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.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Shanghua Feng,Binbin Zhao,Yu Liang,Lei Liu,Jinxiang Dong
Tungsten and aluminum were directly incorporated into SBA-15 via one-step synthesis method under an acidic medium. The W- and Al-incorporated SBA-15 was applied as support for Pt nanoparticles to catalyze glycerol hydrogenolysis toward 1,3-propanediol. A combination of the characterization techniques showed that the tungsten and aluminum were incorporated into SBA-15 homogeneously, and the platinum nanoparticles could be uniformly dispersed on the modified-SBA-15. The catalytic performance of Pt-loaded SBA-15 could be significantly improved after the incorporation of tungsten and aluminum into SBA-15, reaching a 1,3-PDO selectivity near 50% when the glycerol conversion was 66%. The glycerol hydrogenolysis reaction proceeds through a dehydration–hydrogenation process, and the enhanced 1,3-PDO selectivity greatly benefited from the synergism between Brønsted acid and Lewis acid sites, which is tightly related with the incorporation of tungsten and aluminum species on the modified SBA-15.
研究领域:
催化化学
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材料科学
·
绿色化学
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能源化工
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纳米催化
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多相催化
✓ 已验证
DOI
高影响因子
CELLULOSE
·
2025
·
IF 4.8
Liu Wanni,Shi Xian,Liu Dongqi,Xing Xinyi,Ruan Mengya,Sun Song,Lyu Gaojin,Xu Siquan
Converting glucose-based carbohydrates such as microcrystalline cellulose and cellulose components in lignocellulose into 5-hydroxymethylfurfural (HMF) is a feasible way to achieve high-value utilization of biomass. To this end, this work assembled a series of bifunctional (x)Hf/SBA-15-S catalysts by introducing active hafnium species and grafting sulfonic acid groups onto the mesoporous SBA-15 silica carrier to drive the conversion of glucose, cellulose and untreated wheat straw into HMF. Through detailed parameter evaluation, competitive HMF yields were achieved from glucose (74%) and cellulose (51%), respectively. More importantly, the cellulose and hemicellulose components in untreated wheat straw could be efficiently converted simultaneously to obtain HMF and furfural with yields of 50 and 30%, respectively. Systematic characterization revealed that (x)Hf/SBA-15-S catalysts had an ordered pore channel, bifunctional acidity and good hydrothermal stability, which were beneficial to the process of cellulose undergoing depolymerization, isomerization and dehydration to produce HMF. Therefore, it is believed that the catalytic transformation strategy presented in this study has application prospects for realizing the utilization of glucose-based carbohydrates.
研究领域:
催化化学
·
生物质转化
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绿色化学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 16
·6406-6416
·
IF 5.287
Mengshuai Liu,Kunqi Gao,Lin Liang,Jianmin Sun,Li Sheng,Masahiko Arai
The combination of a metal-modified SBA-15 catalyst with potassium iodide was developed as heterogeneous dual catalysts for chemical fixation of CO2 to cyclic carbonates. It was observed that the binary Zn-SBA-15/KI catalysts were the most efficient among various metal-modified SBA-15/KI catalysts and showed an excellent synergetic effect in promoting the reaction under mild conditions. Moreover, the effects of reaction parameters on cycloaddition of CO2 with propylene oxide (PO) to propylene carbonate (PC) were optimized. Under the optimal conditions determined, the Zn-SBA-15/KI catalytic system was also versatile in CO2 cycloaddition with other epoxides. Additionally, the mechanistic details for the fixation of CO2 into a cyclic carbonate catalyzed by SBA-15/KI and Zn-SBA-15/KI were also contrastively elucidated using the density functional theory (DFT) method. The DFT results suggested that the zinc-modified and unmodified catalysts showed different coupling modes of CO2, and the ring-opening reaction was the rate-determining step in the SBA-15/KI catalyzed cycloaddition reaction, but the zinc-modified SBA-15/KI catalysts could enhance the CO2 cycloaddition, as the formation of a stable complex was beneficial to CO2 trapping. As a result, the ring-closing reaction became the rate-determining step in the Zn-SBA-15/KI catalyzed cycloaddition reaction, which was a promising result to guide the catalyst design for CO2 conversion.
