A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition...A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition, followed by carbonization under nitrogen atmosphere. The bulk densities of carbon aerogels obtained are in the range of 0.21g/cm3~0.27g/cm3 and the sizes of the interconnected carbon nano-particles are in the range of 20nm^30nm. All of the aerogel samples exhibit high BET surface areas in the range of 730m2/g^900m2/g. The bulk density, micro-pore volume, meso-pore volume and meso-pore diameter can be controlled by gelation conditions such as R/I ratio and R/C ratio.展开更多
The metal-organic framework MO-5 has been synthesized by solvothermal method. Obtained material consists of nano-sized particle of ca. 100 nm size. The material has been physico-chemical characterized regarding struct...The metal-organic framework MO-5 has been synthesized by solvothermal method. Obtained material consists of nano-sized particle of ca. 100 nm size. The material has been physico-chemical characterized regarding structural and textural properties by XRD, FTIR, nitrogen adsorption/desorption, thermal analysis and ESA experiments. Palladium supported MOF-5 catalyst has been prepared by adsorption inclusion method. The catalyst was activated by treatment with supercritical carbon dioxide (scCO2) followed by mild reduction with hydrogen solved in scCO2. The obtained catalyst is shown to be stable and active and shape selective in hydrogenation reactions of alkenes using supercritical carbon dioxide as reaction medium. The catalytic active Pd species are located inside the pores. Positive surface charging seems to prevent deposition of active species at the crystal surface of the MOF. The catalyst is long time stable and re-useably. These findings show the potential of porous MOFs for applications under supercritical conditons and resisted repeated pressuring to 120 bar at elevated temperature.展开更多
Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an env...Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al_2O_3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al_2O_3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H_2 and NH_3 pressure were examined, and the reaction processes were discussed in detail.展开更多
基金The National Natural Science Foundation of China (No. 59973028), The Team Project of the Natural Science Foundation of Guangdong (No.[( )(20003038)]), and The Talent Training Program Foundation of the Higher Education Departmen
文摘A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition, followed by carbonization under nitrogen atmosphere. The bulk densities of carbon aerogels obtained are in the range of 0.21g/cm3~0.27g/cm3 and the sizes of the interconnected carbon nano-particles are in the range of 20nm^30nm. All of the aerogel samples exhibit high BET surface areas in the range of 730m2/g^900m2/g. The bulk density, micro-pore volume, meso-pore volume and meso-pore diameter can be controlled by gelation conditions such as R/I ratio and R/C ratio.
文摘The metal-organic framework MO-5 has been synthesized by solvothermal method. Obtained material consists of nano-sized particle of ca. 100 nm size. The material has been physico-chemical characterized regarding structural and textural properties by XRD, FTIR, nitrogen adsorption/desorption, thermal analysis and ESA experiments. Palladium supported MOF-5 catalyst has been prepared by adsorption inclusion method. The catalyst was activated by treatment with supercritical carbon dioxide (scCO2) followed by mild reduction with hydrogen solved in scCO2. The obtained catalyst is shown to be stable and active and shape selective in hydrogenation reactions of alkenes using supercritical carbon dioxide as reaction medium. The catalytic active Pd species are located inside the pores. Positive surface charging seems to prevent deposition of active species at the crystal surface of the MOF. The catalyst is long time stable and re-useably. These findings show the potential of porous MOFs for applications under supercritical conditons and resisted repeated pressuring to 120 bar at elevated temperature.
基金supported by the National Basic Research Program of China(2016YFA0602900)Youth Innovation Promotion Association CAS(2016206)Jilin Provincial Science and Technology Program of China(20150301012GX)
文摘Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al_2O_3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al_2O_3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H_2 and NH_3 pressure were examined, and the reaction processes were discussed in detail.