Co-reporter:Guojun Lan, Yi Yao, Xiaoming Zhang, Miao Guo, Haodong Tang, Ying Li and Qihua Yang
Catalysis Science & Technology 2016 vol. 6(Issue 7) pp:2181-2187
Publication Date(Web):09 Nov 2015
DOI:10.1039/C5CY01027F
Fischer–Tropsch (F–T) synthesis at low temperature has attracted a lot of research attention due to its thermodynamically favorable nature at low temperature. Herein, we report a highly efficient solid nanoreactor for low temperature liquid-phase F–T synthesis. The solid nanoreactor was fabricated by encapsulation of Ru–PVP nanowires in ethane–silica hollow nanospheres via a one-pot co-condensation method. Under similar reaction conditions, the solid nanoreactor shows higher activity (activity: 6.35 versus 5.96 molCO mol−1Ru h−1) and selectivity towards oxygenate products (41.3 versus 21.6%) than free Ru–PVP in aqueous F–T synthesis. The high activity and selectivity of the encapsulated Ru–PVP is mainly attributed to the low PVP/Ru ratio and the unique yolk–shell nanostructure in increasing the degree of exposure of the active sites. It was also observed that the selectivity towards C5–12 products could be increased to 63.8% in a water/cyclohexane biphasic system. Encapsulation not only gave rise to the quasi-homogeneous Ru–PVP with facile recycling ability, but also enhanced its activity and selectivity towards oxygenates.
Co-reporter:Guojun Lan;Dr. Haodong Tang;Yaping Zhou;Dr. Wenfeng Han; Huazhang Liu;Dr. Xiaonian Li ;Dr. Ying Li
ChemCatChem 2014 Volume 6( Issue 1) pp:353-360
Publication Date(Web):
DOI:10.1002/cctc.201300693
Abstract
Uniform ruthenium nanoparticles (1–2 nm) confined in ordered mesoporous carbon (Ru-OMC) with various embedding degrees have been fabricated by using a boric acid-assisted hard template method. The catalytic performance of Ru-OMC catalysts was determined through the hydrogenation of toluene at 110 °C and 4.0 MPa. The effects of pore size and embedding degree on the catalytic performance were studied and compared with those of OMC-supported ruthenium (Ru/OMC) catalysts with various pore sizes. The catalytic activities of embedding Ru-OMC catalysts are much higher than those of supported Ru/OMC catalysts, which can be attributed to the strong interaction between ruthenium nanoparticles and the carbon support. Furthermore, the activities of Ru-OMC catalysts are closely related to the embedding degree of ruthenium nanoparticles in the carbon matrix. The Ru-OMC catalysts with an appropriate embedding degree affords a turnover frequency of up to 4.69 s−1 in toluene hydrogenation.
Co-reporter:Dr. Ying Li;Guojun Lan;Guoquan Feng;Wei Jiang;Dr. Wenfeng Han;Dr. Haodong Tang ; Huazhang Liu
ChemCatChem 2014 Volume 6( Issue 2) pp:572-579
Publication Date(Web):
DOI:10.1002/cctc.201300873
Abstract
A two-step liquid oxidation approach was developed for the activation of carbon materials. Following nitric acid treatment and subsequent liquid oxidation by a mild oxidant such as H2O2, the number of surface acidic functional groups was increased without destroying the physical structures of the carbon materials. Ruthenium catalysts supported on activated carbon prepared by this two-step liquid oxidation method show significantly improved Ru dispersion and excellent catalytic performance in the hydrogenation of benzene. The dispersion of ruthenium and the catalytic performance of Ru/activated carbon increases monotonically with the amount of surface functional groups.
Co-reporter:Ying LI, Jian ZHONG, Xia-zhen YANG, Guo-jun LAN, Hao-dong TANG, Hua-zhang LIU
New Carbon Materials 2011 Volume 26(Issue 2) pp:123-129
Publication Date(Web):April 2011
DOI:10.1016/S1872-5805(11)60071-1
Ordered mesoporous carbons (OMCs) with adjustable pores were synthesized by using an ordered mesoporous silica, SBA-15 as a hard template and boric acid as a pore expanding agent. The prepared samples were characterized by X-ray diffraction, N2 porosimetry, thermogravimetry, transmission and scanning electron microscopy, and Raman spectroscopy. Results show that the pore size of the prepared samples can be finely tuned in the range of 3–7 nm by using boric acid as the pore expanding agent. The OMCs possess extensive graphitic domains as evidenced by the well-resolved powder X-ray diffraction peaks, Raman spectra, transmission electron microscope images and thermogravimetric curves. This approach gives a simple method that can be widely used in the controlled synthesis of mesoporous carbons.
