APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
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IF 14.229
Kun Chen,Huihuang Fang,Simson Wu,Xi Liu,Jianwei Zheng,Song Zhou,Xinping Duan,Yichao Zhuang,Shik Chi Edman Tsang,Youzhu Yuan
The direct hydrogenation of CO 2 to methanol has become a very active research field because CO 2 can be prospectively recycled to mitigate greenhouse effect and store clean synthetic fuels. This reaction can be catalyzed by supported Cu catalysts and the catalysts display strong support or promoter effects. Sintering of Cu species accelerates the separation of Cu–oxide interfaces, reduces the active component, and diminishes the methanol selectivity. In this work, we report a Cu catalyst supported on La-modified SBA-15, where the Cu–LaO x interface is generated through the interaction of highly dispersed Cu nanoparticles with LaO x species bedded into the SBA-15 pore wall. The optimized Cu 1 La 0.2 /SBA-15 catalyst can achieve methanol selectivity up to 81.2% with no deterioration in activity over 100 h on stream compared with the La-free catalyst. A thorough study reveals that La species not only significantly improve the CO 2 adsorption but also enhance Cu dispersion to produce well-dispersed active sites. The H/D exchange experiments show that the methanol synthesis displays a strong thermodynamic isotope effect and the Cu–LaO x interface plays a crucial role for the methanol synthesis rate in CO 2 /D 2 feed. In situ DRIFTS studies reveal that *HCOO and *OCH 3 species are the key intermediates formed during the activation of CO 2 and methanol synthesis over the Cu 1 La 0.2 /SBA-15 catalyst.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2018
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IF 3.909
Yue Li,Nanjing Zhong,Ling-Zhi Cheong,Jianrong Huang,Hongxiao Chen,Shaoyan Lin
In this study, SBA-15 was modified by a series of silane coupling reagents and later used to immobilize Candida antartica lipase B (CALB). The enzymatic properties of the immobilized CALB samples were studied. In addition, the catalytic performance in glycerolysis of soybean oil for diacylglycerols (DAG) production was also investigated. The highest enzymatic activity up to 6100.00 ± 246.41 U/g was observed from the propyl methacrylate group modified SBA-15 supported CALB. No loss of activity was observed from the propyl methacrylate group modified SBA-15 supported CALB, but a higher-than-initial activity was notably found from 3-aminopropyl group and n -octyl group modified SBA-15 supported CALB after a 4-h incubation in air at 70 °C. 1-isocyanatopropane group modified SBA-15 supported CALB exhibited selectivity for DAG production. DAG content up to 61.90 ± 2.38 wt% and a DAG/MAG ratio at 3.11 ± 0.08 was obtained after a 24-h reaction at 60 °C in a solvent-free system.
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PubMed
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2016
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IF 3.958
Mengshuai Liu,Bo Liu,Lin Liang,Fangxiao Wang,Lei Shi,Jianmin Sun
The novel bifunctional Zn/SBA-15 supported ammonium salt (NH 3 I-Zn/SBA-15) as single-component heterogeneous catalyst for the coupling of CO 2 with epoxides was developed. FT-IR, XRD, N 2 adsorption/desorption, TEM, XPS techniques were used to determine the morphological structure and physicochemical properties of NH 3 I-Zn/SBA-15 sample. The catalyst exhibited exceptionally effective activity with 93% yield and 99% selectivity and a high TOF of 306 h −1 to propylene carbonate at 130 °C and 3 MPa of CO 2 for 12 h in the absence of cocatalyst and solvent participation. Also the catalytic system was versatile to the cycloadditions of other epoxides with CO 2 under the optimized reaction conditions. Additionally, the catalyst was easily recycled and reused only with slight loss of activity after five recycles. Besides, a possible catalytic mechanism involving cooperative activation of epoxide and ring-opening by one-component and bifunctional catalyst was proposed. The protocol herein provides important insights on design of novel single-component heterogeneous catalysts for CO 2 relevant transformations.
