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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2000,Vol.16>> Issue(07)>> 601-607     doi: 10.3866/PKU.WHXB20000706         中文摘要
Study on Laser Stimulated Surface Reaction of Methanol Oxidative Coupling
Zhong Shun-He, Gao Feng, Ye Xiu-Qiang, Xiao Xiu-Fen
College of Chemical Engineering and Technology,Tianjin University,Tianjin 300072
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Solid phosphates Li3PO4,BiPO4 and Li3PO4•BiPO4 prepared by precipitation were used as the surface materials. Their surface composition, structure and reaction behavior have been investigated by the techniques of XRD,IR,TPD and laser stimulated surface reaction (LSSR).In solid phosphates, there are surfaces Lewis base sites P=O and Lewis acid sites Mn+. Two types of methanol adsorption species have been found, the molecular type consists of the adsorption of the H of C-H bond on the Lewis base site P=O and the dissociative type that of O and H of O-H bond on the Lewis acid site Mn+ and Lewis base site P=O separately. Because of the interaction of Li+ and Bi3+,the introduction of Li3PO4 into BiPO4 can promote the molecular type adsorption and reduce the dissociative type adsorption. On the selective excitation of the surface P=O bond by 1077cm-1 laser photons, the activated terminal oxygen reacts with the adsorbed H of C-H bond forming CH2OH and P-OH. The former species then transfers to the Lewis acid site Mn+ and ethanediol is produced by the coupling reaction. The surface hydroxyl P-OH reacts with each other to form H2O and the surface oxygen defect. The Lewis acid sites Mn+ on the surface of solid materials can chemisorb gaseous molecular oxygen continuously and transform it into O2-to compensate the consumed surface lattice oxygen. Under atmospheric pressure and at the tempurature of 120℃,the methanol conversion of 16% and ethanediol selectivity of 97.7% can be obtained by using 1077 cm-1 laser exciting the surface P=O bond on Li3PO4•BiPO4 for 1000 illuminating times. Increase of temperature has the effects of compensating the energy density of laser photon and enhancing the desorption of reaction products. But it also causes the formation of dimethyl ether by thermal catalytic reaction while the temperature is over 120℃.



Keywords: Laser stimulated surface reaction   Oxidative coupling   Methanol   Ethanediol   Complex phosphates  
Received: 1999-09-30 Accepted: 2000-01-04 Publication Date (Web): 2000-07-15
Corresponding Authors: Zhong Shun-He Email:


Cite this article: Zhong Shun-He, Gao Feng, Ye Xiu-Qiang, Xiao Xiu-Fen. Study on Laser Stimulated Surface Reaction of Methanol Oxidative Coupling[J]. Acta Phys. -Chim. Sin., 2000,16 (07): 601-607.    doi: 10.3866/PKU.WHXB20000706
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89. YI Jian-Hua; ZHAO Feng-Qi; XU Si-Yu; GAO Hong-Xu; HU Rong-Zu; HAO Hai-Xia; PEI Qing; GAO Yin.Nonisothermal Thermal Decomposition Reaction Kinetics of Double-base Propellant Catalyzed with Lanthanum Citrate[J]. Acta Phys. -Chim. Sin., 2007,23(09): 1316-1320
90. YANG Su-Dong; ZHANG Xiao-Gang; HUANG Jian-Shu; SUN Jing-Yu.Pd-Ni/MWCNT Electrocatalysts for Ethylene Glycol Electro-oxidation in Alkaline Medium[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1224-1228
91. DENG Hui-Ning; WANG Yu-Xin.Preparation and Properties of Proton Conducting Composite Membranes from Sulfonated Poly(phthalazinone ether keton) and Phosphotungstic Acid[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1235-1240
