RSC Advances
·
2015
·Vol. 5
·期 89
·73083-73090
·
IF 3.84
Kuiyi You,Renjie Deng,Jian Jian,Pingle Liu,Qiuhong Ai,He’an Luo
Developing a new environmentally friendly process for benzene nitration to nitrobenzene has been highly desirable for a long time. In this work, NO2 was used as a nitration agent to replace traditional nitric acid, and different mesoporous SiO2 and their supported heteropoly acid (salt) were employed to catalyze benzene nitration to nitrobenzene. Several typical catalysts were characterized using XRD, BET and FT-IR, and the acid amounts of the various catalysts were determined. The effects of various factors such as different catalysts, the molar ratio of benzene to NO2, reaction temperature, reaction time, HPW loading, the acid amounts of the catalyst and the reuse of the catalyst on the nitration reaction have also been systematically examined. The results indicate that the supported HPW/MCM-41 catalysts exhibit a remarkably synergistic catalytic performance on the nitration reaction of benzene to nitrobenzene. In particular, the 50%HPW/MCM-41 catalyst gives the best results with 73.4% benzene conversion and 98.8% selectivity to nitrobenzene under the optimal reaction conditions. Moreover, the mesoporous structure of MCM-41 was retained under the high loading of HPW. The possible reaction mechanism for the nitration reaction of benzene with NO2 over HPW/MCM-41 is suggested in the present work. This method provides a promising strategy for the preparation of nitro-aromatic compounds from a catalytic nitration reaction by using NO2 as the nitration reagent.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Lu Li,Sihong Xu,Liang Jin,Wenxing Chen,Shichang Chen
It is essential to find a depolymerization system with good catalytic activity, easy operation, and high efficiency for the degradation of waste PET. The synergistic catalytic effect of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) and zinc 2-ethylhexanoate (ZnEH) in PET glycolysis was investigated. Waste PET can be more efficient when completely degraded than single organocatalyst or zinc salt or previous DBU/Zn(OAc) 2 , and the yield of BHET reaches 84.1 % under optimal reaction conditions with the molar ratio of 2:1 of DBU to ZnEH and the weight ratio of 3:1 of EG to PET, the temperature of 180 °C and at 60 minutes. By combining experimental results with density functional theory (DFT) calculations, the synergistic enhancing degradation mechanism that generates hydrogen and coordination bonds is proposed. The purified depolymerization product of BHET was repolymerized to PET, delightfully the r-PET was almost identical to virgin PET.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 5
·2192-2200
·
IF 5.503
Zhewen Ma,Qiuyu Zhang,Wen Zhu,Darvaish Khan,Chuanzhu Hu,Tianping Huang,Wenjiang Ding,Jianxin Zou
TMA-TM (TM = Fe, Ni) MOFs were synthesized successfully by a facile method. A MgH2-TM MOF (TM = Fe, Ni) composite was obtained via ball milling and the corresponding hydrogen storage performance was investigated. Particularly, high-resolution transmission electron microscopy was performed to in situ characterize the dehydrogenation behavior of the MgH2-TM MOF composite. The results reveal that nano α-Fe and Mg2NiH4/Mg2Ni derived from the TMA-TM MOFs display a synergetic improving effect on the de/hydrogenation of MgH2. During the hydrogen desorption process, Mg2NiH4/Mg2Ni works as a “hydrogen pump” to quickly deliver hydrogen and facilitates hydrogen diffusion. Meanwhile, α-Fe accelerates the nucleation and growth of Mg by reducing the nucleation energy of Mg from MgH2. The hydriding activation energy of the MgH2-TM MOF declines to 45.3 kJ mol−1 H2. Meanwhile, the peak dehydriding temperature of the MgH2-TM MOF is 530.9 K, which is much lower compared with the MgH2–Fe MOF composite (541.7 K) and as-milled MgH2 (685.2 K). Therefore, nano Mg2Ni and α-Fe derived from the TMA-TM MOFs can remarkably improve the hydrogen storage properties of the MgH2/Mg system due to their synergetic catalytic effects.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
ACS Omega
·
2023
·
IF 4.1
Yanghao Meng,Hongbiao Du,Shuai Lu,Yanwei Liu,Jinglai Zhang,Hualong Li
Hydrothermal liquefaction (HTL) is one of the most promising technologies for biofuel production. The preparation and application of catalysts for HTL have been the research focus in recent years. In this study, a new synergistic catalytic process strategy is proposed. CuO–CeO2/γ-Al2O3 was used as an in situ hydrogen donor catalyst and Ni–Co/SAPO-34 was synthesized for hydroprocessing to improve bio-oil production process. The results of XRD and XPS demonstrated that the metal components were well supported on the catalyst. When the two catalysts were mixed, the yield of bio-oil increased from 51.00% to 64.51%, the carbon recovery rate raised from 69.53% to 88.18%, the energy recovery rate grew from 63.42% to 80.22%, and the S content is relatively reduced by 83.3%. Also, TG analysis showed that the content of light components in bio-oil increased. Moreover, the hydrocarbons and alcohols were observed to a higher proportion from the GC-MS analysis. This new method still has high catalytic activity after repeated use for five times. This study provides a new idea for preparing higher yield and superior quality bio-oil.
