The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influen...The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influenced by the morphology of the support.Hydrothermal synthesis was employed to produce different morphologies ofγ-Al_(2)O_(3):flower-likeγ-Al_(2)O_(3)(f)exposing(110)crystal faces,sheet-likeγ-Al_(2)O_(3)(s)revealing(100)crystal faces,and rod-likeγ-Al_(2)O_(3)(r)displaying(111)crystal faces,followed by loading PtCo nanoparticles.The exposed crystal faces of the support impact the alloying degree of the PtCo nanoparticles,and an increase in the alloying degree correlates with enhanced catalyst reactivity.Pt_(3)Co intermetallic compounds were identified onγ-Al_(2)O_(3)(f)exposing(110)crystal faces,and PtCo/γ-Al_(2)O_(3)(f)showed high catalytic activity in the CO-PROX reaction,achieving 100%CO conversion across a broad temperature range of 50−225°C.In contrast,only partial alloying of PtCo was observed onγ-Al_(2)O_(3)(s).Furthermore,no alloying between Pt and Co occurred in PtCo/γ-Al_(2)O_(3)(r),resulting in a reaction rate at 50°C that was merely 11%of that of PtCo/γ-Al_(2)O_(3)(f).The formation of Pt3Co intermetallic compounds led to a more oxidized state of Pt,which significantly diminished the adsorption of CO on Pt and augmented the active oxygen species,thereby facilitating the selective oxidation of CO.展开更多
High-temperature experiments were carried out for the slag systems of“FeO”−SiO_(2)−CaO−Al_(2)O_(3)and“FeO”−SiO_(2)−CaO−MgO at 1200℃and p(O_(2))of 10^(−7)kPa.The equilibrated samples were quenched,and the phase co...High-temperature experiments were carried out for the slag systems of“FeO”−SiO_(2)−CaO−Al_(2)O_(3)and“FeO”−SiO_(2)−CaO−MgO at 1200℃and p(O_(2))of 10^(−7)kPa.The equilibrated samples were quenched,and the phase compositions were measured by electron probe microanalysis(EPMA).A series of pseudo-ternary and pseudo-binary phase diagrams are constructed to demonstrate their applications in copper smelting process and evaluation of the thermodynamic database.Spinel and tridymite are identified to be the major primary phases in the composition range related to the copper smelting slags.It is found that the operating window of the smelting slag is primarily determined by w_(Fe)/w_(SiO_(2))ratio in the slag.Both MgO and Al_(2)O_(3)in the slag reduce the operating window which requires extra fluxing agent to keep the slag to be fully liquid.Complex spinel solid solutions cause inaccurate predictions of the current thermodynamic database.展开更多
基金supported by the National Natural Science Foundation of China(22376063,21976057)the Fund of the National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2020A05)Fundamental Research Funds for the Central Universities.
文摘The preferential oxidation of CO(CO-PROX)reaction is a cost-effective method for eliminating trace amounts of CO from the fuel H2.Pt-based catalysts have been extensively studied for COPROX,with their activity influenced by the morphology of the support.Hydrothermal synthesis was employed to produce different morphologies ofγ-Al_(2)O_(3):flower-likeγ-Al_(2)O_(3)(f)exposing(110)crystal faces,sheet-likeγ-Al_(2)O_(3)(s)revealing(100)crystal faces,and rod-likeγ-Al_(2)O_(3)(r)displaying(111)crystal faces,followed by loading PtCo nanoparticles.The exposed crystal faces of the support impact the alloying degree of the PtCo nanoparticles,and an increase in the alloying degree correlates with enhanced catalyst reactivity.Pt_(3)Co intermetallic compounds were identified onγ-Al_(2)O_(3)(f)exposing(110)crystal faces,and PtCo/γ-Al_(2)O_(3)(f)showed high catalytic activity in the CO-PROX reaction,achieving 100%CO conversion across a broad temperature range of 50−225°C.In contrast,only partial alloying of PtCo was observed onγ-Al_(2)O_(3)(s).Furthermore,no alloying between Pt and Co occurred in PtCo/γ-Al_(2)O_(3)(r),resulting in a reaction rate at 50°C that was merely 11%of that of PtCo/γ-Al_(2)O_(3)(f).The formation of Pt3Co intermetallic compounds led to a more oxidized state of Pt,which significantly diminished the adsorption of CO on Pt and augmented the active oxygen species,thereby facilitating the selective oxidation of CO.
文摘High-temperature experiments were carried out for the slag systems of“FeO”−SiO_(2)−CaO−Al_(2)O_(3)and“FeO”−SiO_(2)−CaO−MgO at 1200℃and p(O_(2))of 10^(−7)kPa.The equilibrated samples were quenched,and the phase compositions were measured by electron probe microanalysis(EPMA).A series of pseudo-ternary and pseudo-binary phase diagrams are constructed to demonstrate their applications in copper smelting process and evaluation of the thermodynamic database.Spinel and tridymite are identified to be the major primary phases in the composition range related to the copper smelting slags.It is found that the operating window of the smelting slag is primarily determined by w_(Fe)/w_(SiO_(2))ratio in the slag.Both MgO and Al_(2)O_(3)in the slag reduce the operating window which requires extra fluxing agent to keep the slag to be fully liquid.Complex spinel solid solutions cause inaccurate predictions of the current thermodynamic database.
