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METHANE OXIDATIVE COUPLING: SYNERGISTIC PROMOTION OF BINARY METAL FLUORIDES TO THORIA BASED CATALYST ThO2/LaF3/BaF2

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Journal of Energy Chemistry 1996年第1期 31-44页

作者： ZHOU Xiao-Ping CHAO Zi-Sheng WAN Hui-Lin tsai khi-rui (Department of Chemistry, Xiamen University Xiamen, Fujian 361005 To whom correspondence should be addressed)

Methane oxidative coupling was investigated on ThO2/LaF3,ThO2/BaF2 and ThO2/LaF3/BaF2 catalysts. A synergistic promoting effect of binary metal fluorides BaF2 and LaF3 to metal oxide ThO2 was found over ThO2/LaF3/BaF2 catalyst. The analysis of phase composition shows that there are abundant. lattice defect in ThO2/LaF3/BaF2 catalyst. XPS and Raman charactenzation indicate that there exist O22-, O2 and the intermediate oxygen species, and a large amount of quasi-free electrons over ThO2f/LaF3/BaF2 catalyst.

关键词： methane oxidative coupling binary metal fluorides synergistic promotion. thoria based catalyst oxygen species

THE ADSORPTION OF OXYGEN OVER ThO2-BaF2 CATALYST

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Journal of Energy Chemistry 1996年第1期 22-30页

作者： ZHOU Xiao-Ping CHAO Zi-Sheng WAN Hui-Lin tsai khi-rui(Department of Chemistry, Xiamen University Xiamen, Fujian 361005 To whom correspondence should be addressed)

The adsorption of O2 over ThO2-BaF2 catalyst was studied at room temperature. Raman experiments reveal that there is much stronger adsorption of O2 on ThO2-BaF2 than on ThO2 XRD results suggest that ionic exchange exists between BaF2 and ThO2 phases forming the O-species and quasi-free electrons in ThO2-BaF2. The XPS, Raman and EPR results indicate that O22-, O2- and intermediate oxygen species O2n- and O2δ- (1更多还原AbstractFilter('ChDivSummary', 'ChDivSummaryMore', 'ChDivSummaryReset');

关键词： oxygen species metal fluoride ThO2-BaF2

CHARACTERISTIC STUDIES OF MoSx/K+-SiO2 CATALYSTS FOR SYNTHESIS OF MIXED ALCOHOLS FROM SYNGAS

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Journal of Energy Chemistry 1992年第1期 1-10页

作者： ZHANG,Hong-Bin HUANG,Hao-Ping LIN,Guo-Dong tsai,khi-rui Department of Chemistry and Institute of Physical Chemistry Xiamen University,Xiamen,Fujian 361005 Received February 28,1991

Characteristic studies,by means of XRD,XPS and TPD,of MoS/K-SiOcatalysts for thesynthesis of mixed alcohols provided experimental evidence for the formation of Mo-S-K surface phaseand the presence of disulfide species,（S-S）,at the surface of *** of the origins of thepromoter action in shifting the selectivity from hydrocarbons to alcohols is likely that the addition ofalkali salt led to a decrease in concentration of（S-S）at the surface,which in turn would reduce thegeneration of the reactive hydrogen.

关键词： SiO2 CATALYSTS FOR SYNTHESIS OF MIXED ALCOHOLS FROM SYNGAS CO CHARACTERISTIC STUDIES OF MoS_x/K

Studies of Catalysis in Partial Oxidation of Methane to Syngas（Ⅱ）──Chemisorbed Species，Energetics and Mechanism

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Chemical Research in Chinese Universities 1995年第4期11卷 323-335页

作者： CHEN Ping ZHANG Hong-bin LIN Guo-dong andtsai khi-rui(Department of Chemistry &State Key Laboratory for Physical Chemistyry of the Solid Surface ,Xiamen University ,Xiamen 361005) XIAMEN UNIV DEPT CHEMXIAMEN 361005PEOPLES R CHINA XIAMEN UNIV STATE KEY LAB PHYS CHEM SOLID SURFACEXIAMEN 361005PEOPLES R CHINA

he characteristic study,by means of in-situ IR spectroscopy, of chemisorbed species on the Ni-catalysts for the partial oxidation of methane(POM)to syngas demonstrated the existence of CH_x(a)and H_xCO(a)adspecies on the functioning Ni-catalysts, Several designed experimental investigations on the reactivities of methane with CO_2 and with O_2,respectively,over the Ni-catalysts, and of CO_2 with the prereduced Ni-catalyst,ats well as of the deposited carbon with CO_2 and with O_2,respectlvely,liave been carried out and the reLqults were unfavorable to the two-step mechanistic interpretation proposed for the POM reaction. By means of tlie BOC-MP Approach,energetics of a set of elementary reactions,which may be involved in the POM process,on the clean(111)surface of Ni,Fe,Cu and Pd, re- spectively,has been *** result;of the experiments and the calculation of the present work favor the direct catalytic dissociation-plus-surface oxidation-plus-further debdrogenation mechanism as the dominant pathway making major contribution to the POM reaction.