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Catalysis Science & Technology
·
2017
·Vol. 7
·期 3
·725-733
·
IF 5.773
Ning Liu,Zhimin Wu,Meng Li,Shanshan Li,Yongfei Li,Rongdong Yu,Langsheng Pan,Yuejin Liu
Bimetallic Al–La oxides were conjointly precoated on SBA-15 prior to the introduction of potassium fluoride to achieve solid superbases at low temperature by a modified wetness impregnation method. This breaks the tradition of decomposition of KNO3 at high temperature and gives rise to a new approach to generating superbasic sites on SBA-15. The physico-chemical characteristics of the prepared KF/Al–La@SBA-15 materials were investigated using FT-IR, XRD, TG-DTG, N2 adsorption–desorption, TEM, SEM-EDS, acid–base titration, Hammett indicators and CO2-TPD measurements. The results demonstrated that the addition of Al species promoted the dispersion behavior of La species inside the channels, and the bimetallic species could synergistically protect the mesoporous structures of SBA-15 against KF corrosion. With increasing Al content, KF/Al–La@SBA-15 exhibited a long-range ordering of the pores with relatively narrow pore size distribution as well as high specific surface area. The research results showed that the KF/Al–La@SBA-15 (0.4) catalyst possessed a total basicity up to 0.79 mmol g−1 and superbasicity with a strength of 26.5. The catalytic activity of the prepared materials was evaluated in the ring-opening reaction of propylene oxide with methanol. Compared with the SBA-15 supported monometallic oxide (Al or La) catalysts, KF/Al–La@SBA-15 (0.4) exhibited the highest catalytic activity for the ring-opening reaction of propylene oxide with methanol. This is associated with the synergistic effects between Al and La species and the high dispersion of active components on the SBA-15 support.
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CHEMICAL ENGINEERING JOURNAL
·
2017
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IF 6.216
Hao Chen,Houhang Ruan,Xilei Lu,Jie Fu,Timothy Langrish,Xiuyang Lu
In the present study, an economic and environmentally friendly bi-functional catalyst, Zr-SBA-15, has been prepared to develop a single-step process for synthesis of methyl levulinate (MLA) directly from furfural (FAL) in near-critical methanol without added H 2 . The presence of Zr in SBA-15, the structure of the Zr-SBA-15 catalyst, and its physical properties have been determined by X-ray diffraction (XRD), N 2 adsorption and desorption (N 2 -BET) and transmission electron microscopy (TEM). The Zr-SBA-15 catalyst has high activity for the production of MLA and good reusability. A possible reaction pathway containing two possible reaction pathways during this single-step synthesis of MLA has been proposed: the FAL has been transformed to β-Methoxy-2-furanethanol (MFE) and 2-Furfuryl methyl ether first, which then have been converted to MLA, and the conversion of FAL to MFE has been much easier and faster than that to 2-FME, which may be the major reaction pathway. The SBA-15 has given high activity for the conversion of FAL to MFE, and the incorporation of Zr has converted the MFE to MLA efficiently. The reaction of FAL to MFE to MLA has been found to be the dominant reaction. Finally, the catalyst has shown good reusability for at least five times without any reduction in the catalytic activity.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yingjie Niu,Shiying Zou,Haonan Liu,Minyue Hu,Jinjun Cai,Chao'en Li,Kathryn A. Mumford,Masood S. Alivand,Francesco Barzagli,Rui Zhang
Improving the energy efficiency of CO 2 desorption remains a key challenge in post-combustion carbon capture using amine solvents. In this work, a series of solid acid catalysts based on sulfonated mesoporous SBA-15 and functionalized with phosphotungstic acid (HPW) were synthesized via post-synthetic modification and applied to the catalytic regeneration of monoethanolamine (MEA). The catalysts, featuring both Brønsted and Lewis acid sites, were thoroughly characterized and tested in desorption experiments using CO 2 -loaded MEA solutions. Among the synthesized materials, HPW-SBA-15-SO 3 H-1 exhibited the best performance, achieving significantly higher CO 2 desorption rate and cyclic capacity compared to the uncatalyzed system, while reducing the relative heat duty by up to 37.7 %. This catalyst also demonstrated good stability over 20 absorption–desorption cycles, maintaining its structural integrity. In addition, machine learning was employed to correlate the catalysts' physicochemical features with their desorption performance, highlighting the role of acidity and porosity and supporting the proposed mechanism by which acidic sites promote carbamate decomposition and MEAH + deprotonation. These findings underscore the potential of functionalized mesoporous silica as efficient solid catalysts for lowering the regeneration energy penalty in MEA-based carbon capture systems.
