The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized ...The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic state.The Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the reaction.Moreover,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic system.The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.展开更多
The direct activation of methane under mild condition to achieve highly selective of oxygenates is a challenging project.In this study,a well dispersed silver supported ZnTiO_(3) catalyst was prepared to achieve selec...The direct activation of methane under mild condition to achieve highly selective of oxygenates is a challenging project.In this study,a well dispersed silver supported ZnTiO_(3) catalyst was prepared to achieve selective preparation of methanol from methane and water under mild condition.X-ray diffraction,transmission electron microscopy and X-ray photoelectron spectroscopy characterizations demonstrate that silver species are uniformly dispersed on ZnTiO_(3) surface in the form of metallic silver nanoparticles.The photoelectric characterizations reveal that the addition of silver species enhances light absorption and promotes charge separation of the catalysts.Under the reaction conditions of 50℃and 3 MPa,the methanol is obtained as the only liquid product over the designed Ag/ZnTiO_(3) catalyst under light irradiation.In this photocatalytic process,the holes generated by ZnTiO_(3) activate water to produce intermediate·OH,which further reacts with methane to synthesize methanol.The silver species as co-catalysts extend the light absorption range of ZnTiO_(3) as well as promote charge separation.展开更多
基金supported by the National Natural Science Foundation of China under grant numbers 22172032,U22A20431 and U19B2003。
文摘The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic state.The Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the reaction.Moreover,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic system.The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.
基金Project supported by the National Key Technologies R&D Program of China(2022YFE0114800)National Natural Science Foundation of China(22172032,U22A20431)。
文摘The direct activation of methane under mild condition to achieve highly selective of oxygenates is a challenging project.In this study,a well dispersed silver supported ZnTiO_(3) catalyst was prepared to achieve selective preparation of methanol from methane and water under mild condition.X-ray diffraction,transmission electron microscopy and X-ray photoelectron spectroscopy characterizations demonstrate that silver species are uniformly dispersed on ZnTiO_(3) surface in the form of metallic silver nanoparticles.The photoelectric characterizations reveal that the addition of silver species enhances light absorption and promotes charge separation of the catalysts.Under the reaction conditions of 50℃and 3 MPa,the methanol is obtained as the only liquid product over the designed Ag/ZnTiO_(3) catalyst under light irradiation.In this photocatalytic process,the holes generated by ZnTiO_(3) activate water to produce intermediate·OH,which further reacts with methane to synthesize methanol.The silver species as co-catalysts extend the light absorption range of ZnTiO_(3) as well as promote charge separation.