MICROPOROUS AND MESOPOROUS MATERIALS
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2015
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IF 3.453
Hai-Xin Qi,Shang-Ru Zhai,Zhen-Zhen Wang,Bin Zhai,Qing-Da An
Adsorptive desulfurization (ADS) is an effective method for the selective capture of thiophenic sulfur compounds , and the ADS capacity of an adsorbent has been demonstrated to strongly depend on the dispersion degree of active species. Herein, series of zirconia-modified SBA-15 (ZrSBA-15) framework with uniformly dispersed Cu sites have been prepared via a urea-assisted homogeneous deposition strategy, aiming for efficient adsorption towards thiophene . The resultant materials were thoroughly characterized by X-ray diffraction (XRD), N 2 adsorption–desorption isotherms, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and diffuse reflectance spectra (DRS) analysis techniques. It was revealed that the Cu species were highly dispersed inside the ordered ZrSBA-15 framework with platelet morphology, rather than aggregation outside the surface, leading to excellent adsorption capacity for thiophene (up to 9.35 mg/g at 50 °C). The adsorption kinetics and isotherm data can be well described by the pseudo-second-order kinetics model and the Langmuir isotherm, respectively. Spent adsorbent can be regenerated by simple heating treatment in N 2 at 500 °C, without obvious losing of thiophene adsorption capacity even after eight cycles.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 11
·6605-6614
·
IF 3.108
Ce Gao,Qingda An,Zuoyi Xiao,Shangru Zhai
Nowadays, processing of ultra-low sulfur fuel oil has been a hot topic of research all over the world; hence, an efficient adsorption process to tackle this issue is eliciting increasing attention. However, the preparation of high-performance adsorbents is still a challenge. Herein, zirconium-substituted mesoporous SBA-15 with highly dispersed active Cu(I) species has been successfully synthesized by our group at 493 K via a mild vapor-reduction method. The as-prepared material was characterized by powder X-ray diffraction (XRD), nitrogen adsorption and desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and UV-vis diffuse reflectance (DRUV) spectroscopy. All characterization methods demonstrated that the Cu(I) species were highly dispersed in an ordered mesoporous framework with short channels rather than piled on the surface. The as-prepared materials also exhibited an excellent adsorption capacity for thiophene (up to 29.86 mg g−1 at 323 K). Pseudo-second-order kinetics model and Freundlich isotherm can well describe the adsorption kinetics and isotherm data, respectively. More remarkably, an ultrasound-assisted treatment can be effectively employed to regenerate adsorbent, with only a slight reduction in the adsorption capacity after five cycles.
研究领域:
材料科学
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能源化学
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环境工程
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
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IF 4.6
Encheng Liu,Zhenzhen Wang,Zhonghua Sun,Zhihui Zhang,Mingyang He,Qun Chen,Junfeng Qian
The chemical microenvironment modulation of active sites holds promise for facilitating their catalytic performance. Herein, single-atom Ru anchored by ZrSBA-15 modified with diverse organic amine groups has been fabricated and enabled CO2 hydrogenation to produce formic acid (FA) under mild conditions. However, the reaction cannot be achieved without the modification of organic amines. The functional groups as the microenvironment around Ru active sites effectively regulated the activity, in which Ru encapsulated in ZrSBA-15 bearing –NH2 groups exhibited the highest activity, with turnover number (TON) and turnover frequency (TOF) values of 505 and 64 h–1, respectively. Both characterization and experimental results validated that the functional group manipulated the adsorption capacity of the reactant, the electronic state of Ru and hydrophilicity/hydrophobicity of the materials, and thus the catalytic performance.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 74
·70424-70432
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IF 3.289
Ran Ji,Shangru Zhai,Wei Zheng,Zuoyi Xiao,Qingda An,Feng Zhang
Towards the aerobic oxidation of alcohols, palladium nanoparticle immobilized mesoporous catalysts have been extensively investigated; however, the preparation of efficient catalytic materials without using complexing moieties remains a challenge. Herein, a simple yet effective concept that directly utilizes inorganic ZrSBA-15, a mild acidic framework, as a supporting matrix for Pd NPs was applied. The catalysts were fully characterized using X-ray diffraction, N2 adsorption–desorption isotherms, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. It was demonstrated that, on the basis of these characterization results, active Pd NPs had been successfully loaded onto the porous framework of ordered ZrSBA-15. More significantly, the method of preparation was also attributed to the catalytic properties of the resultant sample, in which the interactions between Pd species and acidic framework were improved, leading to a uniform dispersion and enhanced stabilization of Pd particles. Meanwhile, Pd/ZrSBA-15 catalysts exhibited expected activity in the aerobic oxidation of benzyl alcohol with at least 95% conversion and 99% selectivity for benzaldehyde. Moreover, the oxidation reaction could be performed smoothly under solvent- and base-free conditions, and the catalyst was recycled several times with negligible loss in selectivity and conversion.