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Jiaxin Wang,Ying Liu,Baozhong Zhu,Jiuyu Chen,Qing Wang,Yunlan Sun
Amine-modified mesoporous silicon was widely used for CO 2 capture. However, its adsorption capability was significantly affected by temperature and humidity. In this paper, tetraethylenepentamine (TEPA) modified SBA-15 adsorbents were prepared for capturing CO 2 . The effects of the modification method, the concentration of TEPA, the adsorption temperature, and the humidity of atmosphere on CO 2 adsorption capability were studied. Moreover, combined with molecular dynamics (MD) and density functional theory (DFT) computations, the diffusion characteristics and adsorption mechanism were explored. The CO 2 adsorption capability of the adsorbent prepared by the ultrasonic impregnation method was higher than those prepared by the stirring impregnation method, owing to that ultrasonic impregnation could promote the uniformity of TEPA. With the increase of TEPA concentration of SBA-15, the CO 2 adsorption capability increased. SBA-15-2 had the highest CO 2 adsorption capability of 1.17 mmol/g at 30 °C. This was due to the N-containing functional groups, showing good affinity for CO 2 , introduced by TEPA impregnation. When the temperature increased from 30 °C to 70 °C, the CO 2 adsorption capability of all modified SBA-15 adsorbents decreased, since the CO 2 adsorption was an exothermic reaction. SBA-15-2 showed better water vapor resistance than SBA-15-2 (Stir). This was related to the higher dispersity of organic carbon chain introduced by TEPA modification after ultrasonic impregnation. The organic carbon chain of SBA-15-2 increased the water vapor resistance by reducing the hydroxyl group. Finally, from a microscopic aspect, the MD simulation suggested that impregnated TEPA inside SBA-15 may improve CO 2 capture by increasing the thickness of effective adsorption layer. Besides, the DFT simulation showed that TEPA modification increased the adsorption energy of SBA-15 on CO 2 . This serves as a reference for later mesoporous silicon adsorbent research and development on CO 2 capture.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Liqiang Zhang,Ningmin Zhu,Chaochao Wang,Rongzheng Cui,Riyi Lin
Two-step catalytic pyrolysis of Nannochloropsis sp (NS) was conducted with SBA-15 and ZSM-5. Thermogravimetric analyzer (TG) and pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) were used to investigate the effects of SBA-15 and ZSM-5 on the two-step pyrolysis of NS. The comparative study showed that ZSM-5 and SBA-15 had different effects on the pyrolysis characteristic of NS because of their different property. ZSM-5 had no effects on the kinetic mechanism, but SBA-15 obviously changed DTG curves and the reaction order of the low temperature pyrolysis stage. SBA-15 increased the contents of amines and alkanes to 19.40% and 5.62% in the first step compared with those of the one-step pyrolysis (1.95% and 1.83%). Due to the stronger acid sites, ZSM-5 improved the content of olefins (33.79%) and esters (10.79%) in the first step and the contents of nitriles (11.75%) and aromatic hydrocarbons (31.01%) in the second step compared with those of one-step pyrolysis (10.61%, 5.41%, 0.00%, 8.42%). Acid catalyst had no positive effects on the generation of N-heterocyclic compounds. This study is expected to provide a reference for the efficient pyrolysis utilization of microalgae.
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高影响因子
FOOD CHEMISTRY
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2018
·
IF 4.946
Nanjing Zhong,Weilin Chen,Liyan Liu,Hongxiao Chen
In this study, mesoporous silica SBA-15 was modified by organic functional groups through silanization. Series of organosilane compounds were grafted onto the SBA-15, and the obtained functionalized carriers were then used to immobilize the lipase from Rhizomucor miehei (RML). The enzymatic properties of the obtained immobilized RML samples were evaluated, and the catalytic efficiencies in glycerolysis of triacylglycerols (TAG) reaction were studied. Compared with the parent SBA-15 immobilized RML, the organic modification gave a maximum improvement of enzymatic activity from 200.00 to 13211.11 U/g; in addition, TAG conversion and diacylglycerols (DAG) content increased from 21.28 to 84.24% and 15.45 to 59.03% respectively. The organic modification also decreased the sensitivity of immobilized RML in extreme pH values and increased their thermostability.
