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Chinese Journal of Catalysis
2007, Vol. 28, No. 5
Online: 25 May 2007

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Selective Hydrogenation of Cinnamaldehyde by Ionic Copolymer-Stabilized Pt Nanoparticles in Ionic Liquids ZOU Ming;MU Xindong;YAN Ning;KOU Yuan* 2007, 28 (5):  389-391.  Abstract ( 2442 )   [Full Text(HTML)] () PDF (241KB) ( 1126 )   An ionic copolymer, poly(NVP-co-VBIM+Cl-), was used to stabilize the platinum nanoclusters in [bmim]BF4 ionic liquid. The nanoclusters obtained were uniform in size and very stable. The catalytic performance of the platinum nanoparticles was tested by selective hydrogenation of cinnamaldehyde. The system exhibited excellent selectivity (>95%) for cinnamic alcohol with high conversion (>90%), and the catalysts were recycled with the activity and selectivity preserved.

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Effect of CeO2 Redox Behavior on the Catalytic Activity of a VOx/CeO2 Catalyst for Chlorobenzene Oxidation GUAN Yejun;LI Can* 2007, 28 (5):  392-394.  Abstract ( 2133 )   [Full Text(HTML)] () PDF (188KB) ( 1161 )   Three CeO2 samples were prepared by precipitation with urea, ammonia, and sodium carbonate. Vanadium oxide was supported on these CeO2 materials, and their catalytic activity in the total oxidation of chlorobenzene was investigated. Their turnover frequencies for chlorobenzene oxidation are 4.9, 1.6, and 0.8 h-1at 300 ℃, respectively, and depend on the redox properties of the CeO2 supports. These results demonstrate that the oxygen of theV-O-Cebond plays an important role in determining the catalytic activity of the VOx/CeO2 catalyst.

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Activity and Stability of ZnFe0.25Al1.75O4 Catalyst in Catalytic Wet Air Oxidation of Phenol XU Aihua;LU Xiaoyang;YANG Min;DU Hongzhang;SUN Chenglin* 2007, 28 (5):  395-397.  Abstract ( 2232 )   [Full Text(HTML)] () PDF (195KB) ( 846 )   The ZnFe0.25Al1.75O4 spinel type catalyst prepared by the sol-gel method was tested for catalytic wet air oxidation of phenol. High activity and stability were obtained for the catalyst. After five successive reactions, there were still 100% of phenol conversion and 88.7% of COD removal. During the phenol degradation, the returning of leached iron to the catalyst surface was observed, and as a result the amount of iron leaching in the final effluent was very low. After the fifth reaction run, the amount of iron leaching was 2.15 mg/L, and the zinc leaching was 1.53 mg/L.

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Rapid Synthesis of MCM-36 Zeolite under Ultrasonic Treatment WANG Baoyu;WU Jianmei;LI Niu;YUAN Zhongyong;XIANG Shouhe* 2007, 28 (5):  398-400.  Abstract ( 1935 )   [Full Text(HTML)] () PDF (215KB) ( 861 )   Using tetramethylammonium silicate as the pillaring agent, the effects of ultrasonic treatment on the synthesis of the MCM-36 zeolite were investigated. The results show that with the assistance of ultrasonic wave, the intercalation process, in which the pillaring agent enters into the swollen MCM-22 precursor, can be accelerated markedly. The MCM-36 zeolite with various interlayer distances can be synthesized by controlling the ultrasonic time in the intercalation process, and the interlayer distance in the MCM-36 zeolite synthesized is identical.

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Medium-Coupled Catalysts Meeting Euro Ⅲ Emission Standards for Condensed Natural Gas Vehicles YUAN Shuhua;WANG Yongjun;SHI Zhonghua;ZHAO Ming;GONG Maochu;LIU Zhongchang;CHEN Qizhang;CHEN Yaoqiang* 2007, 28 (5):  401-403.  Abstract ( 1925 )   [Full Text(HTML)] () PDF (170KB) ( 1068 )   The Ce0.45Zr0.45Y0.05La0.05O2 oxygen storage material and La-stabilized alumina (La-Al2O3) were prepared. After aging at1000℃ for5 h, Ce0.45Zr0.45Y0.05La0.05O2 maintains superior textual and oxygen storage properties, and La-Al2O3 shows superior textual properties. Medium-coupled Pt-Rh monolithic catalysts for condensed natural gas (CNG) vehicles were prepared by impregnating Ce0.45Zr0.45Y0.05La0.05O2 and La-Al2O3 with H2PtCl6 and RhCl3 solutions and then washcoated on the cordierite honeycomb. The medium-coupled catalysts showed high activity at low temperature and thermal stability. The results from the emission test of JETTA-MT CNG vehicle indicated that the prepared catalysts were capable of fulfilling Euro Ⅲ requirements.

