Molecular Catalysis
·
2025
·
IF 4.9
Yibo Zhang,Yang Liu,Wei Wang,Chunlai Liu,Hongyu Zhou,Na Wang,Jianglei Hu,Fengwei Shi
Metal-organic framework (MOF)-based composites have received significant attention for catalytic applications and are believed excellent heterogeneous catalysts. In this article, we prepared a new type of material, HPW@MOF-199/SBA-15C (PMS-15C). For this material, the MOF-199 encapsulating Keggin-type phosphotungstic acid (HPW) was grown inside the pores of the SBA-15 functionalized by carboxylic acids. The N 2 adsorption-desorption isotherms and pore size distributions, X-ray powder diffraction, transmission electron microscopy, and scanning electron microscopy analyses showed that the PMS-15C composites had an ordered two-dimensional hexagonal mesoporous structure, in which HPW encapsulating by MOF-199 loaded into the SBA-15C. Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy indicated that HPW was successfully loaded, and the Keggin structure of HPW in PMS-15C remained unchanged. With the reaction of acetic acid and ethanol, the catalytic performance of PMS-15C was studied. Under the optimal conditions, ethyl acetate yield reached 81.4 %. The forward reaction rate was 0.432 mL mol −1 min −1 , and the activation energy was 38.35 kJ mol −1 . And the data were found to be consistent with the second-order reversible reaction kinetic model. The catalytic activity of the PMS-15C-0.2 composites remained stable after five catalytic cycles. In addition, the esterification of n-octanol/acetic acid and ethanol/oleic acid were studied using PMS-15C-0.2 as the catalyst. The results suggested that the catalytic activity of PMS-15C-0.2 was weakened upon increasing the substrates’ alkyl chain length.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Shi Jia Li,Guang Tao Fei,Shao Hui Xu,Wen Chao Chen,Hai Yan Xu,Xiao Xuan Qu,Xin Feng Li,Hao Miao Ouyang
Poly (ethylene oxide) (PEO)-based solid-state electrolytes are the most researched and widely used polymer solid-state electrolytes, but their ionic conductivity, electrochemical stability window, and cycling stability all need further improvement. In this work, 15 Crown ether 5 and the high concentration of lithium salts are added into PEO solid-state electrolytes using a solution-casting approach. The resulting solid-state electrolyte exhibits an ionic conductivity of 3.14 × 10 −3 S cm −1 at 60 °C and an electrochemical stability window exceeding 5.2 V. The assembled Li//Li symmetric battery can be stably cycled for over 850 h at a current of 0.1 mA cm −2 , and the LiFePO 4 //Li battery has an initial discharge capacity of 144 mA h g −1 at 2C rate, retaining 85 % of its capacity after 800 cycles. By optimizing the solid-state electrolyte components, Li//Li symmetric batteries can achieve cycling stability for up to 2200 h, and LiFePO 4 //Li batteries can endure up to 2000 cycles at a 2C rate and 4800 cycles at a 5C rate. Moreover, the prepared solid-state electrolyte can be matched with a high-voltage cathode electrode, offering a wide range of potential applications and promising commercialization prospects.
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高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 35
·期 45
·2304285
·
IF 29.4
Yiqi Wei,Yaxiong Yang,Zichong Chen,Panyu Gao,Qihang Ma,Mingxi Gao,Chenhui Yan,Zhijun Wu,Yinzhu Jiang,Jian Chen,Xuebin Yu,Zhenglong Li,Xin Zhang,Yongfeng Liu,Mingxia Gao,Wenping Sun,Hongge Pan
LiBH 4 is a promising solid-state electrolyte (SE) due to its thermodynamic stability to Li. However, poor Li-ion conductivities at room temperature, low oxidative stabilities, and severe dendrite growth hamper its application. In this work, a partial dehydrogenation strategy is adopted to in situ generate an electronic blocking layer dispersed of LiH, addressing the above three issues simultaneously. The electrically insulated LiH reduces the electronic conductivity by two orders of magnitude, leading to a 32.0-times higher critical electrical bias for dendrite growth on the particle surfaces than that of the counterpart. Additionally, this layer not only promotes the Li-ion conductance by stimulating coordinated rotations of BH 4 − and B 12 H 12 2− , contributing to a Li-ion conductivity of 1.38 × 10 −3 S cm −1 at 25 °C, but also greatly enhances oxidation stability by localizing the electron density on BH 4 − , extending its voltage window to 6.0 V. Consequently, this electrolyte exhibits an unprecedented critical current density (CCD) of 15.12 mA cm −2 at 25 °C, long-term Li plating and stripping stability for 2700 h, and a wide temperature window for dendrite inhibition from −30 to 150 °C. Its Li-LiCoO 2 cell displays high reversibility within 3.0–5.0 V. It is believed that this work provides a clear direction for solid-state hydride electrolytes.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2022
