The study explores the feasibility of producing ruthenium catalysts supported on char through a one-pot synthesis,an original approach for the preparation of noble metal-based catalysts in this field.This method combi...The study explores the feasibility of producing ruthenium catalysts supported on char through a one-pot synthesis,an original approach for the preparation of noble metal-based catalysts in this field.This method combines high-temperature stages,such as catalytic support carburization and catalyst activation,in a single step.The innovation represents a significant advancement in utilizing cellulose as a model of waste biomass,enhancing its value,and reducing catalyst production costs.The one-pot catalysts were successfully tested in the hydrogenation reaction of sugar mixtures(L-Arabinose and D-Galactose)under mild conditions,achieving full selectivities.The research also introduces for the first time in that reaction a structural sensitivity analysis of the reaction,comparing experimental results with a theoretical model.The findings reveal a direct correlation between catalytic activity and the{0001}exposed face of hcp ruthenium nanoclusters.This discovery opens new avenues for industrial-scale catalyst development,promising substantial reductions in energy and production costs,and emphasizing the economic appeal of the process.展开更多
The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and...The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.展开更多
基金support for this work was obtained from Spanish Ministerio de Ciencia e Innovación(No.MCIN/AEI(10.13039/501100011033)/FEDER Funds una manera de hacer Europa)Project PID2020-113809RB-C32 and Junta de Andalucía via Consejería de EconómTransformación ica,Industria,Conocimiento y Universidades and its PAIDI 2020 program(No.P18-RT-3405)all co-financed by FEDER funds from the European Union.
文摘The study explores the feasibility of producing ruthenium catalysts supported on char through a one-pot synthesis,an original approach for the preparation of noble metal-based catalysts in this field.This method combines high-temperature stages,such as catalytic support carburization and catalyst activation,in a single step.The innovation represents a significant advancement in utilizing cellulose as a model of waste biomass,enhancing its value,and reducing catalyst production costs.The one-pot catalysts were successfully tested in the hydrogenation reaction of sugar mixtures(L-Arabinose and D-Galactose)under mild conditions,achieving full selectivities.The research also introduces for the first time in that reaction a structural sensitivity analysis of the reaction,comparing experimental results with a theoretical model.The findings reveal a direct correlation between catalytic activity and the{0001}exposed face of hcp ruthenium nanoclusters.This discovery opens new avenues for industrial-scale catalyst development,promising substantial reductions in energy and production costs,and emphasizing the economic appeal of the process.
文摘The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.