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ZnBr2-Quaternary Onium Tribromide Salt as a Catalyst for the Coupling Reaction of Carbon Dioxide and Epoxides CHANG Tao;WU Mei;JIN Lili;JING Huanwang*;QIU Wenyuan 2007, 28 (5):  404-406.  Abstract ( 2420 )   [Full Text(HTML)] () PDF (160KB) ( 967 )   A catalyst system of ZnBr2-quaternary onium tribromide salt has been developed for the coupling reaction of carbon dioxide and epoxides. The effects of metal salts and reaction conditions and the recyclability of the catalysts were investigated. The results demonstrated that the coupling reaction of CO2 and epoxides to form cyclic carbonates with high yield proceeds very effectively at 413 K under 1.0 MPa by using ZnBr2 in conjunction with the phenyltrimethylammonium tribromide co-catalyst without solvent.

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Gas-Phase Hydroxylation of Chlorobenzene Over Cu-HZSM-5 and Catalyst Deactivation CHEN Lingjing;LIN Haiqiang*;YAN Bin;YANG Lefu 2007, 28 (5):  407-412.  Abstract ( 2296 )   [Full Text(HTML)] () PDF (304KB) ( 965 )   Catalytic performance and deactivation of the Cu-HZSM-5 catalyst for gas-phase hydroxylation of chlorobenzene to phenol were studied. Under the conditions of 773 K and water/chlorobenzene volume ratio of 3, a chlorobenzene conversion of 82.4% and a phenol selectivity of 98.2% were obtained. Deactivation of the Cu-HZSM-5 catalyst was observed during the reaction. Characterization byX-raydiffraction, N2 static adsorption, energy dispersive X-ray spectroscopy, and infrared spectroscopy of adsorbed pyridine was performed on fresh, used, and regenerated catalysts to study the essence of the catalytic reaction and catalyst deactivation. The leaching of copper from the catalyst, framework dealumination of HZSM-5, and coking were the main causes for the catalyst deactivation.

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Liquid-Phase Oxidation of Alcohols Catalyzed by ZrO2 under Solvent Free Conditions Mohammad ILYAS;Mohammad SADIQ;Imdad KHAN 2007, 28 (5):  413-416.  Abstract ( 2060 )   [Full Text(HTML)] () PDF (220KB) ( 953 )   The selective oxidation of alcohols, in an environmental friendly protocol, was carried out under solvent free conditions using molecular oxygen as the oxidant and ZrO2 as the catalyst. Benzaldehyde, cyclohexanone, and octanal were the major products from their respective alcohols. The influence of different reaction parameters (speed of agitation, reaction time, and temperature), catalyst parameters (calcination temperature and loading), and oxygen partial pressure on the catalyst performance was studied. ZrO2 calcined at1223K was found to be more active than the one calcined at 723 for the alcohol oxidation to the corresponding carbonyl products. The catalyst is insoluble in the reaction mixture and can be easily separated by simple filtration and reused. The agitation speed beyond 900 r/min show no significant effect on the rate of conversion.

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Structure of Sn/Al2O3 Catalyst and Its Activity for Selective Catalytic Reduction of NO GUO Xikun*;WANG Xiaoming;CHEN Qingsheng 2007, 28 (5):  417-422.  Abstract ( 1846 )   [Full Text(HTML)] () PDF (526KB) ( 771 )   A series of Sn/Al2O3 catalysts were prepared by co-precipitation of SnCl4 and an aluminum salt using different precipitants. The catalyst activity for the selective catalytic reduction of NO by propylene in excess oxygen was investigated. The relationship between the catalytic property and the structure of the Sn/Al2O3 catalysts was explored usingX-raypowder diffraction, scanning electron microscopy, N2 adsorption-desorption, infrared spectroscopy of adsorbed pyridine, and temperature-programmed reduction. The results indicated that over the Sn/Al2O3 catalyst prepared using NH3•H2O and NH4HCO3 as the precipitants and NH4Al(SO4)2 as the aluminum source, NO conversion was the highest (90.9%) at 350 ℃, and the optimal catalytic temperature was lowered to 350 ℃. The specific surface area and the pore volume of this catalyst were 254 m2/g and 0.878 cm3/g, respectively. Distribution of pore size lied in the range of 3-8 nm, and dual-peak nano-structure was observed. Most of Sn species existed as crystalline SnO2. The introduction of NH4Al(SO4)2 increased the amount of Lewis acidity of the catalyst.