关键词： Partial oxidation of methane Syngas Chemisorbed species Energetics. Mechanism

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Coke-Resistant　Ni-based　Catayst　for　Partial　Oxidation　and　CO_2-Reforming　of　Methane　to　Syngas

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Chemical Research in Chinese Universities 1997年第1期13卷 85-87页

作者： CHEN Ping, ZHANG Hong bin, LIN Guo dong, GUO Zhong ping, tsai khi rui (Department of Chemistry & State Key Laboratory for Physical Chemistry of the Solid Surface, Xiamen University, Xiamen, 361005)

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关键词： Coke resistant Ni catalyst Methane Partial oxidation CO 2 reforming Syngas

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ACTIVATION OF O2 AND CATALYTIC PROPERTIES OF CeO2/CaF2 CATALYSTS FOR METHANE OXIDATIVE COUPLING

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Journal of Energy Chemistry 1993年第4期 280-289页

作者： ZHOU Xiao-Ping WANG Shui-Ju WENG Wei-Zheng WAN Hui-Lin tsai khi-rui Department of Chemistry and State Key Laboratory for Physical Chemistry of the Solid Surface Xiamen University, Xiamen, Fujian 361005

The investigation of the catalytic properties of the CaF2modifiedCeO2catalysts for the methane oxidative coupling （MOC） to prepare C2hydro-carbons indicated that most of the CaF2modified CeO2catalysts were efficientfor the MOC reaction. Addition of CaF2to CeO2can make the C2selectivity in-crease from 2. 2％（over CeO2） to 46-63％, and the CH4conversion increasefrom 26％ to 28-30％. When the CeO2content was decreased within a defi-nite region, the activity and C2selectivity of the catalysts increased remark-ably. The XRD characterization revealed that F-—O2-exchange happened be-tween CaF2and CeO2phases. TPD, XPS, Raman and ESR experiments indicat-ed that O-, O22-and O2-species were formed over CeO2/CaF2catalysts. Withthe increase of CaF2content in the catalysts, the kinds and the surface concen-trations of the above mentioned oxygen species decreased, while the C2selectivi-ty increased.

关键词： ACTIVATION OF O2 AND CATALYTIC PROPERTIES OF CeO2/CaF2 CATALYSTS FOR METHANE OXIDATIVE COUPLING DMC over DMA

METHANE OXIDATIVE COUPLING OVERALKALINE-EARTH FLUORO-OXIDE CATALYSTS

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Journal of Energy Chemistry 1993年第4期 344-347页

作者： ZHOU Xiao-Ping ZHANG Wei-De WANG Shui-Ju WAN Hui-Lin tsai khi-rui Department of Chemistry and State Key Laboratory for Physical Chemistry of the Solid Surface Xianen University Xiamen, Fujian 361005

The investigation of methane oxidative coupling （MOC） reactionover a series of alkaline-earth fluoro-oxides model catalysts indicated that theCH4conversion and C2selectivity over fluoro-oxide catalysts are apparentlyhigher than those over pure oxide or pure fluoride catalysts. The XRD charac-terization of fluoro-oxide model catalysts indicated that F-, O2-exchangemight happen.

关键词： Wang over CaO METHANE OXIDATIVE COUPLING OVERALKALINE-EARTH FLUORO-OXIDE CATALYSTS XRD

METHANE OXIDATIVE COUPLING ON ThO2/CaF2CATALYST

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Journal of Energy Chemistry 1995年第2期 202-211页

作者： CHAOZi-Sheng* ZHOU Xiao- PingWAN Hui-Lin tsai khi-ruiDepartment of Clie-mudry, Xiamen University Xiamen, Fujian 36 1 005

The oxidative coupling of methane（OCM）over ThO/CaFcatalystwas *** catalyst was found to be active and selective for *** 1153 K,the Cyield was 19.9% with 61.7% Cselectivityand 32.1% *** results indicated that F（?）Oexchangehappened between ThOand *** and Raman results suggestedthat the active oxygen species were generated and suitable for OCM reactionover the catalyst.

关键词： methane oxidative coupling catalyst ThO2/CaF2

HYDROFORMYLATION OF PROPYLENE AND ETHYLEN'E CATALYZED BY WATER-SOLUBLERu3（CO）9（TPPMS）3 CATALYST

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Journal of Energy Chemistry 1997年第4期 284-287+289-291页

作者： GAO Jing-Xing XU Pian-Pian ZHENG Rong-Hui HUANG Pei-Qiang WAN Hui-Lin tsai khi-rui(Department of Chemistry Institute of Physical ChemistryState Key Laboratory of Physical Chemistry of Solid Surface Xiamen UniversityXiamen, Fujian 361005)

Water-soluble and air-stable triruthenium carbonyl clusterRu3(CO)9(TPPMS)3 (TPPMS=sodium diphenylphosphinobenzene-msulphonate) was used as catalyst to hydroformylate Propylene with syngas inWater. The main product is n-butyraldehyde, side-products are isobumpdehyde and a small amount of 1-butyl and isobutyl alcohols. At120℃ and propylene, CO and H2 pnal Pressures of 0.7 MPa, 2.0 MPa and2.0 MPa respectively, catalytic turnover of 61.2 ***-1.h-1 (products/cluster) and product n/i ratio of 15.9 were obtained. For ethylenehydroformylation, the main product is propanal, side-Products are3-pentanone, 1-Propanol and 2-methyl-pent-2-en-1-al. The catalyst Wascharacterized before and after the reaction by IR and X-ray photoelectronspectroscopy and the results were dianssed as related to the possiblecatalytic active species.

关键词： hydroformylation propylene ethylene water-soluble catalyst