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ACTA PHYSICO-CHIMICA SINICA · 2017 ·Vol. 33 ·期 7 ·1462-1473 · IF 0.767

Surface Modification of SBA-15 and Its Effect on the Structure and Properties of Mesoporous La0.8Sr0.2CoO3

HUANG Xue-Hui,SHANG Xiao-Hui,NIU Peng-Ju

Mesoporous SBA-15 with mesopore diameter up to 10.1 nm was prepared by a hydrothermal method, and was further functionalized to obtain different surface properties. Thus-prepared SBA-15 was employed as a template to synthesize rhombohedrally crystallized mesoporous La0.8Sr0.2CoO3 perovskite via a nanocasting method. The surface properties of the SBA-15 were adjusted by treatment with concentrated hydrochloric acid, trimethylchlorosilane (TMCS), and 3-aminopropyltriethoxysilane (APTES). A series of characterization techniques verified that all the synthesized templates possessed ordered two-dimensional hexagonal mesoporous structure, and the surface was successfully modified with methyl and amino groups. The mesoporous perovskite structure was formed in the samples and the surface properties of SBA-15 significantly influenced the structure and properties of La0.8Sr0.2CoO3 perovskite oxides. Wide-angle X-ray diffraction patterns suggested that the modified silica templates were conducive to the formation of pure perovskite frameworks with good crystallinity. The catalysts also possessed mesoporous structure, as confirmed by small-angle XRD patterns, high-resolution transmission electron microscopy images, and nitrogen adsorption analysis. Moreover, the La0.8Sr0.2CoO3 materials synthesized using surface-functionalized templates exhibited relatively higher catalytic activity and stability in CO oxidation. Complete CO conversion could be achieved at 140°C #xb0;Cusing the thus-prepared La0.8Sr0.2CoO3 materials, and no significant loss in catalytic activity was observed after 100 h of on-stream reaction experiments. X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, and O2 temperature-programmed desorption experiments revealed that the existence of Co4+, Sr enrichment in the perovskite structure, and high content of adsorbed oxygen species play a critical role in the enhanced catalytic activity of the catalysts. We also proposed the possible reasons for the effect of surface properties of the silica templates on the structure and properties of the La0.8Sr0.2CoO3 nanomaterials.

研究领域: 材料科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Continuous synthesis of mesoporous Y zeolites from normal inorganic aluminosilicates and their high adsorption capacity for dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT)

Wenwu Zhou,Yasong Zhou,Qiang Wei,Sijia Ding,Shujiao Jiang,Qing Zhang,Meifang Liu

Mesoporous Y composites which exhibit both crystallized micropores and large mesopores with narrow mesopore diameter distributions and controlled pore diameters were successfully synthesized. The composite is synthesized through an elaborate design of the SiO 2 @cationic surfactant cetyltrimethylammonium bromide (SiO 2 @CTAB) micelle swelled by an appropriate amount of 1,3,5-trimenthylbenzene (TMB); it is subsequently fabricated from the condensing of the Y zeolite precursors, which contain Y zeolite seeds, on the mesoscale micelle followed by a hydrothermal crystallization process. The effect of synthesis conditions such as the amounts of CTAB, TMB and TEOS added to the synthesis system on the physicochemical properties of the obtained products was examined. The as-synthesized materials were carefully characterized by employing XRD, N 2 adsorption–desorption, SEM, TEM and pyridine-adsorbed FTIR techniques. The mesoporous Y zeolite exhibited both the typical diffraction characteristics of Y zeolites in the wide-angle XRD pattern, and the typical diffraction characteristics of a narrowly dispersed mesopore structure in the small-angle XRD pattern is successfully synthesized for the first time. Finally, the adsorption capacity for DBT and 4,6-DMDBT by samples with different mesopore diameters were assessed by a batch method. Sample MY-0.5C-0.35T-0.9B showed the highest capacity for adsorbing DBT in model diesel, and sample MY-0.5C-0.35T-1.5B showed the highest capacity for adsorbing 4,6-DMDBT in model diesel. Most importantly, sample MY-0.5C-0.35T-1.5B showed the highest adsorptive rate for both DBT and 4,6-DMDBT, which is at least 10 times faster than that of sample MY-0C-0.35T-0B because of the elimination of the diffusion limitation.

