ACS Nano
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2025
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IF 16
Liqun Wang,Jingting Jin,Cunshuo Li,Wenzhi Li,Meng Miao,Liang Yuan
Using monometallic catalysts to selectively catalyze methane to methanol while suppressing the formation of liquid-phase overoxide products is beneficial for industrial applications. However, the balance between yield and selectivity over monometallic active sites remains challenging. This work proposes a strategy anchoring binary rhodium species to influence their surface dispersion properties. Binary Rh species are located both on the inert SBA-15 support surface and in the defect sites, resulting in a sizable methanol yield of 4360 μmol·gcat–1·h–1 and excellent liquid phase selectivity of ∼99%. It has been demonstrated that the reaction mechanism is closely associated with the adsorption state of reaction intermediates on the catalyst surface. The formation of Rh–O–Rh sites leads to significant charge transfer, making the adsorption strength of CO more favorable for generating the key Rh–O active sites. Further exploration shows that the Rh/SBA-15 catalyst facilitates the activation of methane at the Rh–O sites to form *CH3OH adsorbate species, promoting its desorption when CO is coadsorbed.
研究领域:
催化
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化学工程
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材料科学
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表面化学
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反应工程
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PubMed
高影响因子
Chemistry Africa-A Journal of the Tunisian Chemical Society
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2025
·
IF 2.2
Chen Wang,Zhang Fen,Xu Jianghe,Lai Feifan
Purpose To immobilize snailase on SBA-15 to enhance the efficient conversion of Epimedium wushanense extracts for the preparation of rhamnosyl icariside II. Methods The snailase was covalently coupled to amino and aldehyde modified SBA-15, and the immobilization conditions were optimized. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), N 2 adsorption-desorption analysis, scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to characterize the physicochemical properties of immobilized snailase. The optimal enzymatic hydrolysis conditions, enzymatic kinetic parameters, storage stability and reusability of the immobilized snailase were investigated. Results The optimal immobilization conditions were pH 5.0, temperature 30℃, immobilization time 3 h and snailase concentration 10 mg⋅mL − 1 . The immobilized snailase showed a retained activity of 235.8 µmol⋅(h⋅g) −1 and a high enzyme loading capacity of 249.6 mg⋅g − 1 support. The optimum hydrolysis conditions for immobilized snailase were pH 5.5, temperature 50℃, substrate concentration 3.0 mg⋅mL − 1 , and reaction time 6 h. The V max and K m of the immobilized snailase were 3.92 µg⋅min − 1 and 1.18 mmol⋅L − 1 , respectively. Conclusion The immobilized snailase has a high enzyme loading capacity, strong conversion capability, better storage stability and good reusability, making it suitable for the efficient conversion of Epimedium wushanense extracts to produce rhamnosyl icariside II.
研究领域:
酶学
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生物催化
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植物化学
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纳米技术
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生物技术
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ENVIRONMENTAL RESEARCH
·
2021
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IF 6.498
Dan Yu,Jiahong He,Taiping Xie,Qiang Xu,Guoqiang Li,Ling Du,Junhao Huang,Jun Yang,Wenpo Li,Jiankang Wang
The sluggish Ni(II)/Ni(III) redox cycle does not benefit perxymonosulfate (PMS) activation for recalcitrant pollutant degradation . To solve this problem, a heterogeneous catalyst, Cu 0.2 Ni 0.8 O/SBA-15 (CNS), was constructed to activate PMS for decomposing two sulfonamide antibiotics, sulfachlorpyridazine (SACP) and sulfapyridine (SAP). SACP and SAP were completely degraded over Cu 0.2 Ni 0.8 O/SBA-15/PMS (CNSP) after 90 min. O 2 .- was the dominant active species involved in the degradation of SACP and SAP. Structural analysis and elemental valence state observations indicated that Cu(Ⅰ) provided electrons through Cu–O–Ni bonds to realize the charge compensation for Ni(Ⅲ) in the CNSP system. Thus, the in situ Cu(I)/Cu(II) promoting the Ni(II)/Ni(III) cycle could accelerate the PMS activation. This work provides new insights into the electron transfer between transition metals and the charge compensation mechanism for PMS activation. The degradation mechanism was proposed based on the XPS results before and after the reaction, a radical quenching test, and an EPR test. Combined with the SACP and SAP degradation intermediates identified by LC-MS, we suggest that the choice of treatment process depends on the occurrence of a steric hindrance effect between the molecular structure of the degradation target and free radicals.