·Vol. 45
·期 6
·1075-1088
·
IF 3.434
Wei Kaixin,Wu Xiaomei,Ma Baodi,Li Zhi,Xu Yi
A series of nickel-incorporated SBA-15 mesoporous molecular sieves (Ni-SBA-15) were prepared as support for the immobilization of his-tagged recombinant Microbacterium esterase. The Ni-SBA-15 could strongly and specific absorb the his-tagged esterase from cell disrupted supernatant. It was found that the nickel amount in Ni-SBA-15 has dramatic influence on the activity and thermo-stability of immobilized enzyme, while the kinds of nickel precursor had little effect on enzyme stability. The morphology, chemical composition and structure of the best support NiCl 2 -SBA-15 (Ni-SBA-15 prepared from NiCl 2 precursor) were characterized by various spectroscopy techniques. The immobilized esterase retained full activity of free esterase and showed high immobilized yield (> 90%) with higher thermo-stability, pH stability and organic solvent resistance compared with free enzyme. The optimum reaction temperature increased from 35 to 40 °C and the optimal reaction pH moved from 10.0 to 8.0 after enzyme immobilization. The immobilized esterase exhibited excellent storage stability and keeping 92% of the initial activity after 30 days’ storage at 25 °C. In addition, the immobilized esterase had excellent reusability for the synthesis of key chiral intermediate of d -biotin and the substrate conversion could still keep 100% after 13 cycles continuously. Finally, optical pure (4 S , 5 R )-hemiester was obtained in 80.8% isolated yield and 99% purity in the gram preparative scale.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhijun Li,Qinghui Ren,Xuexia Wang,Wenxing Chen,Leipeng Leng,Mingyang Zhang,J. Hugh Horton,Bo Liu,Qian Xu,Wei Wu,Jun Wang
Single-atom catalysts (SACs) have great potential to revolutionize heterogeneous catalysis, enabling fast and direct construction of desired products. Given their notable promise, a general and scalable strategy to access these catalyst systems is highly desirable. Herein, we describe a straightforward and efficient thermal atomization strategy to create atomically dispersed palladium atoms anchored on a nitrogen-doped carbon shell over an SBA-15 support. Their presence was confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurement. The nitrogen-containing carbon shells provide atomic diffusion sites for anchoring palladium atoms emitted from palladium nanoparticles. This catalyst showed exceptional efficiency in selective hydrogenation of phenylacetylene and other types of alkynes. Importantly, it showed excellent stability, recyclability, and sintering-resistant ability. This approach can be scaled up with comparable catalytic activity. We anticipate that this work may lay the foundation for rapid access to high-quality SACs that are amenable to large-scale production for industrial applications.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chengming Wu,Quan Wang,Jifan Li,Chun-Ling Liu,Wen-Sheng Dong
Catalytic conversion of biomass-derived platform chemicals into bulk chemicals p -xylene (PX) is appealing yet challenging due to low catalytic efficiency and severe reaction conditions. In this work, we fabricated a series of phosphate-modified ZrO 2 /SBA-15 ( x P-Zr/SBA-15) via adjusting the addition of phosphoric acid, and used them for the catalytic conversion biomass-derived 2,5-dimethylfuran (DMF) and ethylene to PX. Because of the enhanced adsorption capability for the reactant molecules (DMF and ethylene) and the good synergistic effect between Brønsted acid sites (P-OH) and Lewis acid sites (Zr 4+ ), 30P-Zr/SBA-15 revealed an excellent catalytic performance in the selective conversion of DMF into PX. The DMF conversion was 98.5%, PX yield was 92.0% at 250 °C for 12 h, and the corresponding PX productivity was upto 50.5 mmol PX ·g cat −1 ·h −1 . The results are far superior to those obtained on most previously reported catalysts in the literature under similar reaction conditions. The kinetic study revealed that 30P-Zr/SBA-15 has a lower apparent activation energy for the tandem reaction including the Diels-Alder reaction (57.0 kJ·mo −1 ) and dehydration reaction (37.7 kJ·mo −1 ). Moreover, the 30P-Zr/SBA-15 catalyst exhibited the excellent recyclability and could be recycled at least six times without a significant loss of activity. On the basis of the temperature-programmed surface reaction of DMF and ethylene, a reasonable reaction mechanism was proposed.