研究领域: 材料科学 · 化学工程
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Nanomaterials · 2018 ·Vol. 8 ·期 6 ·427 · IF 3.504

Construction of g-C3N4-mNb2O5 Composites with Enhanced Visible Light Photocatalytic Activity

Meiyin Wang,Hui Wang,Yuanhang Ren,Cheng Wang,Zhewei Weng,Bin Yue,Heyong He

A series of composites consisting of g-C3N4sheet and mesoporous Nb2O5(mNb2O5) microsphere were fabricated by in situ hydrolysis deposition of NbCl5onto g-C3N4sheet followed by solvothermal treatment. The samples were characterized using powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), N2adsorption-desorption, X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance spectroscopy (DRS) and photoluminescence spectroscopy (PL). The photocatalytic activity of the composites was studied by degradation of rhodamine B (RhB) and tetracycline hydrochloride (TC-HCl) in aqueous solution under visible light irradiation (λ> 420 nm). Compared with g-C3N4and mNb2O5, g-C3N4-mNb2O5composites have higher photocatalytic activity due to synergistic effect between g-C3N4and mNb2O5. Among these composites, 4% g-C3N4-mNb2O5has the highest efficiency and good recyclability for degradation of both RhB and TC-HCl.Keywords:photocatalytic degradation;g-C3N4;mesoporous Nb2O5;organic pollutant

研究领域: 材料科学 · 环境科学
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Nanomaterials · 2020 ·Vol. 10 ·期 4 ·686 · IF 4.324

Removal of Cr(VI) from Aqueous Solution by Polypyrrole/Hollow Mesoporous Silica Particles

Linlin Du,Peng Gao,Yuanli Liu,Tsuyoshi Minami,Chuanbai Yu

The removal of Cr(VI) in wastewater plays an important role in human health and environment. In this work, polypyrrole/hollow mesoporous silica particle (PPy/HMSNs) adsorbents have been newly synthesized by in-situ polymerization, which prevent the aggregation of pyrrole in the process of polymerization and exhibit highly selective and powerful adsorption ability for Cr(VI). The adsorption process was in good agreement with the quasi-second-order kinetic model and the Langmuir isotherm model. And the maximum adsorption capacity of Cr(VI) was 322 mg/g at 25 °C. Moreover, the removal rate of Cr(VI) by PPy/HMSNs was ~100% in a number of binary systems, such as Cl−/Cr(VI), NO3−/Cr(VI), SO42−/Cr(VI), Zn2+/Cr(VI), Fe3+/Cr(VI), Sn4+/Cr(VI), and Cu2+/Cr(VI). Thus, the PPy/HMSNs adsorbents have great potential for the removal of Cr(VI) in wastewater.Keywords:polypyrrole/hollow mesoporous silica particle;chromium(Cr);adsorption

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Removal of perfluorooctanoic acid from water with economical mesoporous melamine-formaldehyde resin microsphere

Jing Li,Qian Li,Lu-shuang Li,Li Xu

Perfluoroalkyl and polyfluoroalkyl substances are priority contaminants of global concern. It is urgent to remove them from the environment. Adsorption is an efficient approach, but the adsorption capacity and regeneration of adsorbent were not satisfactory. In the present study, mesoporous melamine-formaldehyde resin microsphere (MMFRS) was fabricated through suspension polymerization. Owing to its mesoporous property and large anion-exchange capacity of 0.3   mmol/g, MMFRS was applied to the adsorption of perfluorooctanoic acid, a model target. The sorption kinetics obeyed pseudo-second-order equation and the sorption isotherms fitted both Freundlich and Langmuir models well. MMFRS exhibited a superiority over commercial powdered activated carbon on the adsorption amount. The sorption could reach equilibrium within 24   h. In addition, the material could be easily and economically regenerated by dilute NH 3 ·H 2 O (7.5   mM); a regeneration percentage (>85%) after 20 recycles was obtained. This study provides a facile, environmentally-friendly and low energy-consumption strategy for removal of perfluorooctanoic acid from aqueous solution in waste-water treatment.

CAS / MDL: 335-67-1 50-28-2
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Mesoporous LaCoO3 perovskite oxide with high catalytic performance for NOx storage and reduction

Wen Xie,Guangyan Xu,Yan Zhang,Yunbo Yu,Hong He

A mesoporous LaCoO 3 perovskite oxide (LaCoO 3 -Meso) with three-dimensionally ordered helical interwoven structure was synthesized by a nano-casting method using KIT-6 as the hard template. The obtained LaCoO 3 -Meso with high surface area was tested for its catalytic performance in the NO x storage and reduction (NSR) reaction and compared with a sample synthesized by the conventional sol-gel method. The LaCoO 3 -Meso showed a significant advantage for NO x storage, with a NO x storage capacity 2 times higher than the regular sample. LaCoO 3 -Meso also exhibited improved NSR catalytic performance in the 150–450 °C temperature range, especially within 350–400 °C, where the NO x conversion was raised for 40%. The results of X-ray photoelectron spectroscopy and X-ray absorption fine structure measurements suggested the presence of a high concentration of oxygen defects on the LaCoO 3 -Meso surface. Further results provided by temperature programmed reduction and temperature programmed desorption indicated that the oxygen defects not only increase the amount of trapped NO x , but also improve the low-temperature redox performance of the catalyst. The lower stability of NO x species adsorbed on oxygen defects promotes the NO x release step in the NSR reaction and benefits the regeneration of storage sites.

