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氟化锶/氧化钕催化剂的甲烷氧化偶联性能及其吸附氧物种的原位FTIR光谱研究龙瑞强,万惠霖,赖华龙,蔡启瑞(厦门大学化学系固体表面物理化学国家重点实验室,厦门,361005)关键词甲烷氧化偶联,氟化锶/氧化钕,吸附氧物种近年来,甲烷氧化偶联(OCM)的... 相似文献
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直接利用甲烷氧化偶联产物中的稀乙烯制环氧乙烷刘育,徐法强,沈师孔(中国科学院兰州化学物理研究所,兰州,730000)关键词乙烯环氧化,甲烷氧化偶联,负载银催化剂1.前言甲烷氧化偶联(OCM)是一个产物较为复杂的反应,从目前研究结果来看,产物中C2烃总... 相似文献
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甲烷氧化偶联La-Me-O(Me=Mg,Ca,Sr,Ba)系催化剂表面氧种的研究 总被引:2,自引:0,他引:2
利用CO_2-TPD法考察了La-Me-O(Me=Mg,Ca,Sr,Ba)系催化剂的表面碱性,并用O_2-TPD、CH_4-TPD法对该体系的表面活性氧种进行了表征,并与催化性能相关联。结果表明,La-Ba-O催化剂由于表面强碱性中心数目多,产生活性氧种的数目也多,有利于甲烷的活化,因而具有最高的甲烷转化率和C_2烃选择性。脉冲反应表明,在无气相氧存在下,表面晶格氧参与了氧化偶联,而且是选择氧化的活性氧种。 相似文献
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甲烷氧化偶联La—Me—O(Me=Mg,Ca,Sr,Ba)系催化剂表面氧种的研究 总被引:2,自引:1,他引:2
利用CO2-TPD法考察了La-Me-O(Me=Mg,Ca,Sr,Ba)系催化剂的表面碱性,并用O2-TPD,C4-TPD法对该体系的表面活性氧种进行了表征,并与催化性能相关联,结果表明,La-Ba-O催化剂由于表面强碱性中心数目多,产生活性氧种的数目也多,有利于甲烷的活性,因而具有最高的甲烷转化率和C2烃选择性,脉冲反应表明,在无气相氧存在下,表面晶格氧参与了氧化偶联,而且是选择氧化的活性氧种。 相似文献
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微波场中甲烷部分氧化制合成气 Ⅱ.Co/ZrO_2催化剂在微波场中的升温行为及催化活性 总被引:4,自引:0,他引:4
近年来,甲烷部分氧化制合成气(POM)的研究一直十分活跃[1,2].前文报道了用于甲烷部分氧化制合成气的镍基催化剂(Ni/La2O3)在微波场中的升温行为和催化活性[3],发现在达到相同的CH4转化率时,微波活化方式下的催化剂床层温度比常规加热低得多... 相似文献
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微波辐照下(Bi_2O_3)_(0.8)(La_2O_3)_(0.2)固熔体对甲烷氧化偶联的催化行为陈长林,洪品杰,戴树珊,阚家德(云南大学化学系,昆明,650091)关键词微波,甲烷氧化偶联,(Bi_2O_3)_(0.8)(La_2O_3)_(0.2)甲烷氧化... 相似文献
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甲烷氧化偶联CaF_2/Sm_2O_3催化剂的研究周水琴,龙瑞强,黄亚萍,万惠霖,蔡启瑞(厦门大学化学系,固体表面物理化学国家重点实验室,厦门,361005)关键词甲烷氧化偶联,氟化钙,三氧化二钐,离子交换,氧物种甲烷氧化偶联制乙烯是催化领域中最活跃的?.. 相似文献
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Screening of MgO——and Ce02-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C2+ Hydrocarbons 下载免费PDF全文
The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM)have been investigated over ternary and binary metal oxide catalysts.The catalysts are prepared by doping MgO-and CeO2-based solids with oxides from alkali(Li2O),alkaline earth (CaO),and transition metal groups (WO3 or MnO).The presence of the peroxide (O2^2-)active sites on the Li2O2,revealed by Raman spectroscopy,may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts.The high reducibility of the CeO2 catalyst,an important factor in the CO2-OCM catalyst activity,may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobitity and oxygen vacancies in the CeO2 catalyst.raman and Fourier Transform Infra Red (FT-IR)spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks carresponding to the buld crystalline structures of Li2O,CaO,WO2 and MnO are detected.The performance of 5%MnO/15?O/CeO2 catalyst is the most potential among the CeO2-based catalysts,although lower than the 2%Li2O/MgO catalyst.The 2%Li2O/MgO catalyst showed the most promising C2 hydrocarbons selectivity and yield at 98.0%and 5.7%,respectively. 相似文献
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Screening of MgO- and CeO_2-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C_(2+) Hydrocarbons 总被引:1,自引:0,他引:1
The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may 相似文献
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V. R. Choudhary V. H. Rane S. T. Chaudhari 《Reaction Kinetics and Catalysis Letters》1998,63(2):371-377
Pulse reaction of methane in the presence and absence of free (or gaseous) oxygen and that of ethane and ethylene in the absence
of free oxygen over Li−MgO, La−MgO and Sm−MgO (Li or La or Sm/Mg ratio=0.1) have been investigated for elucidating the role
of lattice and free oxygen in oxidative coupling of methane (OCM) over these catalysts. No significant role is played by the
lattice oxygen from these catalysts in the OCM process. The presence of free oxygen is essential for all these catalysts to
be active and selective in OCM process. However, lattice oxygen plays some role in ethane conversion but a very significant
role in ethylene conversion over these catalysts. 相似文献
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利用Li+/MgO催化剂上乙烷氧化脱氢制乙烯及IR、TPD等测试手段对外[Li+O-]中心的形成机理及其性质进行了研究,表明[Li+O-]中心最初生成与MgO表面的自由羟基相关,气相氧、反应温度配位数等对生成[Li+O-]有一定程度的影响. 相似文献
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XU Yi-De** HUANG Bu-WenWEI Xin-Yun HUANG Jia-ShengState Key Laloratory of CatalysisDalian Institute of Chemical Physics Academia SmicaDalian Ijiaoning 《天然气化学杂志》1995,(2)