研究领域:
能源生物学
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催化化学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Siao Li,Weisong Yan,Changyi Yang,Yanshu Zhu,Ying Liu,Yaohua Gu,Zhiqiang Wu,Keren Shi,Huiqin Yao
Acridine , as a nitrogen heterocyclic pollutant, poses a huge ecological and human health hazard, and its efficient degradation is one of the top tasks. A novel photo-enzyme-coupled catalytic system was constructed by coupling horseradish peroxidase (HRP) with graphite carbon nitride (g-C 3 N 4 ) through a simple inorganic hybridization process. The obtained g-C 3 N 4 /HRP nanoflowers not only increase the enzyme loading capacity and enzyme activity , but also promote the efficient separation of carriers. More importantly, the H 2 O 2 generated by g-C 3 N 4 directly participates in the redox cycle reaction of HRP, inducing photo-enzyme synergistic catalysis. Therefore, compared to HRP nanoflowers and g-C 3 N 4 nanoflowers, g-C 3 N 4 /HRP nanoflowers exhibited higher catalytic efficiency for the degradation of acridine. Thus, the photo-enzyme coupled catalyst proposed in this study provides a promising platform for the degradation of acridine pollutants by combining enzymes with photocatalysts through inorganic hybridization.
研究领域:
环境科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Na Wu,Xiaoqiang Du
One of the most attractive means for mitigation of environmental pollution is to produce hydrogen by electrocatalytic urea splitting. In the paper, the heterogeneous interfacial rich N–CuCo 2 S 4 @Ni 3 S 2 material was in situ synthesized on nickel foam through a typical hydrothermal and sulfuration process. This N–CuCo 2 S 4 @Ni 3 S 2 electrode displays excellent urea oxidation performance (potential of 1.38 V@50 mA cm −2 ), which is one of the best reactivity reported so far. Experimental results show that the superior catalytic activity is attributed to the rapid charge transfer, more reaction center exposed and superior electrical conductivity . Density functional theory shows that this Ni 3 S 2 material accelerates the reaction rate in the catalytic process, the introduction of this N–CuCo 2 S 4 material improves the conductivity of the material, and the synergistic catalysis of the N–CuCo 2 S 4 and Ni 3 S 2 makes this N–CuCo 2 S 4 @Ni 3 S 2 material exhibit superior urea oxidation activity. Notably, long-term tests have shown a decrease in catalytic activity, which suggests that the surface of the sulfide is in situ generated to oxides or hydroxides, which are truly active species. This work provides a new idea for the development of efficient and stable urea oxidation catalysts for sulfides.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Qinglian Wang,Huaiyu Wang,Jintian Zhong,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
Deep desulfurization of fuel oil is always a highly challenging issue. In this work, ZrXPTA material was obtained by directly combining the ZrIV active site with PTA, and it was found that ZrXPTA has excellent catalytic activity in the oxidative desulfurization (ODS) process. Further, ZrXPTA was loaded on γ-Al2O3 by the two-step impregnation to obtain a granular Al2O3@ZrXPTA composite. The successful synthesis of the material was verified by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), and N2 adsorption–desorption. The results show that Al2O3@ZrXPTA maintains the high ODS activity of ZrXPTA and realizes the rapid and complete removal of dibenzothiophene under mild reaction conditions (T = 40 °C, O/S = 4, t = 30 min). The mechanism study shows that the ODS activity of Al2O3@ZrXPTA is wholly derived from the counterpart of ZrXPTA, which benefits from the synergistic catalytic effect between the ZrIV active site and PTA. The direct binding of these two active sites makes the synergistic effect fully exerted. In addition, the recovery of Al2O3@ZrXPTA can be easily realized by simple filtration or decantation, and no significant activity loss was observed after five times recycling. Therefore, Al2O3@ZrXPTA has high ODS activity, high catalytic stability, and great potential as an ODS catalyst in practical applications.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Lihong Ding,Xiuliang Sun,Chongpin Huang,Jianwei Li,Biaohua Chen
