Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sit...Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.展开更多
Sintering inhibition of a catalyst at high temperatures is a challenge during heterogeneous catalysis. In this paper, we report that hexagonal boron nitride(h-BN) is an optimal material for anti-sintering γ-Al_(2)O_(...Sintering inhibition of a catalyst at high temperatures is a challenge during heterogeneous catalysis. In this paper, we report that hexagonal boron nitride(h-BN) is an optimal material for anti-sintering γ-Al_(2)O_(3)-supported Pt nanoparticles(NPs) originating from the high thermal conductivity of h-BN. The high thermal conductivity of h-BN ensures maximal heat dissipation from Pt NPs to γ-Al_(2)O_(3),thereby causing both Ostwald ripening and particle coalescence of Pt NPs to be decelerated at elevated temperatures.Inhibition of Pt NP sintering is also shown in the reducible TiO^(2-)supported Pt NPs with the help of h-BN. The proposed anti-sintering strategy using thermal management is universal, providing new insight into the design of anti-sintering materials and structures for a wide range of applications in heterogeneous catalysis.展开更多
基金supported by China National Natural Science Foundation(22008260,21908123)。
文摘Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.
基金supported by the National Natural Science Foundation of China (21961132026,51888103,21878331,51606192,91645108 and U1162117)the Nanotechnology Specific Project of the National Key Research and Development Program (2020YFA0210900)+1 种基金the CAS Pioneer Hundred Talents Programthe Science Foundation of China University of Petroleum,Beijing (C201604)。
文摘Sintering inhibition of a catalyst at high temperatures is a challenge during heterogeneous catalysis. In this paper, we report that hexagonal boron nitride(h-BN) is an optimal material for anti-sintering γ-Al_(2)O_(3)-supported Pt nanoparticles(NPs) originating from the high thermal conductivity of h-BN. The high thermal conductivity of h-BN ensures maximal heat dissipation from Pt NPs to γ-Al_(2)O_(3),thereby causing both Ostwald ripening and particle coalescence of Pt NPs to be decelerated at elevated temperatures.Inhibition of Pt NP sintering is also shown in the reducible TiO^(2-)supported Pt NPs with the help of h-BN. The proposed anti-sintering strategy using thermal management is universal, providing new insight into the design of anti-sintering materials and structures for a wide range of applications in heterogeneous catalysis.