研究领域:
催化化学
·
环境科学
·
理论化学
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产品关联
DOI
高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 20
·5098-5107
·
IF 4.495
Ning Xiang,Yaqin Hou,Xiaojin Han,Yulin Li,Yaoping Guo,Yongjin Liu,Zhanggen Huang
Room temperature HCHO catalytic oxidation over inert support loaded Pd catalysts remains a significant challenge. Herein, a series of alkali Na (1–4 wt.%) modified 1Pd/SBA-15 catalysts were prepared by a co-impregnation method and used for HCHO catalytic oxidation at room temperature. Results showed that alkali Na significantly improved the HCHO oxidation performance of 1Pd/SBA-15 and the optimal Na loading was 2 wt.%. BET, XRD, STEM, XPS, H 2 -TPR, O 2 -TPD and in situ DRIFTS were performed to reveal the promotion role of alkali Na. As a consequence, alkali Na addition could stabilize well dispersed Pd particles which then facilitated the O 2 activation and accelerated the decomposition of formate intermediates species, thus a superior HCHO catalytic oxidation performance was obtained. This study first clearly illustrated the promotion mechanism of alkali Na without the implication of active support and provides an efficient and facile way to achieve high dispersion of Pd particles on inert support and tremendously expands the selected range of supports for room temperature HCHO catalytic oxidation. Graphical Alkali promoted : A series of Na alkali-promoted 1Pd/SBA15 catalysts were prepared by a co-impregnation method and tested for HCHO catalytic oxidation at room temperature. Addition of alkali Na stabilized well-dispersed Pd particles which facilitated O 2 activation and accelerated formate species decomposition rate, leading to superior HCHO catalytic oxidation performance of 2Na-1Pd/SBA-15.
研究领域:
催化化学
·
环境科学
·
材料化学
·
表面科学
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大气污染控制
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Yansi Cao,Yu Fan,Zhiheng Ma,Zhixuan Cheng,Qun Xiang,Zhiming Duan,Jiaqiang Xu
There is an urgent need for effective and portable gas sensors toward organophosphorus (OP) vapors in the areas of anti-terrorism and pesticides residue monitoring. Herein, we report a series of urea-functionalized SBA-15 (UXs/SBA-15: U1/SBA-15, U2/SBA-15 and U3/SBA-15) prepared by post-grafting methods and their applications in trace-level dimethyl methylphosphonate (DMMP, lab simulate of toxic OP agents) sensing by means of quartz crystal microbalance (QCM) transducers. U3/SBA-15 based QCM sensors exhibited excellent responses and remarkable selectivity toward DMMP vapors. A frequency shift (Δ F ) of −50 Hz was achieved when the DMMP vapors reached 30 ppb. And the limit of detection (LOD) of QCM sensor modified with U3/SBA-15 was found at 12.25 ppb. Moreover, the simulated adsorption enthalpies (Δ H ) of UXs and DMMP molecules were calculated with Gaussian 09 to investigate the sensing mechanism. The results indicated the existence of chemisorption between UXs and DMMP molecules caused by hydrogen-bonding interactions, among which a minimum Δ H (−71.96 kJ mol −1 ) between U3 and DMMP molecule was found, resulting a maximum response to DMMP compared with U1-DMMP (−52.53 kJ mol −1 ) and U2-DMMP (−57.01 kJ mol −1 ). Therefore, the well-defined UXs/SBA-15 lead to a great potential on the detection of OP vapors.
研究领域:
材料科学
·
化学传感
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分析化学
·
环境监测
✓ 已验证
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Zhenzhen Wang,Shufeng Lin,Liujun Wang,Zhe Wang,Bing Lu,Zhonghua Sun,Zhihui Zhang,Mingyang He,Junfeng Qian
The hydrogenation of CO 2 to formic acid (FA) represents a sustainable route for carbon utilization and chemical production, yet it faces challenges in catalytic efficiency, selectivity, and process scalability. Herein, we report a highly efficient catalytic system based on Pd supported on amine-functionalized Zr-SBA-15 (Pd/Zr-SBA-15-AP) for continuous FA synthesis in a fixed-bed reactor. The flake-shaped Zr-SBA-15 support with short mesoporous channels facilitates superior mass transfer. Meanwhile, amine functionalization was identified to serve a dual function: significantly enhancing CO 2 adsorption capacity and modulating the electronic state of Pd to form electron-enriched sites conducive to H 2 activation. The optimized catalyst, 0.3Pd/Zr-SBA-15-AP 3.0 , achieved an exceptional turnover number (TON) of 160 and a turnover frequency (TOF) of 80 h −1 , outperforming the state-of-the-art catalyst under similar continuous-flow conditions. Furthermore, the catalyst demonstrated stable performance over 32 h of continuous operation, underscoring its practical potential. This work provides a scalable strategy for sustainable FA production, effectively bridging laboratory-scale research and industrial application.