Cumyl hydroperoxide (CHP) is an important intermediate in phenol/acetone production; however, its long reaction time and low yield remain industrial challenges. In this study, an active and promising catalyst combination—NHPI + BmimBr ionic liquid (IL)—was developed for cumene oxidation under solvent-, transition-metal-salt-, and CHP-initiator-free conditions, which exhibited a synergistic catalytic effect and excellent catalytic performance. The cumene oxidation rate was accelerated by 33.3 %, leading to the rapid synthesis of a significant amount of the target product, CHP. DFT calculations demonstrated that NHPI undergoes hydrogen atom abstraction reaction through its interaction with BmimBr, forming PINO and carbene-Br radicals that can extract hydrogen. Additionally, EPR analysis demonstrated that both radicals are involved in the reaction. The nature of the synergistic effect was confirmed using theoretical and experimental approaches. The proposed catalyst eliminates the requirement of an initiator for IL and NHPI application, paving the way for the efficient production of CHP without solvents or initiators.
研究领域:
化学工程
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催化化学
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Tao Lv,Kexin Wei,Ting Wang,Xiao Wang,Zuguang Liu
A carbon-based acid was prepared by the sulfonation of activated carbon derived from eucalyptus wood waste, a solid waste from wood processing, and characterized by SEM, BET, FT-IR, Raman, XRD and XPS. Due to activation by phosphoric acid and subsequent sulfonation, the resultant carbon-based solid acid can obtain a porous structure, medium surface area and abundant functional groups including sulfonic groups, carboxyl, hydroxyl and other oxygen-containing groups, which provides excellent mass transfer channels and sufficient reactive sites for catalytic reactions. So, the carbon-based solid acid showed excellent catalytic performance for converting α -pinene to camphene with a conversion of up to 99.8 % and a selectivity of 51.2 %, respectively. Quantum chemical theoretical calculations (electrostatic potential, Gibbs free enthalpy of intermediates, molecular size) are used to further analyze the catalytic mechanism of carbon-based solid acids. Theoretical analysis of the carbon positive ions and their energies as well as experimental results under electron-donating co-catalysts suggests that oxygen-containing functional groups on carbon-based solid acids play an important role in improving α- pinene adsorption onto catalyst as well as camphene selectivity. This work provides a promising approach for converting α -pinene to camphene catalyzed by carbon-based solid catalyst.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 4
·1871-1882
·
IF 10.182
Xiaoling Qu,Guangyuan Zhou,Rui Wang,Bolei Yuan,Min Jiang,Jun Tang
Alcoholysis is a potential method for the degradation of polyesters to their precursor building blocks, which can then be polymerized again to form new qualified polyester materials. This method therefore makes recycling possible in a permanent polymer–monomer–polymer loop. In this study, a series of metal-free tetrabutylphosphonium-based ionic liquids (ILs) were prepared as catalysts for the methanolysis of poly(ethylene 2,5-furandicarboxylate) (PEF), which is well known as an ideal alternative to the petroleum-based plastic poly(ethylene terephthalate) (PET). It was found that anions with stronger electronegativity were more efficient for the methanolysis of PEF. By adjusting the structures of the anions and cations of ILs, 1-butyl-3-methylimidazole acetate ([BMIm][OAc]) exhibited excellent catalytic activity in the methanolysis of PEF. The optimization of reaction parameters enabled the [BMIm][OAc]-catalyzed methanolysis of PEF with nearly 100% PEF degradation and a 77.6% dimethyl furan-2,5-dicarboxylate (DMFD) yield at 130 °C for 30 min. Furthermore, [BMIm][OAc] could keep