACOLOGY
·
2022
·
IF 5.195
Hongyu Zhou,Yang Zhang,Yuan Tian,Yushi Sun,Yajuan Chen,Yanli Zhang,Qin Zhu,Junfang Pan,Chen Qing
9-nitrocamptothecin (9-NC), an active derivative of camptothecin (CPT), demonstrated antitumor effect on experimental tumors in mice by topoisomerase I (Topo I) inhibition. However, under human physiological conditions, the rapid opening of lactone ring of 9-NC resulting in the formation of inactive and high toxic carboxylate limited its clinical efficacy. Therefore, strategies aimed to maintain the active closed-lactone form of 9-NC in the plasma were developed, such as prodrugs . In our study, 9-nitro-20(S)-carbonate-camptothecin (NCP4), a novel prodrug of 9-NC, was designed and synthesized. A preclinical evaluation of the chemotherapeutic potential of NCP4 was performed in vitro and in vivo . In cytotoxicity assay against six human cancer cells, the cytotoxic effect of NCP4 was slightly weaker than 9-NC. In addition, our data showed that 9-NC can be converted from NCP4 in vivo , and that the intracellular conversion of NCP4 to its active metabolites was correlated well with its cytotoxicity, demonstrating that NCP4 could serve as a prodrug of 9-NC. In human hepatoma Bel-7402 xenografts, NCP4 by intravenous injection showed more potent antitumor efficacy than 9-NC. Mechanistically, NCP4 induced cell apoptosis by increasing the expressions of caspase-3 and Bax in tumor tissues. In human hepatoma Hep G2 xenografts, NCP4 by oral administration significantly inhibited tumor growth. Importantly, the toxic effect of NCP4 on mice was much lower than 9-NC, demonstrating improved safety of NCP4. Overall, our study indicated that NCP4 would be a promising anticancer candidate and worthy of further investigation.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yiji Chen,Liang He,Shirong Ai,Hang Yao,Aihua Xiong,Li Li,Jiang Li,Zhongshou Liu,Yansha Gao,Ruimei Wu,Limin Lu
Simultaneous and accurate analysis of multiple heavy metals (HMs) in environment by electrochemical method still faces huge challenges, such as complex experimental process, low detection efficiency and the interference arising from electrochemical interactions between different HMs. To address these issues, we propose a sensing platform combining S-TiO 2 @Ti 3 C 2 MXene with machine learning strategies for simultaneous electrochemical detection of Cu 2+ and Hg 2+ in water samples. Specifically, surface morphology and crystal structure of S-TiO 2 @Ti 3 C 2 were characterized via SEM, XRD, and XPS. Electrochemical behaviors were systematically investigated using cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Orthogonal test-based multi-objective optimization method integrated with comprehensive balance approach were employed to determine the optimal sensing parameters, which were identified pH of 4.5, deposition time of 210 s, and deposition potential of −1.5 V. The fabricated sensor exhibited high sensitivities of 44.122 and 143.795 μA·L·mg −1 , low limits of detection of 0.392 and 0.093 μg·L −1 , and broad linear ranges of 0.001–1000 μg·L −1 for Cu 2+ and Hg 2+ , respectively. Furthermore, machine learning strategy was introduced to resolve the poor accuracy issue associated with traditional calibration curve analysis for the simultaneous detection of Cu 2+ and Hg 2+ across the entire linear range. The results indicated that minimum Redundancy Maximum Relevance (mRMR) algorithm effectively extracted valuable and critical information of Cu 2+ and Hg 2+ from the full voltammetric curves, and the constructed support vector machine (SVM) model remarkably improved detection accuracy. The reliability of the proposed SVM model was validated through simultaneous detection of HMs in actual environmental water samples, yielding favorable recovery rates.
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