研究领域: 材料科学 · 环境科学 · 化学工程
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MICROPOROUS AND MESOPOROUS MATERIALS · 2022 · IF 5.876

Synthesize C@SiO2 with independent spaces produced from carbon slices by the confinement of the silica shell for toluene adsorption

Maosheng Zhang,Zhiqiang Shi,Yongcun Zou,Zongtao Zhang,Runwei Wang,Shilun Qiu

Porous carbons with controlled pore structure have attracted great interest owing to their excellent application potential. Herein, we report a simple synthetic route to synthesize the core-shell C@SiO 2 spheres with various pore structures by calcining core-shell structured RF@SiO 2 (RF = resorcinol-formaldehyde resin). The obtained C@SiO 2 spheres had high surface areas (238.5–732.5 m 2 /g), large pore volume (0.111–0.647 cm 3 /g) and abundant micro-mesoporous structure. The mesopore size of C@SiO 2 spheres can be easily turned in the range of 8–15 nm, by simply modifying the carbonization temperature, size and heating rate of RF@SiO 2 spheres. Among these, S–C@SiO 2 -400 spheres had higher mesopore volume of 0.207 cm 3 /g, this was related to internal carbon slices structure. Meantime, the toluene adsorption capacity of S–C@SiO 2 -400 spheres could reach 448.2 mg/g, which increased by 88.73% compared to ordinary carbon spheres. Moreover, the formation mechanism of the mesopore carbon slices structure was evaluated based on controlled experiments. This work provides a new synthetic method of micro-mesoporous carbon spheres, which can further enrich the application of carbon materials.

CAS / MDL: 108-46-3 108-88-3
研究领域: 材料科学 · 环境科学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2023 · IF 5.2

Rapid synthesis of hierarchical cerium-based metal organic frameworks for carbon dioxide adsorption and selectivity

Jeremiah Amesimeku,Yucheng Zhao,Ke Li,Jinlou Gu

The creation of innovative porous materials for CO 2 capture and separation is proving extremely relevant for environmental sustainability and global warming mitigation. In this study, modified Ce-UiO-66 MOFs were synthesized in 10 min using simultaneous microwave and ultrasound irradiation method. The porosity of the MOF was altered using the soft-templating approach. This strategy resulted in the construction of a hierarchically micro-mesoporous structure with an average mesopore size of 11.10 nm. The as-obtained MOFs, abbreviated as CUT, were characterized with SEM, XRD , FTIR, TGA , BET, and evaluated as CO 2 adsorbents. The results displayed preserved crystal structure, higher thermal stability up to 570 °C. The heightened diffusion of CO 2 molecules to the micropores promoted by mesopore channels, endued CUT with an over-all CO 2 adsorption uptake of 2.53 mmol/g at 273 K at 1 bar outperforming equivalent Ce-UiO-66 MOFs. Notably, the CUT adsorbent showed improved CO 2 /N 2 IAST selectivity (34.2 vs 24.6) and CO 2 isosteric heat of adsorption ( Q st  = 30.15 vs 25 kJ/mol) in contrast to pristine UiO-66 (Zr).

CAS / MDL: 100-21-0
研究领域: 材料科学 · 环境科学
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FUEL · 2023 · IF 7.4

Highly efficient catalytic CO oxidation by balancing the crystal and mesoporous structure of Ta2O5 carrier combined with cobalt

Haijian Qin,Zelong Yang,Qing Xia,PeifeiYao,Chunzhi Zheng,Guangpin Lin,Zhaolian Ye,Songjian Zhao,Fengli Yang

Because the combination of Co and common support (Al, Ti, et al.) usually shows poor catalytic activity, tantalum has been introduced for CO conversion as a novel carrier due to the excellent performance. In this work, Co 3 O 4 was loaded on four forms of tantalum support (amorphous, mesoporous, crystalline and crystalline mesoporous, abbreviated as Co/Ta-am, Co/Ta-me, Co/Ta-cry and Co/Ta-cm, respectively). And among these four states, Co/Ta-cm presents the highest CO conversion rate. The temperature of 90% CO conversion rate of Co/Ta-cm is approximately 130 ℃ at the high space velocity of 780,000 h −1 , which is 70%, 82% and 88% higher than that of Co/Ta-cry, Co/Ta-me and Co/Ta-am, respectively. Moreover, the characteristics of the catalyst have been studied by XRD, SEM, BET, TGA, and H 2 -TPR, and the results reveal that Co/Ta-cm has the excellent crystallinity and stability, and the morphology is regular. X-ray photon spectroscopy and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) have been performed to investigate the reaction mechanism, which indicates that Co 3+ is the active component and lattice oxygen plays a critical role in CO oxidation.

