APPLIED ORGANOMETALLIC CHEMISTRY
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2019
·Vol. 33
·期 6
·e4874
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IF 3.259
Yingpeng Huo,Jiwen Hu,Shudong Lin,Xingming Ju,Yanlong Wei,Zhenzhu Huang,Yangfei Hu,Yuanyuan Tu
Reported herein is an easy-to-prepare novel heterogeneous catalyst of platinum complexes bearing binary ligands of bidentate naphthalenolimine and cyclo-1,5-octadiene that are anchored onto mesoporous silica SBA-15. The presence of the binary ligands not only stabilized the platinum, but also enabled the platinum atoms to form nanoclusters with diameters of ca 1 nm, and led to high platinum loading (8.69 wt%). Moreover, the platinum catalyst exhibited high catalytic activity towards hydrosilylation of terminal alkenes and styrene with silanes under mild and solvent-free conditions, with excellent regioselectivity.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2018
·
IF 3.909
Yongcun Song,Li-Ye Yang,Yang-guang Wang,Di Yu,Jiafeng Shen,Xiao-kun Ouyang
In this work, amino-functionalized Santa Barbara Amorphous-15/calcium alginate (ASBA-15@CA) microspheres were fabricated and characterized by FTIR, SEM, XRD, TGA , and XPS analyses. The Pb(II) adsorption properties of the ASBA-15@CA microspheres were studied in terms of the effects of the adsorption time, adsorbent dose, solution pH, temperature, and initial concentration of Pb(II) on the adsorption capacity. At pH 6 and 298 K, the adsorption reached equilibrium after 100 min and the sample exhibited a good adsorption effect, affording a maximum adsorption capacity of 1029.58 mg/g and a removal rate as high as 98.99%. The adsorption process conformed to the Langmuir model ( R 2 = 0.9937) and followed the pseudo-second-order kinetics model ( R 2 = 0.9995). Regeneration experiments showed that the removal rate of the sample reached 75% even after 6 cycles. Overall, this study provides new insights into the development of novel, highly efficient, and repeatable degradation materials for the removal of Pb(II).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Chi Sun,Yudong Xia,Xue Ye,Wenlin Xu,Hui Shi,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
The direct dimethyl ether (DME) synthesis reaction via CO2 hydrogenation typically requires a bifunctional catalyst that effectively combines a methanol synthesis catalyst with a methanol dehydration catalyst, but the effect of the relationship between the two catalysts on the catalytic performance has not been as well studied. In this study, we developed a CuZnZr/Al–S(10)-PG bifunctional catalyst physically mixed with Al-modified SBA-15 and the traditional CuZnZr catalyst for the hydrogenation of CO2 to DME. A pivotal discovery is that the modulation of interaction intensity between these two constituents significantly influences the electronic configuration of each component. Through X-ray photoelectron spectroscopy characterization and methanol dehydration experiments, it was confirmed that diminishing the synergistic interplay between CuZnZr and Al-modified SBA-15, which regulated the electronic structure of the Cu–Zn interface and enhanced the Cu–Zn interfacial interaction, played a crucial role in enhancing the catalyst’s performance in CO2 hydrogenation to DME. This finding contests established beliefs about the necessity of strong synergistic interactions in such systems and provides new insights for designing rational bifunctional catalysts.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Taipu Chen,Lei Chen,Yutong Zhao,Jinkai Hao,Zhigang Shao
To tackle the challenges of phosphoric acid (PA) leakage and suboptimal proton transfer efficiency in PA-polybenzimidazole (PBI) high-temperature proton exchange membranes (HTPEMs), this research has pioneered the development of a novel porous silicon material, DP/S15, which has been tailored through organic phosphonic acid modification. S15 or DP/S15 was utilized to fabricate PBI composite membranes and subjected these membranes to a thorough examination of their properties. The integration of DP/S15 into the membrane matrix notably enhanced acid uptake and facilitated the formation of a robust and extensive proton transportation network. This was largely