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Reaction Mechanism for Selective Oxidation of Supercritical Propane Catalyzed by β-Hexa-heptabromo-tetrakis (Pentafluorophenyl) Porphyrinato Iron LIU Yinong;XU Zhiming*;SUN Xuewen;ZHAO Suoqi;WANG Renan;LONG Jun 2007, 28 (5):  423-428.  Abstract ( 2298 )   [Full Text(HTML)] () PDF (312KB) ( 843 )   Using BHT (butylated hydroxyltoluene, i.e.,2,6-ditertbutyl-4-methylphenol) as a radical trap, the reaction mechanism for oxidation of supercritical propane catalyzed by β-hexa-heptabromo-tetrakis(pentafluorophenyl) porphyrinato iron was investigated. A small amount of BHT significantly promoted the reaction, whereas its extra amount restrained the reaction. Besides the propyl radical, the isopropoxy radical and a small quantity of oxidation products such as n-hexane, i-hexane, and di-isopropyl peroxide were detected, being the very important evidence to the reaction mechanism of radical chain autooxidation. The minimum other products such as ethanol, acetic acid, and propionic acid could not be explained upon this reaction mechanism.

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Glow Discharge Plasma-Enhanced Preparation of Nickel-Based Catalyst for CO2 Methanation GUO Fang;CHU Wei*;XU Huiyuan;ZHANG Tao 2007, 28 (5):  429-434.  Abstract ( 2552 )   [Full Text(HTML)] () PDF (353KB) ( 1040 )   The novel Ni-based catalyst for CO2 methanation, Ni-La/γ-Al2O3, was prepared by the plasma method and the effect of the plasma introduction mode on the catalytic performance was investigated. The catalyst treated with plasma followed by reduction exhibited high activity at low temperature. The CO2 conversion over this catalyst was 84.6% under the conditions of 101.325 kPa,13500h-1, H2/CO2 molar ratio of 2.5, and 250 ℃, whereas that over the conventional catalyst was 57.4%. The catalyst was characterized using temperature-programmed reduction and desorption, oxygen titration, N2 adsorption,X-raydiffraction,X-rayphotoelectron spectroscopy, and thermogravimetry analysis. The results indicated that the plasma treatment enlarged the surface area of the sample, favored the formation of small size crystals, and facilitated the high dispersion and enrichment of the Ni element on the catalyst surface.

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Effects of Calcination and Reduction Temperature on Catalytic Performance of Ni/TiO2 Catalyst for Hydrogenation of p-Nitrophenol to p-Animophenol YIN Hongwei;CHEN Jixiang*;ZHANG Jiyan 2007, 28 (5):  435-440.  Abstract ( 2278 )   [Full Text(HTML)] () PDF (381KB) ( 1303 )   The effects of calcination and reduction temperature on the properties of the Ni/TiO2 catalyst were studied by means ofX-raydiffraction, temperature-programmed reduction, H2 chemisorption, and the performanceevaluationfor hydrogenation of p-nitrophenol. The results showed that nickel species existed in the form of NiO in the catalysts calcined at ≤923 K, and the interaction between NiO and TiO2 was enhanced with the increase in calcination temperature. However, nickel species existed in the form of NiTiO3 in the catalyst calcined at1023K. For the catalysts calcined at ≤923 K and reduced at 723 K, there was no remarkable difference in the nickel crystallite size, whereas the amount of H2 chemisorption decreased as the calcination temperature increased, which was due to the increase of the interaction between nickel and TiOx (x<2). The catalyst calcined at 923 K showed better catalytic performance for hydrogenation of p-nitrophenol than the ones calcined at lower temperatures, which was also closely related to the strong interaction between nickel and TiOx species. The reduction temperature also deeply affected the properties of Ni/TiO2. At low reduction temperature, the catalyst could not be reduced completely, while the high reduction temperature would cause nickel sintering and an excessively strong interaction between nickel and TiOx, leading to a decrease in H2 chemisorption amount, all of which were not beneficial to the catalytic performance. The suitable reduction temperature was 673 K. It was suggested that both the suitable interaction between nickel and TiOx species and the suitable H2 chemisorption amount favored the harmonious effect of nickel and TiOx on the activation of the -NO2 group.

