LANGMUIR
·
2023
·
IF 3.9
Hongqi Nie,Zikangping Wang,Xue-Xue Zhang,Su-Lan Yang,Zhi Ren,Qi-Long Yan
In this study, a 2D structured triaminoguanidine-glyoxal polymer with a high nitrogen content has been coordinated with metal ions to produce energetic metal complexes (TAGP-Ms) employed as energetic burn rate inhibitors. The metal ions (Ba2+, K+, and Ca2+) are elaborately selected based on their ability of suppressing the burn rate of composite propellants. The CL-20 crystals were intercalated with prepared TAGP-Ms materials via a solvent–antisolvent method for realization of the precise control on burning behaviors of studied propellants. The influence of TAGP-Ms inhibitors on thermal decomposition and combustion characteristics of high-energy composite propellants was evaluated using thermal analysis and a combustion diagnostic method. Results of TGA/DSC-FTIR measurements suggest that the thermal decomposition of CL-20-containing composite propellants was found to be constrained by varied degrees as a result of TAGP-Ms additions, in which the TAGP-K displays a stronger effect on suppressing the thermal decomposition of CL-20 compared with that of other TAGP-Ms. The FTIR spectra indicate that the primary gaseous phase products are composed of N2O, H2O, and CO2 in CL-20 decomposition, as well as by HCl, H2O, NO2, and N2O in the decomposition of AP for all studied composite propellants. The combustion characterizations show that the TAGP-K-containing composite propellant exhibits a significantly reduced rate of heat release but is associated with a higher flame radiation intensity increased by 4.2% compared with that of the reference propellant, which clearly implies that the TAGP-K is capable of suppressing the energy release rate while ensuring the high energetic features of propellants to be well maintained. Moreover, the burn rate pressure exponents are considerably decreased by ∼10% for the TAGP-K-containing propellants in comparison with those of propellants with the typical formulation, which strongly suggests that TGAP-Ms are promising candidates for tuning the combustion behaviors of composite propellants by influencing the decomposition processes of CL-20 and AP collectively.
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高影响因子
CHEMICAL PHYSICS LETTERS
·
2023
·
IF 2.8
Wei Li,Xianhua Sheng,Zhaoliang Yu,Qian Tang,Jinghua Geng,Dangzheng Hu,Xiangdong Meng,Yumei Zhang
Co-based compound is a kind of bifunctional electrocatalyst for the half reactions of water splitting. Here we report the catalytic performance of Co-Cl-C composited catalyst prepared by flash Joule heating system in oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). It is found that Co-Cl-C composited film is an efficient electrocatalyst of OER and HER. In addition, the flash Joule heating is a fast, low energy consumption, and environmentally friendly preparation method. It opens up a new idea for the preparation method of composite materials.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 14
·5355
·
IF 4.6
Keyan Chen,Shiqi Fu,Chenyu Jin,Fan Guo,Yu He,Qi Ren,Xuesheng Wang
Smartphone-assisted fluorescence and colorimetric methods for the on-site detection of Hg2+and Cl−were established based on the oxidase-like activity of the Au–Hg alloy on the surface of Au/Cu/Ti3C2NSs. The Au nanoparticles (NPs) were constructed via in-situ growth on the surface of Cu/Ti3C2NSs and characterized by different characterization techniques. After the addition of Hg2+, the formation of Hg–Au alloys could promote the oxidization of o-phenylenediamine (OPD) to generate a new fluorescence emission peak of 2,3-diaminopenazine (ADP) at 570 nm. Therefore, a turn-on fluorescence method for the detection of Hg2+was established. As the addition of Cl−can influence the fluorescence of ADP, the fluorescence intensity was constantly quenched to achieve the continuous quantitative detection of Cl−. Therefore, a turn-off fluorescence method for the detection of Cl−was established. This method had good linear ranges for the detection of Hg2+and Cl−in 8.0–200.0 nM and 5.0–350.0 µM, with a detection limit of 0.8 nM and 27 nM, respectively. Depending on the color change with the detection of Hg2+and Cl−, a convenient on-site colorimetric method for an analysis of Hg2+and Cl−was achieved by using digital images combined with smartphones (color recognizers). The digital picture sensor could analyze RGB values in concentrations of Hg2+or Cl−via a smartphone app. In summary, the proposed Au/Cu/Ti3C2NSs-based method provided a novel and more comprehensive application for environmental monitoring.Keywords:Au/Cu/Ti3C2NS;Au–Hg alloy;oxidase-like activity;smartphone;colorimetric detection
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ACS Omega
·
2018
·
IF 0
Tingting Cheng,Jian Chen,Aofei Cai,Jian Wang,Haiyan Liu,Yuandong Hu,Xiaojun Bao,Pei Yuan