CAS / MDL: 10026-22-9
研究领域: 催化化学 · 材料科学
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Molecular Catalysis · 2023 · IF 4.6

Confined synthesis of highly dispersed Ni anchored on mesoporous carbon as efficient catalyst for water splitting

Shide Wu,Yifei Zhang,Feng Yi,Dan Ping,Wan Li,Siyuan Cheng,Duwei Fan,Lifeng Han,Shiwen Wang,Junfeng Tian,Shaoming Fang

Developing an efficient and low-cost bifunctional electrocatalysts with superior activity for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is highly required but still challenging. Herein, highly dispersed Ni species containing both Ni nanoparticles (NPs) and atomically dispersed Ni-N X on mesoporous nitrogen-doped carbon (Ni-N-C) were prepared by a facile one-pot pyrolysis strategy using dicyandiamide, citric acid and nickel acetylacetonate as raw materials. The confinement agent citric acid is quite requisite for dispersing Ni NPs and forming mesoporous graphene-like carbon substrate. Due to the uniform size of Ni NPs (3 nm) and the synergistic effect between Ni NPs and Ni-N X , and the unique mesoporous carbon structure, such Ni-N-C catalyst exhibits favorable activities for both HER and OER. The overpotentials for HER and OER are only 218 and 330 mV vs. RHE on glassy carbon to deliver a current density of 10 mA·cm −2 , respectively. Moreover, this catalyst also showed good operation durability with no obvious deactivation after long-term (18 h) potentiostatic electrolysis or continuous CV tests. This work could offer a new avenue for the design of bifunctional electrocatalysts in efficient water splitting.

研究领域: 材料科学 · 能源化学
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COMPOSITES PART B-ENGINEERING · 2020 · IF 7.635

Rapid synthesis of solid amine composites based on short mesochannel SBA-15 for CO2 capture

Beibei Ma,Rijia Lin,Hui He,Qinghua Wu,Shuixia Chen

Hydrothermal is common process for synthesizing well-ordered mesoporous silica, however, it costs time and energy simultaneously. To improve the efficiency of synthesis process, it is necessary to propose a facile synthesis strategy with less time and energy requirement. In this study, an innovative non-hydrothermal method using NH 3 ∙H 2 O as catalyst after ripening step is developed to prepare SBA-15 with short mesochannels (SSBA-15) for the first time. The synthesis period of SSBA-15 framework was extremely shortened within 40 min under the optimized conditions (30 min of ripening step and 25% of NH 3 ∙H 2 O concentration), while obtained material exhibits well-ordered hexagonal pore structure and fine particle morphology of SSBA-15 (pore length of 250 ± 50 nm and mesopore size of 9.8 nm). This method can also be employed to synthesize conventional SBA-15 successfully. Moreover, the application of SSBA-15 as support of solid amine adsorbents on CO 2 adsorption and well-fitting of experimental CO 2 adsorption data with Avrami and intraparticle diffusion models reveal that the adsorbents combine the advantages of micro-mesoporous structure, short mesochannel and amine reagents (high affinity of CO 2 ), resulting in enhanced molecular diffusion, fast adsorption kinetics and high CO 2 adsorption capacity . Notably, the solid amine adsorbents exhibited excellent regeneration ability during ten adsorption-desorption cycles. This work opens up new opportunities in efficient preparation of materials that require hydrothermal process.

研究领域: 材料科学 · 环境工程 · 化学工程
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CHEMISTRY-A EUROPEAN JOURNAL · 2014 ·Vol. 20 ·期 7 ·1829-1833 · IF 5.696

Vertically Oriented Silica Mesochannels as the Template for Electrodeposition of Polyaniline Nanostructures and Their Electrocatalytic and Electroanalytical Applications

Longhua Ding,Wanzhen Li,Qiaohong Wang,Qinqin Sun,Yayun He,Bin Su

Graphical Caught on film : Mesoporous silica films (MSF) with vertically oriented mesochannels on a conductive substrate serve as a hard-template for electrodeposition of polyaniline (PANI; ITO=indium tin oxide; see figure). Such PANI nanostructures are confined in an orderly fashion in silica mesochannels and produce a robust hybrid film. The film displays good electrocatalytic activity toward oxidation of ascorbic acid and can be used for potentiometric pH-sensing. A mesoporous silica film (MSF) with vertically oriented mesochannels on a conductive substrate serves as a hard-template for electrodeposition of polyaniline (PANI). The PANI nanostructures thus prepared are orderly confined in silica mesochannels, eventually producing a robust hybrid film. The film displays a good electrocatalytic activity toward oxidation of ascorbic acid, and can be used for potentiometric pH sensing with a Nernstian response.

研究领域: 材料科学 · 电化学 · 分析化学
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