Design and preparation of highly active hydrodesulfurization (HDS) catalysts is very important for the removal of air pollution. Herein, we report an extraordinarily active HDS catalyst, which is synthesized by loading of Pd on mesoporous zeolite Y (Pd/HY-M). The mesoporous zeolite Y is successfully synthesized using a water glass containing N,N-dimethyl-N-octadecyl-N-(3-triethoxysilylpropyl) ammonium [(C(2)H(5)O)(3)SiC(3)H(6)N(CH(3))(2)C(18)H(37)](+) cation as a mesoscale template. Compared with mesoporous Beta and ZSM-5 supported Pd catalysts (80.0% and 73.4% for Pd/HBeta-M and Pd/HZSM-5-M, respectively) as well as commercial catalyst of γ-Al(2)O(3) supported Pd catalyst (31.4%), Pd/HY-M catalyst exhibited very high activity in HDS of 4,6-dimethyldibenzothiophene (4,6-DM-DBT, 97.3%). The higher activity of Pd/HY-M than that of Pd/HBeta-M and Pd/HZSM-5-M is assigned to the larger micropore size of zeolite Y compared to that of Beta and ZSM-5. Theoretical simulation and adsorption experimental data show that 4,6-DM-DBT has difficulty entering the micropores of ZSM-5 and Beta zeolites, but the micropores of Y zeolite are accessible.
Developing highly active hydrodesulfurization (HDS) catalysts is of great importance for producing ultraclean fuel. Herein we report on crystalline mordenite nanofibers (NB-MOR) with a bundle structure containing parallel mesopore channels. After the introduction of cobalt and molybdenum (CoMo) species into the mesopores and micropores of NB-MOR, the NB-MOR-supported CoMo catalyst (CoMo/NB-MOR) exhibited an unprecedented high activity (99.1%) as well as very good catalyst life in the HDS of 4,6-dimethyldibenzothiophene compared with a conventional γ-alumina-supported CoMo catalyst (61.5%). The spillover hydrogen formed in the micropores migrates onto nearby active CoMo sites in the mesopores, which could be responsible for the great enhancement of the HDS activity.
Mixed NiO/NiCoO nanocrystals grown in situ from the skeleton of a 3D porous nickel network (3DPNN) were prepared with a simple hydrothermal method followed by a low temperature calcination, exhibiting outstanding electrocatalytic efficiencies toward oxygen evolution reactions (OER). The 3DPNN was prepared with a novel leaven dough method and served as both the nickel source for growth of the mixed NiO/NiCoO nanocrystals and the charge transport highway to accelerate the sluggish kinetics of the OER. The mixed NiO/NiCoO nanocrystals exhibited pronounced synergistic effects to achieve a high mass activity of 200 A g at the catalyst mass loading of 0.5 mg cm, largely outperforming the corresponding single component nanocrystal systems, NiO (5.87) and NiCoO (9.35). The NiO/NiCoO@3DPNN composite electrocatalyst achieved a low overpotential of 264 mV at the current density of 10 mA cm and 389 mV at the practically high current density of 250 mA cm, which compete favorably among the top tier of previously reported OER electrocatalysts. Moreover, it exhibited good stability even at the high current density of 250 mA cm, showing only 9.40% increase in working applied potential after a continuous 12 h operation. The present work demonstrates a new design for highly efficient OER catalysts with in situ growth of mixed oxide nanocrystals of pronounced synergistic effects.
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