high-activity after using for six times under the optimum conditions. Assisting with 1H NMR, FT-IR and density functional theory (DFT) calculations, an in-depth study was performed on the feasible synergetic catalytic mechanism of [BMIm][OAc] for the methanolysis of PEF, induced by hydrogen bonds formed between reactants and [BMIm][OAc]. Finally, on the basis of experimental results and scanning electron microscopy (SEM), it was confirmed that PEF with the spiral motif could be degraded under milder conditions than PET. Therefore, this strategy of using adjustable cation and anion structures in ILs provides an opportunity to develop other more efficient ILs for the alcoholysis of furan-based polymers via a green and mild pathway.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Xuqiang Zhao,Lei Tang,Xuwen Chen,Jian Wang,Yanzheng Gao
Phthalic acid esters (PAEs) as common plasticizers, providing convenience to humans. However, they also present a potential threat to ecosystems and human health as emerging contaminants. In this study, co-immobilization of nanozyme (PtCo) and laccase (Lac) into dendritic mesoporous silica (DMSN) constitutes nanomaterials (Lac@PtCo@DMSN). PtCo with an atomic ratio of 3:1 has the highest oxidizing activity. DMSN exhibited a maximum Lac loading capacity of 365 mg/g and activity of Lac@PtCo@DMSN exhibits excellent pH, temperature, and storage stability and reusability, and demonstrated greater recoverability. Remarkably, Lac@PtCo@DMSN (50 mg) achieved 81.83% degradation of total PAEs within 72 h and maintained 72.44% degradation of dimethyl phthalate (DMP) in the fifth cycle. Electron transfer between Pt, Co and adsorbed oxygen (O 2ads ) in PtCo can generate •OH and •O 2 − , which were the dominant reactants for PAEs degradation. •OH could degrade PAEs to phthalic acid via H-abstration and •OH addition. •OH effectively enhanced Lac activity, and promoted the synergistic catalytic performance of nanozymes and natural enzymes. The degradation of phthalic acid by Lac accelerated the release of PtCo@DMSN reaction sites, resulting in significantly enhanced PAEs degradation. Thus, artificial/natural enzymes can degrade PAEs without exogenous additives to solve the limitation of Lac application, providing a new strategy for degrading contaminants in water.
研究领域:
环境科学
·
生物化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Danni Zeng,Tingzhe Shen,Yadong Hu,Fengjiao Liu,Ze Liu,Jun Song,Rongfeng Guan,Changjian Zhou
Photothermal synergistic catalysis is a novel technology that converts energy. In this study, ZnIn 2 S 4 with S-vacancy (ZIS-Vs) is combined with Nickel, Nickle Oxide and Carbon Nanofiber aggregates (Ni-NiO@CNFs) to create a multi-interface coupled photocatalyst with double Schottky barrier, double channel and mixed photothermal conversion effect. Theoretical calculation confirms that the Gibbs free energy (ΔG *H ) of the S-scheme heterojunction in the composite material is −0.07 eV, which is close to 0. This promotes the adsorption of H* and accelerates the formation of H 2 . Internal photothermal catalysis is achieved by visible-near infrared (Vis-NIR, RT) irradiation. The internal photothermal catalytic hydrogen production rate of the best sample (0.9Ni-NiO@CNFs/ZIS-Vs) is as high as 17.24 mmol·g −1 ·h −1 , and its photothermal conversion efficiency (η) is as high as 61.42 %. Its hydrogen production efficiency is 20.52 times that of ZIS-Vs (0.84 mmol·g −1 ·h −1 ) under visible light (Vis, RT) conditions. When the Vis-NIR light source is combined with external heating (75 ℃), the hydrogen production efficiency is further improved, and the hydrogen production efficiency (29.16 mmol·g −1 ·h −1 ) is 26.75 times that of ZIS-Vs (1.09 mmol·g −1 ·h −1 , Vis-NIR, RT). Further analysis shows that the increase in hydrogen production resulted from the apparent activation energy (Ea) of the catalyst decreasing from 16.7 kJ·mol −1 to 9.28 kJ·mol −1 . This study provides a valuable prototype for the design of an efficient photothermal synergistic catalytic system.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）