A series of silica supported Pd (Pd/SiO2) catalysts were prepared in various HCl concentrations (CHCl) of the impregnation solution with different electrostatic interactions between Pd precursor and support, and their catalytic properties were evaluated by the selective hydrogenation of nitrile butadiene rubber (NBR). The results show that with the CHCl increasing from 0.1 to 5 M, the particle size of Pd nanoparticles dramatically decreases from 24.2 to 5.1 nm and stabilizes at ∼5 nm when CHCl is higher than 2 M. Using the catalysts prepared with a high CHCl (>2 M), an excellent hydrogenation degree (HD) of ∼94% with 100% selectivity to C═C can be acquired under mild conditions. Interestingly, the HD could be remarkably increased from 65 to 92% by increasing only CCl– from 0.1 to 2 M with the addition of NaCl while keeping CH+ at 0.1 M. This is because PdCl42– is the predominant existing form of precursor at high CCl–, which has a strong electrostatic attraction with the positively charged support favorable for the formation of small-sized Pd nanoparticles over silica. Notably, Pd leaching behavior during the hydrogenation reaction is closely related to CH+, and the higher the CH+, the less Pd residues are detected in the hydrogenated NBR. Our contribution is to provide a facile strategy to synthesize effective and stable Pd/SiO2 catalysts via adjusting the electrostatic interaction, which exhibits a high activity and selectivity for NBR hydrogenation.
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APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Likai Wang,Jin Peng,Zhenghua Tang,Xiongwu Kang,Mingli Fu,Shaowei Chen
Structurally similar molecule-like Au 11 (PPh 3 ) 7 Cl 3 and [Au 11 (PPh 3 ) 8 Cl 2 ]Cl nanoclusters have been successfully synthesized and employed as catalysts for selective oxidation of styrene. The two clusters exhibited similar but slightly different well-defined optical absorbance, and the subtle structural difference is also reflected in proton nuclear magnetic resonance ( 1 H NMR) studies. In electrochemical measurements, Au 11 (PPh 3 ) 7 Cl 3 and [Au 11 (PPh 3 ) 8 Cl 2 ]Cl show a large electrochemical band gap of 2.15 eV and 2.09 eV, respectively. Styrene oxidation has been employed as a model reaction to investigate the impacts of the ligand shell composition on the catalytic activity and selectivity of the two clusters. Interestingly, the main product is benzaldehyde when oxygen is employed as oxidant, and the catalytic activity of Au 11 (PPh 3 ) 7 Cl 3 is higher than that of [Au 11 (PPh 3 ) 8 Cl 2 ]Cl. Under the same conditions, the two Au 11 clusters exhibit much higher catalytic activity than larger clusters (Au 25 , Au 38 and Au 144 ) capped with phenylethiolates, as a manifestation of both size influence and surface ligand impacts. In addition, the oxidation efficiency of styrene exhibit a sharp increase when tert-butyl hydroperoxide is utilized as the oxidant, where the catalytic activities of Au 11 (PPh 3 ) 7 Cl 3 and [Au 11 (PPh 3 ) 8 Cl 2 ]Cl are comparable with styrene epoxide being the major product. Finally, the twin clusters are either reduced or oxidized to probe the charge effects upon the catalytic reaction, and it was found that the conversion of styrene went up with the charge state from reduced to oxidized for both clusters.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Linghui Zhao,Yufan Chen,Yong Feng,Deli Wu
In this study, three GR/Cu(II) (Green Rust/Cu(II)) composites (GR SO4 /Cu(II), GR CO3 /Cu(II), and GR Cl /Cu(II)) were synthesized and used to activate dioxygen under weakly acidic conditions. The change in the mechanism caused by three interlayer anions, CO 3 2− , SO 4 2− , and Cl − , was discussed for the first time. Both Cu(I) and H 2 O 2 were generated during GR/Cu(II)-induced dioxygen activation, resulting in the rapid degradation of acetaminophen. The inconsistency between the reaction constant rates and oxidation reduction potential (ORP) order revealed the effects of the various types of interlayer ions. To further reveal the effects of the anions, the variations in the morphology and valence states of the composites were examined. To identify the rate-controlling step of dioxygen activation by the three composites, the production of reactive oxygen species (ROS) was investigated and compared. The combination of interlayer anions and metal ions changed the oxide morphology of the solid-phase materials. Furthermore, changes in the content of the reductive species (Fe(II) or Cu(I)) either enhanced or inhibited specific reaction steps. The results from this study could deepen our understanding of the effects of anions on dioxygen activation by transition metals and provide a basis for the study of oxidation reactions and mechanisms in the presence of various anions.