研究领域:
化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2017
·Vol. 7
·期 11
·2213-2220
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IF 5.773
Zhenzhen Wang,Xiufeng Hao,Dianwen Hu,Lin Li,Xiaojing Song,Wenxiang Zhang,Mingjun Jia
A series of amine-modified ZrSBA-15 supported PdAu bimetallic nanoparticle (NP) catalysts were prepared, and their catalytic properties were studied for the dehydrogenation of formic acid in aqueous solution without any additives. The catalytic activities of the supported PdAu catalysts varied with the change of amines and Pd/Au ratios. The optimized catalyst achieves a very high efficiency under ambient conditions, and even works well at a temperature near the freezing point of the solution. During the preparation process of the catalysts, different organic amines could coordinate with the cations of Au and Pd to produce metal complexes with different structure stabilities and redox properties, and finally result in the formation of PdAu NPs with different particle sizes and dispersion states. The co-existence of small PdAu alloy NPs and the suitable amino groups within the single solid support could provide highly efficient bifunctional sites for synergistically activating FA molecules to produce H2 and CO2.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2014
·Vol. 2014
·期 14
·2337-2344
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IF 2.965
Ling-Yan Meng,Shang-Ru Zhai,Shi Li,Bin Zhai,Qing-Da An,Xiao-Wei Song
Graphical A layer-by-layer deposition strategy was used for the preparation of a tungstophosphoric acid/pentaethylenehexamine/ZrSBA-15 composite. This recyclable material was stable at high temperatures and in polar solvents, and it exhibited excellent catalytic properties (84.7 % conversion, >99 % selectivity) in the selective oxidation of benzyl alcohol (BnOH) to benzaldehyde (BzH). A layer-by-layer deposition strategy was employed for the immobilization of tungstophosphoric acid (HPW) onto a pentaethylenehexamine (PEHA)-grafted ZrSBA-15 framework to a give HPW/PEHA/ZrSBA-15 composite. The resulting composite was characterized by XRD, SEM, TEM, FTIR, thermogravimetric analysis, N 2 sorption, and X-ray photoelectron spectroscopy, and these methods showed that the composite was stable in polar environments. These properties were attributed to the method of preparation, which ensured that a dense and stable array of HPW was encapsulated within the pores of PEHA-modified ZrSBA-15. In the H 2 O 2 -mediated oxidation of benzyl alcohol, the 25 % HPW/PEHA/ZrSBA-15 catalyst exhibited high selectivity (>99 %) for benzaldehyde. Moreover, the oxidation reaction was performed under solvent-free conditions, and the catalyst was recycled several times with negligible loss in selectivity and conversion. This HPW-based catalyst was also efficient at selectively oxidizing other benzylic and alkyl alcohols to the corresponding aldehydes.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Yan-Yun Meng,Qing-Da An,Zuo-Yi Xiao,Shang-Ru Zhai,Zhan Shi
Through hydrothermal synthesis and impregnation-reduction processes, a series of Pd-based nanocomposites using N-doped carbon layers coated ZrSBA-15 as the supports have been manufactured, aiming to upgrade the catalytic activity and stability of the catalysts. Pentaethylenehexamine (PEHA) was served as a nitrogen source to generate N-doped carbon (CN) layers that were pre-deposited into the acidic platelet framework ZrSBA-15, and then followed by introducing Pd 0 nanoparticles (NPs) onto it, finally leading to the formation of target composite Pd/CN-ZrSBA-15. The samples were