92. ZHENG Hai-Tao; LI Yong-Liang; LIANG Jian-Ying; SHEN Pei-Kang.Methanol Oxidation on Pd-based Electrocatalysts[J]. Acta Phys. -Chim. Sin., 2007,23(07): 993-996
93. XU Hui-Yuan; CHU Wei; CI Zhi-Min.Effect of Glow Discharge Plasma on Copper-based Catalysts for Methanol Synthesis[J]. Acta Phys. -Chim. Sin., 2007,23(07): 1042-1046
94. YAN Zong-Cheng; CHEN Li; WANG Hong-Lin.Glow Discharge Plasma Electrolysis of Methanol Solutions[J]. Acta Phys. -Chim. Sin., 2007,23(06): 835-840
95. CHEN Jian; HUANG Zheng-Ren; DONG Shao-Ming; JIANG Dong-Liang.Adsorption of Polyethylene Glycol on Silicon Carbide Measured by Thermal Gravimetric and Differential Thermal Analysis[J]. Acta Phys. -Chim. Sin., 2007,23(06): 926-928
96. LI Lan-Lan; WEI Zi-Dong; YAN Can; LUO Yi-Hui; YIN Guang-Zhi; SUN Cai-Xin.Methanol Oxidation on a Pt ElectrodeModified by Underpotential Deposition of Ru[J]. Acta Phys. -Chim. Sin., 2007,23(05): 723-727
97. ZHAO Wen-Xia; HU Man-Cheng; LI Shu-Ni; JIANG Yu-Cheng; ZHANG Xiao-Lei; HU Lei; CHEN Huai-Jun.The Solubility of Ternary SystemRbBr/CsBr-CH3OH/C2H5OH-H2O at Different Temperatures[J]. Acta Phys. -Chim. Sin., 2007,23(05): 695-700
98. WU Wei; CAO Jie-Ming; CHEN Yu; LU Tian-Hong.Preparation of High-alloying Pt-Ru/CMK-3 Catalysts in THF-H2O-EtOH Ternary Solution System[J]. Acta Phys. -Chim. Sin., 2007,23(04): 559-564
99. ZHANG Cheng-Gen;LI Wen-Zuo;HUANG Ming-Bao.Reaction of Methyl Alcohol with Thionyl Chloride in Solution[J]. Acta Phys. -Chim. Sin., 2007,23(03): 399-403
100. ZHANG Shu-Dong;ZHU Xiang-Jun;WANG Yan;KONG Xiang-He.Multiphoton Ionization Mass Spectrum of Methanol Clusters and Ab Initio Calculations[J]. Acta Phys. -Chim. Sin., 2007,23(03): 379-383
101. DENG Hui-Ning;WANG Yu-Xin .Sulfonated Poly(phthalazinones) Membranes For Direct Methanol Fuel Cell[J]. Acta Phys. -Chim. Sin., 2007,23(02): 187-191
102. HUANG Mian-Yan;CHEN Hua-Yan;GUO Jian-Zhao;WANG Zhi-Tao;XU Li;WANG Yu-Xin.Methanol Resistant Poly(Ether Sulfone)/Sulfonated Poly(Ether Ether Ketone) Blend Proton Exchange Membrane for DMFC[J]. Acta Phys. -Chim. Sin., 2007,23(01): 44-49
103. SHEN Pei-Kang;WANG Sheng-Long;HU Zhi-Yi;LI Yong-Liang;ZENG Rong;HUANG Yue-Qiang.Hydrogen Production by Alcohol Electrolysis[J]. Acta Phys. -Chim. Sin., 2007,23(01): 107-110
104. ZONG Ye;WANG Yu;LIN Chang-Jian .Preparation and Characterization of a High Loading Nano PtRu/C Catalysts in DMFC[J]. Acta Phys. -Chim. Sin., 2006,22(11): 1305-1309
105. HOU Si-Cong;LIU Ling-Tao;KOU Yuan.Li-ZnO/La2O3 Catalyst for the Oxidation Coupling of Methane at Low Temperature[J]. Acta Phys. -Chim. Sin., 2006,22(08): 1040-1042
106. ZHANG Xue-Hong;TANG Xing-Hua;CHENG Xin-Sun.Synthesis and Application of Ce-doped Mesoporous TiO2[J]. Acta Phys. -Chim. Sin., 2006,22(05): 532-537
107. CHEN Ling; WANG Xin-dong; GUO Min.The Effect of NdOx as Co-catalyst for the Electro-oxidation of Methanol on PtRu/C[J]. Acta Phys. -Chim. Sin., 2006,22(02): 141-145
108. WU Qiu-mei; RUAN Jian-ming; ZHOU Zhong-cheng; HUANG Bai-yun.Study on the Rheological Properties of Silica /Polyethylene Glycol Non-Newtonian Flow[J]. Acta Phys. -Chim. Sin., 2006,22(01): 48-52
109. CHEN Yu; TANG Ya-wen; Kong Ling-yong; LIU Chang-peng; XING Wei; LU Tianhong.Effect of Surface Modification Extent of Carbon Nanotubes on Electrocatalytic Performance of Carbon Nanotubes Supported Pt catalyst[J]. Acta Phys. -Chim. Sin., 2006,22(01): 119-123
110. WANG Zhen-bo; YIN Ge-ping; SHI Peng-fei.The Influence of Three Groups of Pt-Ru/C Catalyst’s Precursors on Its Performance for Direct Methanol Fuel Cell[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1156-1160