研究领域:
环境科学
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催化化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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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.
研究领域:
化学工程
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催化科学
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CHINESE JOURNAL OF CHEMISTRY
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2011
·Vol. 29
·期 3
·387-398
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IF 0.773
Yan Liu,Zhanchao Liu,Jiangdong Dai,Jie Gao,Jimin Xie,Yongsheng Yan
A novel surface ion imprinted adsorbent [Co(II)-IIP] using polyethyleneimine (PEI) as function monomer and ordered mesoporous silica SBA-15 as support matrix was prepared for Co(II) analysis with high selectivity. The prepared polymer was characterized by Fourier transmission infrared spectrometry, scanning electron microscopy, X-ray diffraction and nitrogen adsorption-desorption isotherm. Bath experiments of Co(II) adsorption onto Co(II)-IIP were performed under the optimum conditions. The experimental data were analyzed by pseudo-first-order and pseudo-second-order kinetic models. It was found that the pseudo-second-order model best correlated the kinetic data. The intraparticle diffusion and liquid film diffusion were applied to discuss the adsorption mechanism. The results showed that Co(II) adsorption onto IIP was controlled by the intraparticle diffusion mechanism, along with a considerable film diffusion contribution. Langmuir, Freundlich and Dubinin-Radushke- vich adsorption models were applied to determine the isotherm parameters. Langmuir model fitted the experiment data well and the maximum calculated capacity of Co(II) reached 39.26 mg/g under room temperature. The thermodynamic data were indicative of the spontaneousness of the endothermic sorption process of Co(II) onto Co(II)-IIP. Co(II)-IIP showed high affinity and selectivity for template ion compared with non imprinted polymer (NIP).
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FUEL
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2023
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IF 7.4
Tingting Liu,Yangyang Guo,Lei Luo,Meng Ye,Wen Liu,Tingyu Zhu
Solid amine adsorbents hold promising application prospects in the realm of industrial flue gas decarbonization. Nevertheless, there remains a need for substantial improvement in the cycling stability of solid amine adsorbents. Additionally, the competitive adsorption mechanism of solid amine adsorbents pertaining to flue gas components lacks thorough verification. In this study, amine-grafted micro-mesoporous ZSM-5/SBA-16 adsorbents were synthesized to improve the CO 2 adsorption capacity and investigate the effect of impurity gases on CO 2 adsorption. Various characterization techniques, including X-ray diffraction (XRD), thermogravimetric analysis (TGA), N 2 adsorption, and elemental analysis, were employed to analyze the properties of the adsorbents. The loading analysis of the micro-mesoporous molecular sieve revealed that ZS-A-2.0 exhibited the highest CO 2 adsorption capacity of 41.39 mg/g. Mass spectrometry was utilized to evaluate the co-adsorption experimentation involving multicomponent gases. The breakthrough curves of CO 2 displayed dual stages at low concentrations, suggesting the simultaneous occurrence of physical and chemical adsorption throughout the entire adsorption process. Based on temperature programming desorption (TPD) and in situ Fourier transform infrared spectroscopy (FTIR), the results indicated a notable enhancement in CO 2 adsorption due to the presence of H 2 O. Conversely, the presence of SO 2 and NO exhibited adverse effects on CO 2 adsorption, consequently hindering the formation of carbamate and (RNH 3 ) 2 CO 3 adsorption products. This study presents, for the first time, a comprehensive investigation into the interactive adsorption mechanism and product distribution between CO 2 and impurity gases. The findings presented herein provide valuable insights and essential support for practical flue gas applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Qinya Huang,Zhiwei Ding,Haoran Lu,Maoxiang Geng,Jinhua Liu,Minjia Meng,Zhanchao Liu,Yan Liu,Jianming Pan