attributable to the synergistic interaction between the organic phosphonic acid groups in DP/S15 and PA. As a result, the membranes incorporating DP/S15 exhibited a host of commendable properties, most notably their substantial mechanical strength , which registered at 89.80 MPa with undoped PA and 13.10 MPa with doped PA. Furthermore, theoretical analyses lent credence to the efficient adsorption between DP/S15 and phosphoric acid. Consequently, the composite membranes delivered superior performance metrics, evident in their high conductivity (reaching 57.7 mS cm −1 at 160 °C) and excellent PA retention capabilities (up to 89.5 %). Of paramount significance was the performance of the single fuel cell equipped with the PA-DP/S15-PBI composite membrane, which achieved a peak power density of 672.29 mW cm −2 . This figure impressively surpassed that of the pure PBI membrane by 262.23 mW cm −2 . In light of these promising outcomes, the PA-DP/S15-PBI composite membrane harbors significant potential for deployment in HT-PEMFCs.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2012
·
IF 2.159
Yan-Jing Gu,Bing Yan,Yan-Yan Li
Novel organic–inorganic mesoporous luminescent polymeric hybrid materials containing europium(III) complexes incorporated to mesoporous silica SBA-15/SBA-16 have been prepared by simple physical doping (impregnation) methods, followed by the addition polymerization reaction of the monomer 4-vinylpyridine (vpd) extending along the mesoporous channels. The precursor europium(III) complexes are synthesized by β-diketonate (β-diketonate=2-thenoyltrifluoroacetonate (tta), hexafluoroacetylacetonate (hfac), trifluoroacetylacetonate (taa)) and monomer 4-vinylpyridine (vpd) coordinated to Eu 3+ , and SBA-15/SBA-16 are obtained via a sol–gel process. After the physical doping and the polymerization reaction , the final ternary materials Eu(β-diketonate) 3 pvpd-SBA-15/Eu(β-diketonate) 3 pvpd-SBA-16 (β-diketonate=tta, hfac, taa) are received. The physical properties and espeically the photoluminescence of these hybrids are characterized, and the XRD and BET results reveal that all of these hybrid materials have uniformity in the mesostructure. The detailed luminescence investigation on all the materials show that Eu(tta) 3 pvpd-SBA-16 have the highest luminescence intensity and the materials with taa ligands have longer lifetimes.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Yifan Liu,Jiangang Wang,Yuhan Liu,Yuan Zhang,Hongzi Tan,Hongyou Cui
Herein, a series of Sn-based catalysts supported on SBA-15 with temperature responsive ability to in situ construct acidic and basic sites are reported for efficient conversion of biomass-derived sugars into ethyl lactate (EL). Based on the investigation on the effects of the molar ratio of Cl/OH in Sn(OH) x Cl 2-x and the support types, it is found that Sn(OH) 0.5 Cl 1.5 @SBA-15 is an excellent catalyst in catalytic conversion of various sugars to EL, achieving a maximum EL yield of 68.1 % from sucrose. The in situ generated basic SnO sites play important roles in accelerating the retro-aldol condensation reaction, while the concomitantly released acidic sites (Sn 2 + , SnCl + and H + ) could catalyze the reactions of hydrolysis, isomerization, intermolecular rearrangement and esterification to EL. Benefiting from the temperature responsive effect, not only can the reaction pathways be regulated toward high EL selectivity, but also the catalyst can be recycled easily. This research paves an avenue for exploring efficient catalysts for biomass valorization.
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ENVIRONMENTAL RESEARCH
·
2021
·
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
·
催化化学
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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.
研究领域:
化学工程
·
催化科学
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CHINESE JOURNAL OF CHEMISTRY
·
2011
·Vol. 29
·期 3
·387-398
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
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
·
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
·
2022
·Vol. 102
·期 11
·4714-4723
·
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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