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RSC Advances
·
2015
·Vol. 5
·期 79
·64358-64367
·
IF 3.84
Jian Cheng,Yan Dong,Hui Ma,Lixia Li,Zuliang Liu,Fengqi Zhao,Siyu Xu
A one-dimensional energetic complex (Na[CL-14·2H2O]) constructed from sodium and 5,7-diamino-4,6-dinitrobenzofuroxan (CL-14) was synthesized, and its crystal structure was analyzed by X-ray diffraction. The crystal belongs to a monoclinic system with space group P21/c. The complex possesses a one-dimensional coordination framework based on the [ONaN]n chain, which might result in its low sensitivity and high heat resistant. The thermal decomposition mechanism of Na[CL-14·2H2O] was predicted by means of TG-DSC, TG-MS and FTIR analyses. The thermal decomposition of Na[CL-14·2H2O] contains one endothermic and one exothermic processes in the temperature range of 25–500 °C with NaNCO, Na2CO3, H2O, NO and CO2 as the final products. The non-isothermal kinetic and thermodynamic parameters for the first exothermic process of the Na[CL-14·2H2O] have been studied, with the apparent activation energy, pre-exponential factor, entropy of activation, enthalpy of activation and free energy of activation of 280.7 kJ mol−1, 57.8, 282.7 J mol−1 K−1, 276.2 kJ mol−1 and 154.8 kJ mol−1, respectively. The impact sensitivity and friction sensitivity of Na[CL-14·2H2O] was tested according to general methods, with the values of 27 J and 360 N, respectively. Na[CL-14·2H2O] has been investigated as an energetic catalyst in ammonium nitrate (AN) by means of TG-DTG, TG-MS, DSC and extent of conversion (α)–T kinetic curve analyses. And the thermal kinetic constants for the catalytic and noncatalytic decomposition of AN samples were calculated using Kissinger's and Ozawa–Doyle's equations. The possible catalytic mechanism was also discussed and proposed. The results show that Na[CL-14·2H2O] decreases the peak temperature and activation energy value of the complete decomposition process for AN by 41.3 °C and 10.9 kJ mol−1, respectively. Furthermore, the thermal decomposition of AN in the presence of Na[CL-14·2H2O] starts at significantly lower temperature (about 30 °C) than that of pure AN. Apparently, Na[CL-14·2H2O] could be incorporated as a potential energetic catalyst in AN-based propellants.
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CATALYSIS LETTERS
·
2015
·Vol. 145
·期 10
·1913-1921
·
IF 2.307
Wu Jing,Zhi Yunfei,Shan Shaoyun,Su Hongying,Wu Shuisheng,Jia Qingming
Abstract Polypyrrole(PPy) supported Cr(III)(salen)Cl catalyst was prepared for alternating copolymerization of cyclohexene oxide and carbon dioxide. The supported catalyst and the copolymerization products were characterized by FTIR, XRD, XPS, ICP-MS, SEM, TEM, NMR, gel permeation chromatography, thermogravimetric analysis and differential scanning calorimetry. After the study, we concluded that the homogeneous Cr(III)(salen)Cl is successfully supported on the PPy, and its catalytic performance is much better than the homogeneous one. Moreover, the copolymerization product catalyzed by PPy-Cr(III)(salen)Cl exhibits higher molecular weight, narrower molecular weight distribution, superior thermal stability and selectivity. Graphical Abstract
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高影响因子
EUROPEAN POLYMER JOURNAL
·
2015
·
IF 3.005
Erjun Tang,Kaidi Du,Xiaoyan Feng,Miao Yuan,Shaojie Liu,Dishun Zhao
The pH-responsive cellulose-g-poly[2-(diethylamino)-ethyl methacrylate] (cellulose-g-PDEAEMA) copolymers were successfully synthesized by atom transfer radical polymerization (ATRP) in the ionic liquid 1-allyl-3-methylimidazolium chloride ([AMIM]Cl). As the functional monomer 2-(diethylamino)ethyl methacrylate (DEAEMA) hardly dissolved in [AMIM]Cl, we used ethyl alcohol as the cosolvent to increase its solubility and thereby form a homogeneous system. Compared with the synthetic mechanism for the heterogeneous system, generation of the byproduct poly[2-(diethylamino)ethyl methacrylate] (PDEAEMA) in the homogeneous system was reduced and the ATRP reaction was easily controlled. Optimum reaction condition was attained at the CuBr/PMDETA/DEAEMA/ethyl alcohol molar ratio of 1:15:150:300. Kinetic analysis confirmed the reaction was living and controllable. Cellulose-g-PDEAEMA was characterized through FTIR, 1 H NMR, TEM and GPC. The results showed that the PDEAEMA brush was covalently bonded to the cellulose backbone and its molecular weight distribution was narrow. In addition, the resultant copolymer could self-assemble into spherical micelles and showed the pH-sensitivity, implying its potential application as biomedical materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ping Ye,Heng Ding,Bo Yang,Weimiao Wang,Xiaodong Li,Zhiqiang Qiao,Rui Li,Guangcheng Yang,Guoqing Lv