Co-reporter:Haodong Tang, Guojun Lan, Jian Zhong, Huazhang Liu, Ying Li
Journal of Natural Gas Chemistry (May 2012) Volume 21(Issue 3) pp:275-281
Publication Date(Web):1 May 2012
DOI:10.1016/S1003-9953(11)60365-4
Precise control of the pore sizes for porous carbon materials is of importance to study the confinement effect of metal particles because the pore size in nanosize range will decide the physical and chemical properties of the metal nanoparticles. In this paper, we report a new approach for the synthesis of iron doped ordered mesoporous carbon materials with adjustable pore size using Fe-SBA-15 as hard template and boric acid as the pore expanding reagent. The pore size can be precisely adjusted by a step of 0.4 nm in the range of 3–6 nm. The carbonization temperature can be lowered to 773 K due to the catalytic role of the doped iron. The present approach is suitable for facile synthesis of metal imbedded porous carbon materials with tunable pore sizes.
Co-reporter:Wei Jiang, Ying Li, Wenfeng Han, Yaping Zhou, ... Huazhang Liu
Journal of Energy Chemistry (July 2014) Volume 23(Issue 4) pp:443-452
Publication Date(Web):1 July 2014
DOI:10.1016/S2095-4956(14)60170-4
A series of high surface area graphitic carbon materials (HSGCs) were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x (x is the ball-milling time in hour) catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.The graphitic degree of high surface area graphitic carbons plays an important role in improving the intrinsic catalytic performance of HSGCs supported ruthenium catalysts for ammonia synthesis.Download full-size image
Co-reporter:Guojun Lan, Yi Yao, Xiaoming Zhang, Miao Guo, Haodong Tang, Ying Li and Qihua Yang
Catalysis Science & Technology (2011-Present) 2016 - vol. 6(Issue 7) pp:NaN2187-2187
Publication Date(Web):2015/11/09
DOI:10.1039/C5CY01027F
Fischer–Tropsch (F–T) synthesis at low temperature has attracted a lot of research attention due to its thermodynamically favorable nature at low temperature. Herein, we report a highly efficient solid nanoreactor for low temperature liquid-phase F–T synthesis. The solid nanoreactor was fabricated by encapsulation of Ru–PVP nanowires in ethane–silica hollow nanospheres via a one-pot co-condensation method. Under similar reaction conditions, the solid nanoreactor shows higher activity (activity: 6.35 versus 5.96 molCO mol−1Ru h−1) and selectivity towards oxygenate products (41.3 versus 21.6%) than free Ru–PVP in aqueous F–T synthesis. The high activity and selectivity of the encapsulated Ru–PVP is mainly attributed to the low PVP/Ru ratio and the unique yolk–shell nanostructure in increasing the degree of exposure of the active sites. It was also observed that the selectivity towards C5–12 products could be increased to 63.8% in a water/cyclohexane biphasic system. Encapsulation not only gave rise to the quasi-homogeneous Ru–PVP with facile recycling ability, but also enhanced its activity and selectivity towards oxygenates.
Co-reporter:Zhengliang Jiang, Guojun Lan, Xiaoyan Liu, Haodong Tang and Ying Li
Catalysis Science & Technology (2011-Present) 2016 - vol. 6(Issue 19) pp:NaN7266-7266
Publication Date(Web):2016/07/14
DOI:10.1039/C6CY01049K
A mesoporous ruthenium containing carbon Ru–MC-g catalyst with a semi-embedded uniform Ru particle distribution was synthesized by using a dry grinding method using nano-silica as a hard template. The structure and catalytic performance of the embedded Ru–MC-g catalysts were compared with those of the Ru–MC-i catalyst prepared via a wet impregnation method and the carbon supported Ru catalyst (Ru/MC). Among all the obtained catalysts, the Ru–MC-g catalyst prepared by the dry-grinding process shows excellent hydrogenation catalytic activity performance for the chemoselective hydrogenation of benzoic acid to cyclohexane carboxylic acid. The turnover frequency of the Ru–MC catalyst reaches ca. 2400 h−1 at 4 MPa, 120 °C, which is a 6 times improvement compared with that of supported Ru/MC catalyst. The dry-grinding process is expected to be easily scaled up for large-scale production of Ru-based catalysts.