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
材料科学
·
环境科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Renna Li,Tianshan Xue,Zhe Li,Qiang Wang
Hydrophobic zeolites have been considered as one of the most promising adsorbents for capturing volatile organic compounds (VOCs). In this contribution, hierarchically structured ZSM-5/SBA-15 composites with different morphologies including platelet, hexagonal prism, long-hexagonal prism, and long-rod were prepared. All materials were characterized using XRD, SEM, and TEM-EDX, which confirmed that the high dispersion of two zeolites within the composites. Due to the presence of intracrystalline mesopores that could shorten the diffusion pathway of toluene, the composites resulted in increased effective diffusion and higher adsorption capacity. The composites also possess higher hydrophobicity, leading to much better toluene adsorption performance under humid conditions. The water contact angle of ZSM-5 could be increased from 15.6° to 44.9° by forming well dispersed zeolite composites. The 29 Si MAS NMR results confirmed that the composites possess higher amount of Q 4 groups (75.3%–80.1%), which is the intrinsic reason for higher hydrophobicity. Notably, ZSM-5/SBA-15-hexagonal prism resulted in the best adsorption performance and cycling stability when compared with pure ZSM-5, the breakthrough time was increased from 20.8 to 49.4 min under dry conditions and from 5.9 to 27.3 min in the presence of 50% relative humidity. This work represents an important scheme for making hydrophobic zeolite-based VOCs adsorbents with also improved toluene diffusion properties due to the unique hierarchical porous structure.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2020
·Vol. 147
·期 1
·04020142
·
IF 1.264
Yuefeng Qiu,Liming Kong,Tonghe Chen,Qin Xu
Cu+-modified SBA-15 (Cu+/SBA-15, SBA-15 refers well-ordered hexagonal mesoporous silica) was prepared for adsorption of tetracycline (TC) by the pH adjusting reduction method. Some Cu+ species (Cu2O) are aggregated on the outside surface of SBA-15, and the other Cu+ species are highly dispersed in SBA-15 via ≡Si-O-Cu. Its adsorption mechanism was firstly studied via comparison with CuO/SBA-15. The TC adsorption kinetic of Cu+/SBA-15 fitted the pseudo-second-order model well. The adsorption isotherms at 293, 303, and 313 K were determined and modeled with Langmuir and Freundlich equations, and the Qmax of Cu+/SBA-15 for TC calculated from Langmuir model could reach 961.54 mg/g at 313 K. Its good adsorption performance for TC is associated with the high surface area of SBA-15, highly dispersed Cu+ species, and mesoporous structure. The adsorption of Cu+/SBA-15 for TC is an endothermic process, and adsorption heat is 66.88 kJ·mol−1, which implies that the adsorption process of Cu+/SBA-15 for TC is weak chemisorption. The adsorption mechanism of Cu+/SBA-15 was mainly explored via comparing with CuO/SBA-15 by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) spectroscopy analysis. Besides the coordination complexation of Cu+ with NH2 radical of TC, the π-complexation between Cu+, and the benzene ring of TC improved the adsorption capacity of Cu+/SBA-15 for TC comparing with CuO/SBA-15 and showed a dominant role for TC adsorption.
研究领域:
环境科学
·
材料科学
·
化学工程
·
分析化学
✓ 已验证
DOI
高影响因子
Green Chemistry Letters and Reviews
·
2024
·
IF 5.8
Hong Zhang,Wenbin Liu,Lei Wang,Xin Zhang,Bo Wang,Xu Zeng,Bin Zhang
The immobilization of enzymes is an important strategy to improve their stability and reusability. However, it often comes with a trade off of reduced biological activity and catalytic efficiency. In this study, a composite hydrogel based on corn stalk carboxymethyl cellulose, acrylic acid, and mesoporous silica SBA-15 was developed as a support for the immobilization of lipase from Pseudomonas S.P. (PSL). The surface morphology and functional properties of the composite hydrogels were investigated by scanning electron microscopy, Fourier transform infrared, X-ray diffraction and simultaneous thermal analyzer, respectively. The composite hydrogel materials had a large number of mesopores and macropores were present in the wall of the hydrogel sheet. The hydrogel had a network structure that reduced the diffusion resistance of the substrate and improved the accessibility of the enzyme. The immobilized PSL exhibited high enantioselectivity (E value: 88.2) and enzyme activity (316.8 µmol/g/min) in the preparation of (S)-ibuprofen by enzymatic hydrolytic resolution of racemic ibuprofen ethyl ester. This prepared novel composite hydrogel is a promising supporting matrix for the immobilization of enzymes.
研究领域:
生物化学
·
材料科学
·
酶工程
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Meng Zhang,Bingxian Chu,Guoying Li,Jianze Xiao,Haowen Zhang,Yujie Peng,Bin Li,Peng Xie,Minguang Fan,Lihui Dong
A series of triethanolamine-modified mesoporous SBA-15 catalysts were synthesized by a facile one-pot process, and used as the catalyst for the synthesis of cyclic carbonates through the cycloaddition of CO 2 with epoxides. The properties of catalysts were characterized by nitrogen adsorption–desorption, elemental analysis (EA), Fourier transform infrared (FT-IR) spectra, Magic angle spinning nuclear magnetic resonance (MAS NMR), X-ray diffraction (XRD), scanning electron microscope (SEM), and transmission electron microscopy (TEM), and the results suggested that triethanolamine (TEA) had been successfully immobilized on SBA-15. It was highly active in the cycloaddition reaction, in which the maximum yield of PC could achieve 93.47% under the conditions as follow: catalyst amount of 0.20 g, reaction temperature of 110 °C, reaction pressure of 2.0 MPa and reaction time of 4 h. Notably, the catalyst can be easily recovered by filtration, and it can be retained most of its catalytic stability and activity after five recycling times. On the basis of the experimental results, the interactions between the catalysts and the substrates were studied by DFT calculations, and the possible mechanism for the reaction was proposed.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）