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高影响因子
Frontiers in Chemistry
·
2023
·
IF 5.5
Jun Xing,Qianqian Han,Jiyang Liu,Zhengzheng Yan
Timely, convenient, and efficient detection of carbohydrate antigen 15-3 (CA15-3) levels in serum holds significant importance in early screening, diagnostic assistance and prognosis prediction of breast cancer. The development of efficient and convenient electrochemical aptasensors with immobilized redox probes for label-free detection of CA15-3 is highly desirable. In this work, a bipolar silica nanochannel array film (bp-SNA) with two distinct functional domains including nanochannels and an outer surface was employed for the immobilization of recognition ligands and electrochemical redox probes, enabling the construction of a probe-integrated aptasensor for reagentless electrochemical detection of CA15-3. Cost-effective and readily available indium tin oxide (ITO) was used as the supporting electrode for sequential growth of a negatively charged inner layer (n-SNA) followed by a positively charged outer layer (p-SNA). The preparation process of bp-SNA is convenient. Functionalization of amino groups on the outer surface of bp-SNA was modified by aldehyde groups for covalent immobilization of recognition aptamers, further establishing the recognition interface. Within the nanochannels of bp-SNA, the electrochemical redox probe, tri (2,2′-dipyridyl) cobalt (II) (Co(bpy) 3 2+ ) was immobilized, which experienced a dual effect of electrostatic attraction from n-SNA and electrostatic repulsion from p-SNA, resulting in high stability of the immobilized probes. The constructed aptasensor allowed for reagentless electrochemical detection of CA15-3 ranged from 0.001 U/mL to 500 U/mL with a low detection limit (DL), 0.13 mU/mL). The application of the constructed aptasensor for CA15-3 detection in fetal bovine serum was also validated. This sensor offers advantages of a simple and readily obtainable supporting electrode, easy bp-SNA fabrication, high probe stability and good stability.
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PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2014
·
IF 3.209
Bing Yan,Qiu-Ping Li
Several kinds of novel lanthanide organic–inorganic mesoporous hybrid luminescent materials have been assembled by introducing the ternary lanthanide ions (Eu 3+ , Tb 3+ ) and beta-diketone (TTA, TAA) into the functionalized mesoporous hosts through the coordination bond and covalent bond by using 3-chloropropyltriethoxysilane modified 1,4,7,10-tetraazacyclododecane (Cyclen-Si) as an organic bridge molecule. These multicomponent hybrids are characterized by FTIR, TEM, XRD, thermogravimetric analysis, diffuse reflectance UV–Vis spectra and nitrogen adsorption–desorption isotherms, especially the photoluminescence properties of them. The luminescent spectra of the hybrids reveal that the MCM-41 based materials show strong emission intensities, high luminescent quantum efficiencies, long luminescent lifetimes and exhibit characteristic red and green luminescence originated from lanthanide ions (Eu 3+ or Tb 3+ ), which suggesting the Cyclen-Si bridge molecule is favorable for the assembly of lanthanide functionalized luminescent hybrids.
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高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 11
·6601-6615
·
IF 9.3
Chao Yuan,Yuan Zhang,Zhiyuan Zong,Shenghui Zhou,Hongyou Cui,Hongzi Tan
Catalytic wet air oxidation (CWAO) is a very promising technology for the elimination of various refractory pollutants, but to activate dioxygen under mild conditions is a great challenge. In this research, we report a series of Cux/CNy@SBA catalysts to activate dioxygen for CWAO of phenols and antibiotics under mild conditions. The catalysts were prepared by in situ growth and dispersion of g-C3N4 and Cu species over the SBA-15 surface. Characterization by HRTEM, EDS, XRD, FT-IR, and XPS showed that the formed ultrathin g-C3N4 coating over the surface of SBA-15 provided abundant locations to embed the Cu species and thus more active sites were generated. UV-vis DRS characterization proved that the synergetic effect between Cu species and the SBA-15-dispersed g-C3N4 greatly enhanced the ability to activate dioxygen. It was found interestingly that superoxide radicals (˙O2−) were the dominating active species at low temperature, while both ˙O2− and hydroxyl radicals (˙OH) became the active species at high temperature during the CWAO of phenol. Among the catalysts tested, Cu1/CN3.3@SBA-N demonstrated the highest activity, affording 100% phenol removal and more than 90% chemical oxygen demand (COD) removal, even at 90 °C and atmospheric dioxygen pressure. Modification of the SBA-15 surface with KH-550 could remarkably improve the recycling stability of the catalyst. These findings provide new insights for the development of highly effective catalysts for the activation of dioxygen, particularly in the field of CWAO wastewater treatment.