111. QU Wei-li; WU Bing; SUN Fang; GAO Ying; LU Tian-hong; LIU Chang-peng; XING Wei.Electrocatalytic Oxidation of Ethylene Glycol at Pt-WO3/C Electrode[J]. Acta Phys. -Chim. Sin., 2005,21(07): 804-807
112. HOU Hai-yun; AN Xue-qin; SHEN Wei-guo.Tricritical Phenomena in Quasi-ternary Solutions of Water+Formamide+Cyclohexane+Diethylene Glycol Monobutyl Ether[J]. Acta Phys. -Chim. Sin., 2005,21(07): 813-816
113. ZHANG Wen-yu; DONG Qing-nian; ZHAO Ning; WEI Wei; SUN Yu-han.The Reaction Mechanism for the Synthesis of 1-methoxy-2-propanol on MgO Catalyst[J]. Acta Phys. -Chim. Sin., 2005,21(06): 653-657
114. MA Hui-ru; GUAN Jian-guo; LU Guo-jun; YUAN Run-zhang.The Preparation and Characterization of PAn-PEG-PAn Rod-coil Triblock Copolymers[J]. Acta Phys. -Chim. Sin., 2005,21(06): 627-631
115. CHEN Yu; TANG Ya-Wen; LIU Chang-Peng; XING Wei; LU Tian-Hong.Research Progress on Proton Exchange Membranes for Direct Methanol Fuel Cell[J]. Acta Phys. -Chim. Sin., 2005,21(04): 458-462
116. JIA Yu-Xiang; GUO Xiang-Yun.Monte Carlo Simulation of Adsorption Process of CO and H2 in Supercritical Fluids[J]. Acta Phys. -Chim. Sin., 2005,21(03): 306-309
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118. Gao Cai;Wang Wen-Hua;Hu Tong-Ji;Xu Yi;Zhou Guo-Yan;Hua Ze-Zhao.Glass Transition and Enthalpy Relaxation Behavior of Ethylene Glycol and Its Aqueous Solution with Different Crystallinity[J]. Acta Phys. -Chim. Sin., 2004,20(07): 701-706
119. Hu Ji-Ming;Zhang Jian-Qing;Zhang Jin-Tao;Cao Chu-Nan.Electrochemical Activities of IrO2 Electrodes in Small Organic Molecules Containing Aqueous Solutions[J]. Acta Phys. -Chim. Sin., 2004,20(07): 740-744
120. Yun Hong;Chen Jian-Hua;Zhang Hui;Lin Jing-Dong;Chen Hong-Bo;Lin Chang-Jian.The Effects of ZrO2 on Cu-ZnO-ZrO2 Catalysts for Hydrogen Generation by Steam Reforming of Methanol[J]. Acta Phys. -Chim. Sin., 2004,20(05): 550-553
121. Yun Hong;Zhang Hui;Chen Jian-Hua;Chen Hong-Bo;Lin Chang-Jian.The Intermediate State and Mechanism of the Steam Reforming of Methanol over CuO-ZnO-ZrO2 Catalysts[J]. Acta Phys. -Chim. Sin., 2004,20(05): 524-528
122. Peng Cheng;Cheng Xuan;Zhang Ying;Chen Ling;Fan Qing-Bai.Comparison of Methanol Electrooxidation on Carbon Supported Pt and PtRu Catalysts[J]. Acta Phys. -Chim. Sin., 2004,20(04): 436-439
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124. Gao Cai;Zhou Guo-Yan;Xu Yi;Hua Ze-Zhao.Freezing Properties of EG and Glycerol Aqueous Solutions Studied by DSC[J]. Acta Phys. -Chim. Sin., 2004,20(02): 123-128
125. Zhou Hai-Hui;Jiao Shu-Qiang;Chen Jin-Hua;Wei Wan-Zhi;Kuang Ya-Fei.Electrocatalytic Oxidation of Methanol on Nano-fibular Polyaniline Electrode Modified with Pt Microparticles[J]. Acta Phys. -Chim. Sin., 2004,20(01): 9-14
126. Chen Wei;Sun Shi-Gang;Si Di;Chen Sheng-Pei.Electrocatalytic Properties of Agglomerates of Pt Nanoparticles in Methanol Oxidation[J]. Acta Phys. -Chim. Sin., 2003,19(05): 441-444
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129. Liang Huan-Zhen;Kim Dong-Jin;Chung Hun S.;Zhang Jie;Yu Ke-Ning;Li Shao-Hua;Li Rui-Xing.Mechanism for the Formation of Flake Silver Powder Synthesized by Chemical Reduction in Ethylene Glycol[J]. Acta Phys. -Chim. Sin., 2003,19(02): 150-153
130. Wang Jin;Chen Hong-Bo;Yun Hong;Lin Jing-Dong;Yi Jun;Zhang Hong-Bin;Liao Dai-Wei.Study on Rh-ZnO/MWNTs Catalyst for Methanol Synthesis[J]. Acta Phys. -Chim. Sin., 2003,19(01): 65-69
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133. Wei Zi-Dong;Miki Atsushi;Ohmori Tadayoshi;Osawa Masatoshi.Methanol Electroxidation on Upd - Sn Modified Platinum Electrodes[J]. Acta Phys. -Chim. Sin., 2002,18(12): 1120-1124
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