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.
✓ 已验证
产品关联
DOI
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
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
✓ 已验证
产品关联
DOI
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.
✓ 已验证
产品关联
DOI
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.
✓ 已验证
产品关联
DOI
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.
✓ 已验证
产品关联
DOI
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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL RESEARCH
·
2020
·
IF 0.593
Zhenzhen Geng,Hong-yu Zhang,Guohui Yin,Yuecheng Zhang,Jiquan Zhao
The ionic liquid 1-methyl-3-(3-sulfopropyl)imidazolium chloride ([MIMPs]+Cl-) in combination with 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) and sodium nitrite (NaNO2) as a catalytic system demonstrates high efficiency in the one-pot two-step aerobic oxidative condensation of benzyl alcohols with 1,2-phenylenediamines to give benzimidazoles. Various benzimidazoles are obtained in good to excellent yields by this strategy.
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Linjie Wang,Xuechao Xu,Peng Liu,Mengzhu Wang,Xiangheng Niu,Jianming Pan
Abnormal levels of halide ions in drinking water have enormous threats to human health, and thus designing reliable and sensitive methods to quantify and distinguish these ions becomes extremely crucial. Herein, we develop a single-nanozyme colorimetric array based on target-induced differential surface passivation for the quantification and discrimination of Cl − , Br − and I − ions. Silver citrate (Ag 3 Cit) is designed as an oxidase mimic to efficiently catalyze the 3,3′,5,5′-tetramethylbenzidine (TMB) chromogenic reaction. When halide ions (Cl − , Br − and I − ) are present, due to their different precipitation interactions with the Ag(Ⅰ) entity in Ag 3 Cit, they can passivate the active surface of the nanozyme to various degrees, resulting in the inhibited TMB chromogenic reaction differentially. According to this principle, simple and efficient quantitative detection of Cl − , Br − and I − ions was achieved, with all the detection limits down to the nM level. By employing Ag 3 Cit as a single sensing element, a nanozyme catalysis-based colorimetric array was further established, and both individual and mixed ions were successfully distinguished by integrating the array with principal component analysis . Accurate identification of unknown samples was also verified via a double-blind protocol, indicating potential applications of the array in practice.
✓ 已验证
DOI
PubMed
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.
✓ 已验证
DOI
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.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）