As the photo-dissociation product of methanol on the TIO2（110） surface, the diffusion and desorption processes of formaldehyde （HCHO） were investigated by using scanning tunneling microscope （STM） and density fu...As the photo-dissociation product of methanol on the TIO2（110） surface, the diffusion and desorption processes of formaldehyde （HCHO） were investigated by using scanning tunneling microscope （STM） and density functional theory （DFT）. The molecular-level images revealed the HCHO molecules could diffuse and desorb on the surface at 80 K under UV laser irra- diation. The diffusion was found to be mediated by hydrogen adatoms nearby, which were produced from photodissociation of methanol. Diffusion of HCHO was significantly decreased when there was only one H alatom near the HCHO molecule. Furthermore, single HCHO molecule adsorbed on the bare Ti02（l10） surface was quite stable, little photo-desorption was observed during laser irradiation. The mechanism of hydroxyl groups assisted diffusion of formaldehyde was also investigated using theoretical calculations.展开更多
CoCu/TiO_2 catalysts promoted using alkali metals（Li, Na, K, Rb, and Cs） were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the ...CoCu/TiO_2 catalysts promoted using alkali metals（Li, Na, K, Rb, and Cs） were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the alkali metals on the physicochemical properties of the CoCu/TiO_2 catalysts and the catalytic performance for CO_2 hydrogenation to long-chain hydrocarbons（C_（5＋））were investigated in this work. According to the characterization of the catalysts based on X-ray photoelectron spectroscopy, X-ray diffraction, CO_2 temperature-programmed desorption（TPD）, and H_2-TPD, the introduction of alkali metals could increase the CO_2 adsorption and decrease the H_2 chemisorption, which could suppress the formation of CH_4, enhance the production of C_（5＋）, and decrease the hydrogenation activity. Among all the promoters, the Na-modified CoCu/TiO_2 catalyst provided the maximum C_（5＋） yield of 5.4%, with a CO_2 conversion of 18.4% and C_（5＋） selectivity of42.1%, because it showed the strongest basicity and a slight decrease in the amount of H_2 desorption;it also exhibited excellent catalytic stability of more than 200 h.展开更多
基金the National Key R&D Program of China(2021YFA0715500)the National Natural Science Foundation of China(NSFC)(12227901)+1 种基金the Shanghai Municipal Science and Technology Major Project(2019SHZDZX01)the Chinese Academy of Sciences President’s International Fellowship Initiative(2021PT0007)。
文摘As the photo-dissociation product of methanol on the TIO2（110） surface, the diffusion and desorption processes of formaldehyde （HCHO） were investigated by using scanning tunneling microscope （STM） and density functional theory （DFT）. The molecular-level images revealed the HCHO molecules could diffuse and desorb on the surface at 80 K under UV laser irra- diation. The diffusion was found to be mediated by hydrogen adatoms nearby, which were produced from photodissociation of methanol. Diffusion of HCHO was significantly decreased when there was only one H alatom near the HCHO molecule. Furthermore, single HCHO molecule adsorbed on the bare Ti02（l10） surface was quite stable, little photo-desorption was observed during laser irradiation. The mechanism of hydroxyl groups assisted diffusion of formaldehyde was also investigated using theoretical calculations.
文摘CoCu/TiO_2 catalysts promoted using alkali metals（Li, Na, K, Rb, and Cs） were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the alkali metals on the physicochemical properties of the CoCu/TiO_2 catalysts and the catalytic performance for CO_2 hydrogenation to long-chain hydrocarbons（C_（5＋））were investigated in this work. According to the characterization of the catalysts based on X-ray photoelectron spectroscopy, X-ray diffraction, CO_2 temperature-programmed desorption（TPD）, and H_2-TPD, the introduction of alkali metals could increase the CO_2 adsorption and decrease the H_2 chemisorption, which could suppress the formation of CH_4, enhance the production of C_（5＋）, and decrease the hydrogenation activity. Among all the promoters, the Na-modified CoCu/TiO_2 catalyst provided the maximum C_（5＋） yield of 5.4%, with a CO_2 conversion of 18.4% and C_（5＋） selectivity of42.1%, because it showed the strongest basicity and a slight decrease in the amount of H_2 desorption;it also exhibited excellent catalytic stability of more than 200 h.