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PubMed
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Ziheng Wei,Yongping Liu,Qi Ding,Yuena Zhang,Yu Ren,Jihu Chen,Mingming Si,Yuchi Fan,Wan Jiang
Conductive two-dimensional (2D) materials exhibit excellent electromagnetic wave (EMW) absorption properties at high frequencies due to their high conductivity loss. However, their unsatisfactory EMW absorption at low frequencies, attributed to impedance mismatch, remains a significant challenge. In this work, high-conductivity 1T′ WTe 2 nanosheets were incorporated into insulating mesoporous channels of Santa Barbara Amorphous-15 (SBA-15) via chemical vapor deposition (CVD), resulting in the formation of 1T′ WTe 2 /SBA-15 composites. These mesoporous channels restrict the growth of 1T′ WTe 2 and hinder carrier migration cross the channels, reducing their conductivity. Meanwhile, heterogeneous interfaces were formed between 1T′ WTe 2 nanosheets and mesoporous channels of SBA-15, accompanied by defects within the 1T′ WTe 2 nanosheets. This interaction promotes dipole polarization losses, significantly enhancing the attenuation of incident EMW, particularly at low frequencies. Consequently, the effective absorption bandwidth (EAB) of 1T’ WTe 2 /SBA-15 composites within the S band reached to 0.72 GHz, ranging from 3.28 GHz to 4.0 GHz, with a minimum reflection loss (RL min ) of −26.5 dB at 3.68 GHz. Furthermore, the EAB of the composites extended to 3.92 GHz at 1.5 mm in the high-frequency range. This work introduces a novel strategy for enhancing EMW absorption performance in the S band through heterogeneous interfaces and defect engineering, driven by the limiting effects of mesoporous channels.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Guanwei Zhao,Wei Ma,Hongyu Pang,Ligang Zhang,Yuzheng Wang,Xiaoxue Ren,Kuo Liu,Hongling Yang,Yongchun Liu
Low-temperature catalytic oxidation is a prevalent technology for toluene removal due to its reduced energy demand. In this study, N,N-dimethylformamide (DMF) was used to control the particle size of active metals. The activity tests revealed that Pt nanoparticles with a particle size of 5–15 nm exhibited higher activity for toluene oxidation and maintained good hydrothermal stability on the SBA-15 support. The results suggest that despite the increase of Pt particle size by using DMF, the proportion of Pt 0 and the oxygen activation ability were both increased. The reaction pathway of the toluene oxidation over Pt/SBA-15 was examined in depth by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), proton transfer reaction time-of-flight mass spectrometry (PTR-TOF-MS) and cluster analysis, revealing that the benzyl alcohol, benzaldehyde, and benzoic acid species were primary intermediate products. The benzaldehyde on the larger Pt nanoparticles is conducive to decomposing and generating CO 2 for complete mineralization, promoting the activity of toluene oxidation. This work highlights the significance of DMF-induced size effects in the development of low-temperature oxidation catalysts and understanding of reaction mechanism, guiding the design of new efficient toluene oxidation catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Qian-Wen Lu,Qing He,Qing-Shuai Zhang,Da Sheng,Song-Hai Wu,Yong Liu,Xu Han
Although thermocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-formylfuran (DFF) by O2 is an important reaction, achieving a high yield of DFF is still challenging. In this study, a series of MoxCuy/NH2-SBA-15 are prepared, and Mo3Cu1/NH2-SBA-15 exhibits the desirable catalytic reactivity with a complete conversion of HMF and high selectivity of 94.4% toward DFF. XPS and EPR analyses indicate that the abundant oxygen vacancies (Ov) and Cu(I) are the reactive sites for O2 activation. Quenching experiments and various characterizations reveal that superoxo (≡Cu(II)/Ov-OO•) on the surface of catalyst, instead of •OH and O2•–, are the primary oxidizing species to abstract H from HMF to RCH2-O•, accompanied by the formation of ≡Cu(II)/Ov-OOH peroxo. Meanwhile, the doped Mo(V/VI) further activates ≡Cu(II)/Ov-OOH peroxo to form ≡Mo-(η2-O2) peroxo, which significantly promotes the oxidation selectivity of RCH2-O• toward DFF via the H-abstraction pathway. This study provides new insight on selective thermal-oxidation of biomass-derived compounds to high-value-added chemicals via regulating reactive oxidizing species on the surface of catalysts.
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