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Effect of Supports on Catalytic Performance of Palladium Catalysts for Hydrogenation of Phenol to Cyclohexanone ZHU Junhua;DING Jielian;ZENG Chongyu* 2007, 28 (5):  441-445.  Abstract ( 2329 )   [Full Text(HTML)] () PDF (255KB) ( 1563 )   The Pd/MgO, Pd/Al2O3, and Pd/HT catalysts with 0.5% Pd contents were prepared by the impregnation method using MgO,γ-Al2O3, and hydrotalcite (HT) as the support, respectively, and PdCl2 as the precursor. Catalytic performance of the catalysts for hydrogenation of phenol to cyclohexanone was evaluated in a fixed-bed reactor. These catalysts were characterized byX-raydiffraction, N2 adsorption, H2 temperature-programmed desorption, CO2 temperature-programmed desorption, andX-rayphotoelectron spectroscopy. The results showed that bigger average pore diameter, higher surface Pd content, and more surface base sites were favorable for the adsorption of hydrogen and phenol and consequently increased the conversion of phenol and the selectivity for cyclohexanone. Under the conditions of 130 ℃, H2∶phenol molar ratio = 4∶1, and LHSV=0.19 h-1, the conversion of phenol was 90% and the selectivity for cyclohexanone reached 97% over the 0.5%Pd/HT catalyst.

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Promotion Effect of Xylose Co-substrate on Stability of Catalytic System for Asymmetric Redox of (R,S)-1-Phenyl-1,2-ethanediol to Its (S)-Enantiomer by Candida Parapsilosis LV Tengfei;XU Yan*;MU Xiaoqing;NIE Yao 2007, 28 (5):  446-450.  Abstract ( 2643 )   [Full Text(HTML)] () PDF (312KB) ( 1288 )   The asymmetric redox of (R,S)-1-phenyl-1,2-ethanediol to its optically active (S)-enantiomer catalyzed by Candida parapsilosis in an aqueous phase was investigated. A new efficient and economical cofactor regeneration system was established using D-xylose as the co-substrate by analyzing the reaction mechanism and the metabolic pathway of sugars in yeast. The results showed that the xylose co-substrate was advantageous for the stability of the catalytic system in a repetitive batch mode. In the presence of xylose (8 g/L), the optical purity and the yield of the (S)-enantiomer were increased by 14% and 10%, respectively. Furthermore, whole cells could be reused3-4times and the enantiomeric excess of the (S)-enantiomer remained at a high level of 98%. The effects of xylose on the accumulation of 2-hydroxyacetophenone in repetitive batch experiments and the asymmetric reaction catalyzed by carbonyl reductases from recombinant Escherichia coli were investigated. It was proposed that xylose improved the stability of the catalytic system by strengthening the (S)-carbonyl reductase system, in which NADPH that is necessary for the asymmetric reaction could be regenerated via the pentose phosphate pathway of xylose metabolism.

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Functionalization Transform of Polystyrene by Phase-Transfer Catalysis ZHU Yong;GAO Baojiao*;ZUO Haili 2007, 28 (5):  451-456.  Abstract ( 2129 )   [Full Text(HTML)] () PDF (350KB) ( 1097 )   The nucleophilic substitution reaction of chloromethylated polystyrene was performed using the sodium salt of p-hydroxybenzaldehyde as the nucleophilic substitution agent via phase-transfer catalysis, and polystyrene with aldehyde groups on its side chains was prepared. The structure of the product was characterized by FT-IR spectroscopy. The effects of various factors, such as the polarity of solvents, the kind and used amount of the catalysts, and the ratio of organic phase to water phase, on the phase-transfer catalysis reaction were studied, and these effects were analysed according to the reaction mechanism and kinetics theory. The results showed that functionalization of polystyrene could be realized by phase-transfer catalysis, the chlorine atoms on the chains of chloromethylated polystyrene could be favorably transformed, and polystyrene with aldehyde groups on its side chains was successfully obtained. For this phase-transfer catalysis system, the suitable catalyst is tetrabutylammonium bromide, the solvent with stronger polarity is favorable, and the fitting volume ratio of organic phase to water phase is equal to 1/2.