A comparative study of the role of lattice and gaseous oxygen in theoxidative coupling of methane over Na~ /Cao and Ca_xSr_(1-x)TiO_3 perovskiteoxide catalysts was performed by using a pulse reaction technique with CH_4,O_2 and mixtures of CH_4and O_2.It was found that there is an oxygen species onthe Surface of Cao which is active only for the total oxidation of methane at thereaction temperature.These oxygen species.once reacted with methane andconsumed,can be regenerated by the adsorption of oxygen molecules from thegas phase or by the migration of the lattice oxysen from the bulk onto thesurface.In contrast,no such oxygen species and no reaction can be detected bymethane pulsed over Ca_xSr_(1-x)TiO_3perovskite oxide catalysts.Na~ can heavilysuppress the non-selective oxygen species on the surface,and When 5mol%Na~ was incorporated onto the surface of Cao,the sample showed no reactivityto methane.When oxygen exists in the gas phase,or the pulse containsmethane and oxygen,the reaction over(Cao is mai 相似文献
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Partial Oxidation of Methane to Syngas Using Lattice Oxygen of La1-xSrxFeO3 总被引:1,自引:0,他引:1 下载免费PDF全文
Catalytic partial oxidation of methane to syngas using the lattice oxygen of La1-xSrxFeO3 perovskite oxide catalysts in place of molecular oxygen was studied. La1-xSrxFeO3 (x=0, 0.1, 0.2,0.5) perovskite oxides were prepared by the "auto-combustion method". XRD analysis showed that all La1-xSrxFeO3 samples have a single-phase perovskite-type oxide. The redox properties of the catalysts were investigated by temperature programmed reduction with hydrogen (H2-TPR). Reducibility of the catalysts increase with the increasing of the Sr2+ content. The oxygen species of the catalysts and their reaction with CH4 were studied by the temperature programmed surface reaction (CH4-TPSR). In the absence of gas phase oxygen, there exist two kinds of oxygen species on the catalysts. One kind of the oxygen species with strong oxidative ability is produced first, which can oxidize CH4 completely to CO2 and H2O.Then, the second oxygen species with weak oxidative ability is formed, which can oxidize CH4 partially to CO and H2 with high selectivity. The number of the oxygen species with strong oxidative ability in the CH4-TPSR tends to become zero at low x values (x≤0.1). Under suitable reaction conditions, switching alternatively the reactions of 11% O2-Ar and 11% CH4-He over a La0.sSr0.2FeO3 catalyst at 900 ℃ allows methane to be selectively converted to synthesis gas (CH4 conversion ~90%, CO selectivity >93%) using the lattice oxygen of the perovskite oxide catalyst in a redox mode. 相似文献
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用原位FT-IR研究了甲烷和氧与纯CaO,La_2O_3和SrO氧化物以及LC和SLC催化剂的相互作用和反应.当不存在气相氧时,引入的甲烷与表面晶格氧反应生成碳酸盐物种。在室温或高温下,在这些氧化物和催化剂上不能检测到CH_4或O_2的吸附物类。但是,当CH_4和O_2同时存在时,在La_2O_3和LC催化剂上能检测到1118cm~-1的新谱带、这一谱带可能来自于表面碳酸盐在高温下氧气氛中的分解,并可归属为物种。甲烷与这一活性氧物种反应生成C_2H_4。但对SLC催化剂,在高温下不能检测到物种,而甲烷和氧在高温下反应也能产生表面碳酸盐并在气相中形成乙烯,这就表明,气相氧对这些催化剂也起着关键作用,但是在LC和SLC催化剂上甲烷氧化偶联反应可能有本质上的差别。 相似文献
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YUAN Song-Yue ZHAO Zhen Changchun institute of Applied Chemistry Academia Sinica Changchun. Jilin YU Zuo-LongChengdu Institute of Organic Chemistry Academia Sinica Chengdu Sichuan 《天然气化学杂志》1995,(4)
The correlations of the calcination temperature.structure and catalvtic activity of the LiLa_(0.5)Ti_(0.5)O_(2-(?)) catalvsts with main phase and major active phase of perovskite-type trmary complex oxide LaTi_(l-y)Li_yO_(3-λ)m the Oxidative coupling of methane(OCM)have been studied The surface and bulk structures of the catalysts were characterized by means of XRD,XPS. IR.BFT and so on. The results clearly indicated that the effect of calcination temperature on the activity for the oxidative coupling of methaneis twofold On one hand.high calcination temperature is favoragble for Lisubstitution for Ti~(3 )into the lattice of LaTiO_3 and the production of moreoxygen vacancies at which active oxygen species are formed However,excessivelv high calcmation temperature makes Li~ substitution for Ti~(3 )less due to a httle change of structure or phases of the catalvst On the otherhand,the conversion of CH_4 drops because of the decrease of surface area,when the calcination temperature is raised. 相似文献