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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DOI
PubMed
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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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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高影响因子
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
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
·
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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高影响因子
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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高影响因子
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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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120487
·
IF 7.2
Jifang Zhang,Chengcheng Suo,Hongru Zhang,Wei Li,Sha Luo,Bing Tian,Chunhui Ma,Shouxin Liu
Constructing an efficient and low-cost electrocatalyst was highly necessary in electrocatalytic lignin depolymerization study. We prepared a unique 1D/2D/1D nanoflower electrocatalyst (Ti 20 @ZIS-Sv@C 0.5 (Ⅱ)) composed of TiO 2 , ZnIn 2 S 4 and C nanosheets by electrostatic self-assembly through solvothermal method. The TiO 2 was located as the core of catalyst and covered by the C deposited ZnIn 2 S 4 nanosheets. The electrochemical impedance (R ct , 248.5 Ω; R L , 6.511 Ω), C dl (1.75817 mF cm −2 ), Tafel efficiency (6.28 mV dec −1 ) and photocurrent intensity (5.23 μA) of Ti 20 @ZIS-Sv@C 0.5 (Ⅱ) exhibited higher electrocatalytic activity than that of original ZnIn 2 S 4 . Under optimized conditions, electrocatalytic process achieved 100 % C α -C β (β-O-4) and C Ar -O (α-O-4) cleavage efficiency and 244.37 mg g −1 benzaldehyde yield. We have further indicated C α -C β (β-O-4) and C Ar -O (α-O-4) cleavage mechanism by Cl-induced radical oxidation pathway. The electrocatalytic depolymerization of G-type lignin could obtained at least 14 molecular products (including 18.21 mg g −1 2-hydroxy-1-phenylethan-one, 11.39 mg g −1 pyrocatechol and 1.25 mg g −1 benzaldehyde). Mechanism investigation suggested the generation of chlorine radical (•Cl), followed by C-H activation and synergistic effect of Ti 20 @ZIS-Sv@C 0.5 (Ⅱ), leading to highly efficient lignin linkages cleavage. This work has developed an efficient electrocatalyst for lignin valorisation to produce aromatics via an electrocatalytic radical pathway.
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高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Lei Zhou,Xin Wei,Junxiang Zhang,Xuecui Mei,Yun Li,Chaoyue Zheng,Furong Zhang,An Wen,Bin Wang
Sulfide solid electrolytes (SSEs) have some huge advantages in high room-temperature conductivity, good thermal stability, low interfacial resistance, etc. They are one of the ideal solid electrolytes for developing high energy density and high safety for all-solid-state lithium batteries (ASSLBs). However, the preparation of SSEs requires expensive Li2S as the raw material, whose high cost limits its practical application. Herein, a cost-effective SSE Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) was designed and prepared by using low-cost lithium and sulfur instead of expensive Li2S. Significantly, the cost of SSEs was reduced from $169.72 to $28.13 kg–1 based on replacing the Li2S strategy. Moreover, the prepared Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) solid electrolytes have a high ionic conductivity of 1.86–2.73 mS cm–1 at room temperature and a high voltage window of 5 V. On this basis, we assembled the all-solid-state lithium battery TiS2/Li7.3P2.9S10.75I0.3/Li–In, which presented a high initial discharge capacity of 219 mA h g–1 at room temperature and satisfactory cycle stability with a capacity retention of 86.7% after 100 cycles at 0.50 mA cm–2. This work provides an effective strategy for reducing the cost of SSEs, advancing the practical process of ASSLBs.
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高影响因子
EUROPEAN POLYMER JOURNAL
·
2018
·
IF 3.741
Teng Xue,Erjun Tang,Xiaofeng Guo,Ruihong Wang,Lei Zhao,Jian Zhou,Shaojie Liu
The ionic liquid 1-(triethylene-tetramine)ethyl-3-methyl chloride ([N 4 MIM]Cl) was first prepared to replace the organic ligand coordinating with CuBr to catalyze atom-transfer radical polymerization (ATRP) in ionic liquid system. [N 4 MIM]Cl was synthesized via the intermediate IL 1-chloroethyl-3-methyl chloride ([CeMIM]Cl) reacting with the aliphatic amine triethylene tetramine (TETA) and [CeMIM]Cl) was obtained by N′-alkylation of N -methylimidazole with 1,2-dichloroethane. This catalyst has been applied to the ATRP of methyl methacrylate (MMA) in the ionic liquid (IL) 1-allyl-3-methylimidazolium chloride ([AMIM]Cl) and presented a perfect catalytic performance. The chemical structures of the ILs obtained were confirmed by FTIR and 1 H NMR. The coordination ability of [N 4 MIM]Cl was assessed by cyclic voltammetry (CV) and its coordination mechanism towards CuBr was discussed. The [N 4 MIM]Cl/CuBr catalyst system showed good controllability in the aforementioned ATRP reaction in [AMIM]Cl. The amount of residual Cu 2+ in the polymer product was determined by atomic absorption spectrometry (AAS) and the result showed that the Cu catalyst was easily separated from the obtained polymer. Thus, the coordinating IL could overcome the shortcomings of traditional organic ligands, such as poor compatibility with IL media resulting in the weakly catalytic performance and inferior separation of the catalyst from the polymer. It implied that the coordinating ionic liquid ([N 4 MIM]Cl) has highly promising application in the ATRP of ionic liquid system.
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Menglu Wang,Bolong Liang,Shumin Lin,Zhe Zhao,Hongbin He,Xiliang Li,Shu-xuan Liang
The magnetic Fe 3 O 4 @ZIF-8 with high adsorption properties and easy separation were embedded in BiOX (X = Cl, Br, I) to synthesize Fe 3 O 4 @ZIF-8@BiOX using a simple one-pot solvothermal strategy. The crystal structure, surface morphology, photoelectric properties, thermal stability and magnetic response of the three materials were compared and analyzed, and the effect on the removal of OTC and Cr(VI) from single and coexisting systems by adsorption-photocatalysis is discussed. The results show Fe 3 O 4 @ZIF-8@BiOI has the highest separation efficiency of photogenerated carriers upon photoexcitation and stronger light absorption capacity, and exhibits better adsorption-photocatalytic activity than the other two materials in the photocatalytic reduction of Cr(VI) (68 % and 65 % removal for single and coexisting systems) and degradation of OTC (86 % and 59 % removal for single and coexisting systems). It is noteworthy that in the coexistence of Cr(VI) and OTC, a slight decrease of removal occurred, which could be due to a competitive effect between two pollutants being greater than the synergistic effect. ∙O 2 - is the main active substances in the adsorption-photocatalysis process. Finally, this work demonstrates the excellent adsorption and photocatalytic ability of Fe 3 O 4 @ZIF-8@BiOI for the simultaneous removal of Cr(VI) and OTC, which has great potential for practical wastewater treatment.
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高影响因子
危险品化学品经营许可证（带存储）