characterized by XRD , TEM, SEM, N 2 adsorption-desorption isotherm, FTIR, XPS etc. The catalytic performance of as-prepared catalysts was evaluated by the aerobic oxidation of benzyl alcohol and the reduction of 4-NP, respectively. Duo to the platelet-like morphology with shortened channels and the modification of N-doped carbon layers, which could effectively decrease pore blocking in the process of preparation and reactions as well as enhance the metal-support interaction, the derived catalysts could afford 85% conversion of benzyl alcohol and 100% selectivity of benzaldehyde, and the conversion of 4-NP was also up to 96%. More remarkably, the catalysts could be reused at least ten times without significantly loss in catalytic activity.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Lixue Gai,Qingda An,Zuoyi Xiao,Shangru Zhai,Haisong Wang,Weijie Cai,Zhongcheng Li
The configurations and compositions of an absorber play crucial role on the microwave absorption performance. Accordingly, the attenuation mechanism on the nanostructure with skillfully integrated components (e.g. dielectric loss and magnetic loss substances) is a highlight for constructing excellent absorbers. Herein, utilizing hierarchical succulent-like ZrSBA-15 as a template, the N-doped carbon layer containing Co nanoparticles embedded within ZrSBA-15 (Co-NCL@ZrSBA-15) composites were rationally constructed to acquire enhanced microwave absorption performance for the first time. The resultant Co-NCL@ZrSBA-15 composites exhibited high-performance microwave absorption capacity with low loading content of 25 wt % in a wax matrix. The minimum reflection loss (RL) value of −61 dB was achieved with the thickness of 2.0 mm at 16.8 GHz, and an effective frequency bandwidth (RL < −10 dB) was 4.4 GHz (13.6–18.0 GHz). Additionally, the minimum RL value are all less than −30 dB with thickness changing from 2.0 to 5.5 mm in the whole C, X and Ku absorbing band. Such excellent absorbing properties at lower filler loading and thin thickness endow the novel Co-NCL@ZrSBA-15 composites with gigantic potential for application in restrain electromagnetic wave pollution and interference.
研究领域:
材料科学
·
电磁学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2018
·
IF 4.484
Zhenzhen Wang,Haoyang Zhang,Lili Chen,Songsong Miao,Shujie Wu,Xiufeng Hao,Wenxiang Zhang,Mingjun Jia
In this work, a series of amine-modified ZrSBA-15-supported PtPd bimetallic catalysts with different Pt/Pd ratios were prepared and characterized by a variety of means. Introducing amino groups on the surface of ZrSBA-15 is beneficial for achieving high dispersion of PtPd nanoparticles (NPs) and can effectively prevent the overgrowth of PtPd NPs during the preparation process. The resulting hybrid catalysts exhibit very high catalytic activity and stability for H2 generation from aqueous ammonia borane (AB) and can also efficiently catalyze the reduction of p-nitrophenol to p-aminophenol using AB as the hydrogen source. Among them, the catalyst with the Pt/Pd ratio of 85/15 shows the highest activity for AB dehydrogenation under ambient condition, whereas the catalyst with the Pt/Pd ratio of 50/50 exhibits the highest efficiency for the reduction of p-nitrophenol with AB. These results suggest that highly efficient interface active sites could be constructed by optimizing the composition of bimetallic PtPd NPs and changing the chemical surrounding of mesoporous ZrSBA-15, which demonstrate effective synergistic catalysis for AB dehydrogenation and p-nitrophenol reduction.
研究领域:
材料科学
·
催化化学
✓ 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）