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Nano-Ag/ZnO Photocatalyst and Its Catalytic Performance for Degradation of Nonylphenol Ethoxylate-10 ZHANG Jingfeng;DU Zhiping*;ZHAO Yonghong;TAI Xiumei 2007, 28 (5):  457-462.  Abstract ( 2527 )   [Full Text(HTML)] () PDF (402KB) ( 1101 )   Ag-modified nano-ZnO samples with different Ag loadings were prepared by the ammonia immersion method. The crystal structure, specific surface area, surface composition, and spectral characteristics were analyzed byX-raydiffraction, N2 adsorption,X-rayphotoelectron spectroscopy, and diffuse reflectance ultraviolet-visible spectroscopy, respectively. The photocatalytic activity of Ag/ZnO samples for degradation of nonylphenol ethoxylate-10 (NPE-10) was studied under the irradiation with ultraviolet light and visible light. The results showed that Ag could be successfully supported on the nano-ZnO surface. The particle size of Ag/ZnO increased and its specific surface area decreased with the increase of Ag loading. Compared with the nano-ZnO, the binding energy of Ag 3d5/2in Ag/ZnO dropped, but the binding energy of Zn 2p and O 1s increased. The contents of adsorbed oxygen and hydroxy oxygen on the Ag/ZnO surface increased remarkably in contrast to that of the pure ZnO sample. The 0.5%Ag/ZnO exhibited a red shift in the absorption spectrum. The photocatalytic activity of the 0.5%Ag/ZnO sample was the highest, and the degradation rate of NPE-10 was 77% and 56% under 3 h irradiation of ultraviolet light and visible light, respectively.

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Effect of Doped Ag on Performance of Manganese Oxide Octahedral Molecular Sieve for CO Oxidation HU Rongrong;CHENG Yi;XIE Lanying;WANG Dezheng* 2007, 28 (5):  463-468.  Abstract ( 2059 )   [Full Text(HTML)] () PDF (439KB) ( 1094 )   A series of Ag-doped manganese oxide octahedral molecular sieves (OMS-2) were synthesized by the reflux method in an acid medium. The structure of the catalysts was characterized by X-ray diffraction, N2 adsorption, transmission electron microscopy, and temperature-programmed desorption (TPD). The effect of the promoter Ag was deduced. The results showed that the catalysts have the typical cryptomelane structure with a one-dimensional channel. The doping with Ag resulted in Ag/OMS-2 catalysts with a higher specific surface area and narrower pore size distribution than OMS-2. The catalysts showed excellent catalytic activity for CO oxidation and the catalytic activity was increased after Ag introduction. O2-TPD and CO-TPD results showed that this was because the doping with Ag increased the rate of CO adsorption and the diffusion of lattice oxygen ions.

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Asymmetric Epoxidation of Styrene in Chiral Microreactor of Cyclodextrin XIAO Zisheng;LAN Zhili*;YIN Dulin;LIU Fang;LI Chuanhua 2007, 28 (5):  469-473.  Abstract ( 2185 )   [Full Text(HTML)] () PDF (308KB) ( 1174 )   The asymmetric epoxidation of styrene included by cyclodextrins with dioxirane produced in situ from ketones and potassium peroxymonosulfate (Oxone) was achieved. The effects of different cyclodextrins and ketones on the epoxidation of styrene were investigated, and the possible mechanism for the synergistic catalysis of cyclodextrins and ketones was suggested. The results indicated that β-cyclodextrin had good ability of chiral recognition to dioxirane that was generated in situ from methyl isobutyl ketone (MIBK) and Oxone. Various factors, such as molar ratio of MIBK to cyclodextrin inclusion complex, NaHCO3 amount, reaction time, and reaction temperature, that affected the enantiometric excess of the reaction products were examined, and the maximum enantiometric excess of1,2-epoxyethylbenzene was up to 46% under the optimal reaction conditions.