The ignition strategy of energetic materials using low-energy near-infrared (NIR) laser has garnered significant attention due to its enhanced safety and reliability. This study explores the use of a relatively photosensitive but mechanical insensitive energetic material, DATNBI, to facilitate the self-assembly of nano-CL-20 crystals into polycrystalline particles though solvothermal induction, yielding a rough structure conducive to NIR laser ignition. The findings demonstrate that by adjusting the content of DATNBI, it is possible to achieve micro-nano controllable spherical CL-20/DATNBI (C/D) particles, with CL-20 as the primary component and DATNBI as the auxiliary component. The incorporation of DATNBI and the rough surface structure enhance the light absorption of C/D particles in the NIR band. Additionally, the unique synergistic effect between CL-20 and DATNBI during thermal decomposition further promotes NIR laser ignition. As expected, the C/D particles achieved self-sustained combustion and exhibited excellent combustion performance under a 1064 nm laser, which is challenging to be achieved with raw CL-20 or raw DATNBI. Furthermore, the relatively insensitive DATNBI and spherical structure reduced the impact sensitivity of the C/D particles. This multifunctional material strategy, integrating energy, safety, environment-friendliness, and laser ignition performance, offers a novel approach for laser ignition of energetic materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Feng Gao,Jingcun Shao,Yanting Tang,Yajie Tian,Lin Sun,Xin Yu
To address the escalating concerns related to organic pollutions in aquatic environments, there is an urgent demand for exploring an efficient and eco-friendly method for the removal of organic pollutants. In this work, porous Cl-C 3 N 4 (ClCN)and step-scheme (S-Scheme) Cl-C 3 N 4 /WO 3 (ClCN/WO 3 ) composites have been designed and fabricated through a facile calcination approach for tetracycline removal under visible-light irradiation. The synthesized S-Scheme ClCN/WO 3 composites exhibited porous structures, though their visible-light absorption was lower compared to the ClCN and C 3 N 4 samples. The surface areas of the ClCN/WO 3 composites can reach 81.43 m 2 g −1 , significantly higher than that of the ClCN and C 3 N 4 samples. These composites also demonstrated prolonged carrier lifetime and improved charge separation efficiency, primarily due to the formation of S-Scheme heterostructures. Among the prepared samples, the ClCN/WO 3 -2 composite demonstrated the highest photocatalytic activity with a rate constant reaching 0.0547 min −1 , approximately 4.56 times that of pristine C 3 N 4 . Additionally, when applied to tetracycline degradation in simulated seawater, the ClCN/WO 3 -2 composite achieved a rate constant of 0.047 min −1 , outperforming the C 3 N 4 and ClCN samples. Mechanistic studies showed that the S-Scheme heterostructures markedly promoted charge separation and tetracycline degradation. Furthermore, the ClCN/WO 3 composites contributed to a reduced the biological toxicity of the degraded intermediates. This study underscores the immense potential of ClCN/WO 3 composites as high-performance photocatalysts for the photodegradation of organic pollutants under visible-light irradiation.
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RARE METALS
·
2024
·
IF 9.6
Hu Xiao-Jie,Sun Yu-Han,Liu Ling-Yue,Mao Dan-Jun,Zheng Shou-Rong
Monochloroacetic acid (MCAA) is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water. In this study, a series of CeO 2 -supported Pd catalysts (Pd/MCeO 2 ) were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC (Ce-MOF), and the liquid-phase catalytic hydrodechlorination of MCAA was explored using these catalysts. For comparison, Pd/CeO 2 catalysts were additionally synthesized using the conventional impregnation method. The characterization results reveal that the catalysts exhibit strong metal–support interaction, leading to high Pd dispersion and Pd n + content. Additionally, the calcination temperature significantly influences catalytic performance, with the catalyst calcined at 500 °C (Pd/MCeO 2 -500) demonstrating the highest catalytic activity and achieving complete dechlorination of MCAA within 50 min. Furthermore, it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir–Hinshelwood model. Accordingly, low reaction pH is favorable for the catalytic hydrodechlorination of MCAA, enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface. Theoretical results suggest that the presence of Pd n + efficiently facilitates MCAA adsorption and C–Cl cleavage, thus significantly enhancing the liquid-phase catalytic hydrodechlorination. Graphical abstract
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