Novel 3D mesoporous silica SBA-15 and 2D graphene oxide (GO) composite nano-fillers incorporated polysulfone (PSf) ultrafiltration (UF) membranes (GO-SBA-15/PSf) were first prepared via blending modifications by non-solvent induced phase separation (NIPs). 3D honeycomb-like SBA-15 not only improved the surface hydrophilicity but also provided extra nano-channels parceled in 2D GO networks for convenient hydrone transport via confinement-effect. The lamellar GO networks relieved the agglomeration of inorganic materials inside the polymer, anticipating in the interfacial polymerization reaction. GO-SBA-15/PSf UF membranes were systematically investigated using contact angle, scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscope (AFM) and Brunauer-Emmett-Teller (BET) methods. The pure water flux reached 641.7 L m -2 h −1 which was 3 times than that of pristine PSf membranes (229.2 L m -2 h −1 ) under the pressure of 0.1 MPa. Negative charge of GO generated electrostatic repulsion with protein, which facilitated a high rejection of 98.22% and excellent FRR value of 85% that was 1.5 times than that of pristine PSf membranes (58%). The UF membranes fabricated by new multidimensional nano-fillers overcame the trade-off effect between permeability and protein rejection.
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Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Xiuqin Dong,Jianhang Tian,Junwei Lei,Yifei Chen
Copper as a non-noble metal catalyst has great prospects in the hydrogenation of acetic acid to ethanol. In this paper, Cu-MnO/SBA-15 catalysts with highly catalytic performance and stability were prepared. The mechanism was elucidated by experiments and DFT calculations . The Cu and MnO were coexistent on reduced x Cu y Mn/SBA-15. Appropriate Cu/Mn ratio was beneficial for increasing the Cu surface area and reducing the size of Cu. The rate-controlled step was found and the MnO could effectively lower the difficulty of acetaldehyde formation by dioxyethylidene. DFT calculations indicated that the formation of ethyl acetate at the Cu-MnO interface was largely prevented. The optimal catalytic hydrogenation activity was obtained for 9Cu1Mn/SBA-15, with the conversion of acetic acid and selectivity of ethanol of 99.9% and 90.1%, respectively. The catalytic activity could remain within 72 h which was more stable than the original Cu-based catalyst.
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
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2022
·Vol. 102
·期 11
·4714-4723
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IF 4.125
Ke Cheng,Jianghua Zhang,Shasha Yang,Fawen Yin,Zixuan Li,Ting Wang,Dayong Zhou
BACKGROUND Efficient and sustainable production of structured phospholipids (SPLs) enriched in medium-chain fatty acids (MCFAs) in a heterogeneous manner is crucial for their potential applications in functional foods and drugs. Herein, for the first time, Zn- and Al-incorporated SBA-15 silicas were prepared by the coprecipitation method and further researched for catalytic synthesis of MCFA-enriched SPLs through acidolysis reaction of natural phospholipids with capric or caprylic acid. RESULTS The as-prepared Zn- and Al-incorporated SBA-15 samples exhibited superior catalytic activities under mild experimental conditions (50 °C, 6 h) to commercial homogeneous Lewis acids and benchmark enzymes. Correspondingly, the capric acid and caprylic acid incorporations were respectively achieved up to ~40.25 ± 0.40% (or 35.08 ± 0.09%) and 37.26 ± 0.38% (or 33.02 ± 0.13%) for Zn- (or Al-) incorporated SBA-15 catalyst. Moreover, various methods such as scanning electron microscopy with energy-dispersive X-ray spectrometry, ultraviolet–visible diffuse reflectance spectroscopy and pyridine–Fourier transform infrared spectroscopy were utilized to characterize the two catalysts in order to elucidate the possible structure–performance relationship. Accordingly, the above-mentioned satisfactory results are most probably due to the well-ordered mesostructures and large amounts of active Lewis acid sites existing in the investigated materials. Noticeably, the two catalysts featured good separation and excellent recyclability as well. CONCLUSION The Zn- and Al-incorporated SBA-15 catalysts studied in this work might shed light on novel, sustainable and economic alternatives for effective SPL production to diminish the applications of conventional homogeneous catalysts and biocatalysts in food industries. © 2022 Society of Chemical Industry.
