Precipitation and impregnation procedures unevenly distribute metals on zeolite,limiting chemical transformation in Lewis-acid,Brönsted-acid and metal-catalyzed tandem reactions.Although,heterogeneous multitask t...Precipitation and impregnation procedures unevenly distribute metals on zeolite,limiting chemical transformation in Lewis-acid,Brönsted-acid and metal-catalyzed tandem reactions.Although,heterogeneous multitask transition metals oxides@zeolites are promising catalysts for sustainable processes;nevertheless,synthesis is fascinating and complex.Herein,the construction of purposely designed multitask materials segregated in selective shells reveals the remarkable spatial organization of metals-zeolite,resulting in them being suitable for a wide range of tandem reactions.The synthesis of multi-site catalysts begins with a universal wet chemistry approach that yields nickel oxide(NiO)crystals.Then,the NiO crystals are stabilized using cationic dodecyltrimethylammonium bromide,followed by achieving cross-linking carbon growth by emulsion polymerization of glucose in hydrothermal treatment to yield uniformed NiO@carbon spheres(NiO@CSs).Next,sequential adsorption of cobalt cations and colloidal ZSM-5(1%in H_(2)O,mass fraction),followed by calcination in air,yielded NiO@cobalt oxide@zeolite denoted as NiO@Co_(3)O_(4)@ZEO hollow spheres.The hollowing mechanism and materials segregation within shells are revealed by scanning and transmission electron microscopy,thermogravimetric analysis,and X-ray diffraction.The finding advances the rational synthesis of heterogenous core-shell hollow structures for various gas phase catalytic tandem reactions to yield valuable chemicals.展开更多
文摘Precipitation and impregnation procedures unevenly distribute metals on zeolite,limiting chemical transformation in Lewis-acid,Brönsted-acid and metal-catalyzed tandem reactions.Although,heterogeneous multitask transition metals oxides@zeolites are promising catalysts for sustainable processes;nevertheless,synthesis is fascinating and complex.Herein,the construction of purposely designed multitask materials segregated in selective shells reveals the remarkable spatial organization of metals-zeolite,resulting in them being suitable for a wide range of tandem reactions.The synthesis of multi-site catalysts begins with a universal wet chemistry approach that yields nickel oxide(NiO)crystals.Then,the NiO crystals are stabilized using cationic dodecyltrimethylammonium bromide,followed by achieving cross-linking carbon growth by emulsion polymerization of glucose in hydrothermal treatment to yield uniformed NiO@carbon spheres(NiO@CSs).Next,sequential adsorption of cobalt cations and colloidal ZSM-5(1%in H_(2)O,mass fraction),followed by calcination in air,yielded NiO@cobalt oxide@zeolite denoted as NiO@Co_(3)O_(4)@ZEO hollow spheres.The hollowing mechanism and materials segregation within shells are revealed by scanning and transmission electron microscopy,thermogravimetric analysis,and X-ray diffraction.The finding advances the rational synthesis of heterogenous core-shell hollow structures for various gas phase catalytic tandem reactions to yield valuable chemicals.