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BioEnergy Research
·
2015
·Vol. 8
·期 3
·1263-1274
·
IF 3.541
Zhang Zhi-bo,Lu Qiang,Ye Xiao-ning,Wang Ti-peng,Wang Xian-hua,Dong Chang-qing
Solid phosphoric acid (SPA) catalysts with different carriers were prepared and used for catalytic fast pyrolysis of poplar wood to produce levoglucosenone (LGO), a valuable anhydrosugar derivative that can be used in various organic synthesis applications. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to evaluate the catalytic capabilities of these catalysts under different reaction conditions. The results indicated that SPA catalyst prepared with the SBA-15 carrier exhibited the best catalytic capability for selectively producing LGO. Both the catalytic pyrolysis temperature and catalyst-to-biomass ratio affected the pyrolytic products greatly. The maximal LGO yield reached as high as 8.2 wt% from poplar wood, obtained at the pyrolysis temperature of 300 °C and the catalyst-to-biomass ratio of 1. The by-products during the catalytic pyrolysis process were mainly acetic acid (AA) and furfural (FF). In addition, the SPA catalyst possessed better catalytic capability than the liquid phosphoric acid (H 3 PO 4 ) catalyst to produce LGO.
研究领域:
生物能源
·
催化化学
·
生物质转化
·
热解化学
·
绿色化学
·
可再生资源利用
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 14
·6192-6205
·
IF 3.591
Haiqing Xu,Yuhang Gao,Qiantu Tao,Aiping Li,Zhanchao Liu,Yinhua Jiang,Hongwei Liu,Rongguang Yang,Yan Liu
A novel salicylic acid (SA) molecularly imprinted polymer (MIP) has been synthesized successfully by a surface imprinting technique based on the SBA-15 nanoreactor. SBA-15, selected as the nanoreactor for immobilizing the monomers and template molecules, would be an option to develop a new SA imprinting strategy. The obtained imprinted materials were characterized by Fourier transmission infrared spectrometry (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and nitrogen adsorption–desorption isotherms. The results suggested that MIP possessed an excellent ordered hexagonal mesoporous structure, which preserved the highly ordered mesoporous structure of SBA-15. Experimental variables influencing the adsorption process, including the initial pH, initial concentration and temperature, were optimized by the three-level Box–Behnken experimental design with the three factors combining the response surface method (RSM) for the first time. The optimal adsorption conditions were obtained to achieve the maximum adsorption capacity of SA as follows: initial solution pH 4.62, initial SA concentration 52.38 mg L−1, and temperature 35.0 °C. Under these conditions, the experimental value of the adsorption capacity was 44.435 mg g−1, which was very close to the predicted value (43.429 mg g−1). Furthermore, the adsorption isotherm and selectivity towards SA onto MIP and non-imprinted polymer (NIP) were investigated, indicating that MIP had splendid recognizing ability and a superior specific adsorption capacity (145.19 mg g−1) compared to that of NIP (64.30 mg g−1) at 35 °C. Meanwhile, MIP was regenerated and found to be suitable for reuse in successive adsorption–desorption cycles five times without significant loss in the adsorption capacity. The results suggested that MIP could be used as an excellent adsorbent for the efficient removal of SA from aqueous solution.
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高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Yi Yu,Fanfan Li,Zhouxuan Zang,Li Xu,Guoji Liu
Catalytic oxidation of 2-methylnaphthalene to 2-methyl-1,4-naphthoquinone (vitamin K 3 ) is a significant pathway to produce vitamin groups K. High pollution and low-productivity of the traditional method require a greener catalyst and process. In this work, Al/Ti-SBA-15 with different n Si /n Al and n Si /n Ti ratios were hydrothermally prepared in mild acidic condition and tested in partial oxidation of 2-methylnaphthalene. Commercial zeolites NaY, β and ZSM-5 were applied to investigate the influence of mass transfer resistance and acidity on catalytic performance. Catalysts were characterized by XRD, N 2 adsorption-desorption, TEM, NH 3 -TPD, FTIR and Py -FTIR. We have found that the 2-methylnaphthalene conversion and vitamin K 3 selectivity depend strongly on the mesoporous structure as well as Brönsted acid concentration and strength. Irregular micropores and strong acidity will accelerate the cleavage of C = C in aromatic rings, leading to the production of phthalic anhydride. DFT calculation reveals that incorporation of aluminum in SBA-15 can reduce the energy gap, facilitating the electron transfer. And as a consequence of the substitution of Al in tetrahedral positions in SBA-15, Al-SBA-15 (10) gives the best result with 72% yield to vitamin K 3 . This catalyst markedly reduces the activation energy due to the modified activated center. Repeated experiments recommend that Al-SBA-15 is a steady and high-efficiency catalyst for the production of vitamin K 3 .
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