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高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2021
·Vol. 44
·期 22
·4181-4189
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IF 3.645
Lixin Song,Huige Wang,Chaofan Rui,Qing Liu,Yunxia Zhang,Yong Cheng,Juan He
Mesoporous silica Santa Barbara-15 was functionalized by methacryloxypropyl trimethoxysilane. Taking this as the carrier material, a new mesoporous silica surface imprinted polymer was synthesized by using the C=C bond, functional monomer α-methacrylic acid, and crosslinker ethylene glycol dimethacrylate, which was used to extract aflatoxin from grain efficiently. It is different from the preparation of surface imprinted polymers which is physically wrapping carrier materials with polymer layers. The chemical grafting method makes the coating of the polymer layer more controllable. A new method for selective separation, enrichment, and determination of trace aflatoxin in grain was established by using the polymers as the filter of the solid-phase extraction column and high-performance liquid chromatography. The linear range of the method was 0.5–100 μg/kg, R 2 = 0.9990–0.9993. The recovery of aflatoxin G2, G1, B2, and B1 was 98.9–119.7% and the relative standard deviation was 3.07–5.76%. By comparing the self-made column with the immunoaffinity column, it was found that the self-made column had better extraction performance for aflatoxins than the immunoaffinity column. It can be used for the analysis and detection of aflatoxins in cereal.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Xi Cheng,Qingge Feng,Dachao Ma,Hongcheng Chen,Xu Zeng,Feifan Xing,Jiayang Teng
To eco-friendly catalyze glucose to levulinic acid, recyclable acid catalyst has been researched. The synthesis process of propyl sulfonic acid functionalized SBA-15 was improved and the hydrophobic treatment was performed. The structure and functional groups of materials were characterized by X-ray diffraction, transmission electron microscopy , N 2 adsorption–desorption isotherms, elemental analysis, Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy and simultaneous thermal analysis. The catalytic activity , recyclability and hydrothermal stability of CH 3 -SBA-15-SO 3 H material were researched. The highest yield of levulinic acid at 61.56% was obtained at 180 ℃ for 2.5 h in γ-GVL-water solvent system, and the yield of levulinic acid was only decreased by 2% after 4 times reuse. The high degree of silicon polycondension and hydrophobic surface of CH 3 -SBA-15-SO 3 H were the key to maintain the hydrothermal stability. The CH 3 -SBA-15-SO 3 H solid acid had great potential in development and utilization of biomass resources .
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Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 19
·3636-3645
·
IF 5.958
Yifei Ye,Dazhi Li,Ping Xu,Jianmin Sun
Until recently, many metal-based catalysts have been developed for the cycloaddition reaction of CO2 with epoxides. However, the leaching of the active metal component would lead to various environmental problems. A novel nonmetal B-doped Lewis acid–base catalyst with hydrogen bond donor (HBD) groups (B-SBA-15-NH2) was prepared successfully through the hydrothermal process and post-modification. B-SBA-15-NH2 exhibited good catalytic performance for the CO2 cycloaddition reaction, and 95% yield of propylene carbonate and satisfied selectivity (98%) were achieved in the presence of the KI cocatalyst. The efficient catalytic activity of B-SBA-15-NH2 resulted from the synergistic effects of B and HBD groups, together with the functionalized –NH2 groups. B-SBA-15-NH2 also exhibited good generality with acceptable yields for the corresponding cyclic carbonates in the CO2 cycloaddition with various epoxides. Furthermore, the developed B-SBA-15-NH2 catalyst could be easily separated by centrifugation and reused for five runs without an obvious loss in activity. The good activity and stable reusability of the metal-free B-SBA-15-NH2 catalyst demonstrate that it is a promising green candidate catalyst in the field of CO2 conversion.
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