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Selective Oxidation of Cyclohexene to 2-Cyclohexene-1-one Catalyzed by V2O5 in Room-Temperature Ionic Liquids TAO Liang;YU Ningya*;LI Biaomo;TAN Rong;YIN Donghong* 2007, 28 (5):  474-478.  Abstract ( 2225 )   [Full Text(HTML)] () PDF (242KB) ( 966 )   2-Cyclohexene-1-one was synthesized via the oxidation of cyclohexene using V2O5 as the catalyst and H2O2 as the oxidant in room-temperature ionic liquids (RTILs). Compared with the reaction performed in the organic solvent of acetone, higher conversion of cyclohexene and selectivity for 2-cyclohexene-1-one were obtained in the solvent of [bmim]BF4-acetone. The effects of various RTILs, reaction temperature, and the amount of V2O5 and H2O2 on the oxidation were investigated. A conversion of 88.7% with the selectivity for 2-cyclohexene-1-one of 91.1% was obtained when the reaction was carried out in the neutral solvent of [bmim]BF4-acetone ([bmim]BF4/acetone volume ratio of 2/5) with 2% of V2O5/cyclohexene molar ratio and 110 mmol of H2O2 at 313 K for 10 h. Furthermore, the ionic liquids could be conveniently recovered for recycle use. The conversion of cyclohexene and the selectivity for 2-cyclohexene-1-one decreased slightly with the increase in the reuse times.

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Effect of Straight Chain Alkanes on the Synthesis ofTi-HMS Molecular Sieve SUN Dewei;LI Gang*;JIN Changzi;ZHAO Lixia;WANG Xiangsheng 2007, 28 (5):  479-483.  Abstract ( 2119 )   [Full Text(HTML)] () PDF (319KB) ( 995 )   Ti-HMS was synthesized at ambient temperature using dodecylamine as the template, tetraethylorthosilicate as the silicon source, tetrabutylorthotitanate as the titanium source, and incorporating straight chain alkanes as swelling agents. Effects of the dosage and the number of carbon atoms of the alkanes on the structural and catalytic properties of the Ti-HMS were investigated. The molecular sieve was characterized by X-ray diffraction (XRD), N2 physical adsorption, diffuse reflectance ultraviolet-visible (UV-Vis) spectroscopy, and transmission electron microscopy (TEM). The catalytic performance of Ti-HMS was evaluated by the oxidative removal of4,6-dimethyl dibenzothiophene (4,6-DMDBT). The Ti-HMS samples obtained possess wormlike mesostructure, which was confirmed by XRD and TEM analysis. The Ti-HMS prepared with the addition of alkanes has lower crystallinity and framework titanium content than the original sample. The physical adsorption results exhibit that the pore diameter of Ti-HMS, as well as the surface area and pore volume, was enlarged with the addition of alkanes. In addition, the pore diameter of Ti-HMS increased with the increase in the dosage of alkanes and the number of carbon atoms in alkane molecules. The samples thus obtained have preferable activity than the original Ti-HMS for the oxidative removal of4,6-DMDBT, which can be attributed to the improvement of their diffusion performance arising from the larger pore diameter.

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Catalytic Performance of Ru Catalyst Supported on Ba-Doped Nano-Magnesia Prepared by Ultrasonic Method for Ammonia Synthesis HUO Chao*;YAN Gang;ZHENG Yifan;YU Fengwen;LIU Huazhang 2007, 28 (5):  484-488.  Abstract ( 2366 )   [Full Text(HTML)] () PDF (404KB) ( 880 )   Ba-doped nano-magnesia (Ba-MgO) was prepared by the chemical co-precipitation method using ultrasonic technique, and a Ru catalyst was prepared using this Ba-doped nano-magnesia as the support andRu3(CO)12as the Ru precursor by impregnation. The catalyst was characterized by field-emission scanning electron microscopy,X-raydiffraction, and N2 physical adsorption.The Ba-doped nano-magnesia treated with ultrasonic wave has large surface area and regular porosity, and Ba was uniformly dispersed in the support. The activity of the Ru catalyst for ammonia synthesis was evaluated under the conditions of10000h-1, 10.0 MPa, and400-450℃. With the promotion of Ba, the Ru catalyst supported on Ba-MgO showed high activity. When the nano-magnesia was treated with ultrasonic wave for 30 min, the reaction rate of ammonia synthesis over4%Ru/Ba-MgOreached 61.02 mmol/(g•h) under the conditions of 10.0 MPa, 425 ℃, and10000h-1.