Silicoaluminophosphate(SAPO)molecular sieves possess diverse architectures and exceptional high-temperature hydrothermal stability,rendering them important acid catalysts.However,enhancing acid concentration of certai...Silicoaluminophosphate(SAPO)molecular sieves possess diverse architectures and exceptional high-temperature hydrothermal stability,rendering them important acid catalysts.However,enhancing acid concentration of certain SAPO materials remains challenging,which limits their catalytic applications.Here,we report the synthesis of a series of SAPO materials using a developed SAPO precursor plus dual template(SPDT)strategy.A variety of SAPO materials characterized by high silica content and enhanced acidity,such as SAPO-34/56 intergrowths,SAPO-56,and SAPO-17,have been synthesized and thoroughly characterized using various techniques including integrated differential phase-contrast scanning transmission electron microscopy,two-dimensional solid-state nuclear magnetic resonance spectroscopy,and continuous rotation electron diffraction.The use of silica-enriched SAPO precursor combined with the flexible selection of the second template enables the crystalline phase regulation and improves the Si atoms incorporation into the framework.Notably,the synthesized SAPO-17 with abundant Si(4Al)species and unprecedentedly high acid density exhibits exceptional DeNO_(x)activity after Cu loading,with NO_(x)conversion exceeding 90%at 175–700℃.This outstanding performance can be attributed to the unique ERI structure and the increased acidity of SAPO-17.This work not only presents an effective method for synthesizing SAPO molecular sieves with enhanced acidity but also offers a new perspective for expanding the active temperature range of the ammonia selective catalytic reduction reaction.展开更多
文摘Silicoaluminophosphate(SAPO)molecular sieves possess diverse architectures and exceptional high-temperature hydrothermal stability,rendering them important acid catalysts.However,enhancing acid concentration of certain SAPO materials remains challenging,which limits their catalytic applications.Here,we report the synthesis of a series of SAPO materials using a developed SAPO precursor plus dual template(SPDT)strategy.A variety of SAPO materials characterized by high silica content and enhanced acidity,such as SAPO-34/56 intergrowths,SAPO-56,and SAPO-17,have been synthesized and thoroughly characterized using various techniques including integrated differential phase-contrast scanning transmission electron microscopy,two-dimensional solid-state nuclear magnetic resonance spectroscopy,and continuous rotation electron diffraction.The use of silica-enriched SAPO precursor combined with the flexible selection of the second template enables the crystalline phase regulation and improves the Si atoms incorporation into the framework.Notably,the synthesized SAPO-17 with abundant Si(4Al)species and unprecedentedly high acid density exhibits exceptional DeNO_(x)activity after Cu loading,with NO_(x)conversion exceeding 90%at 175–700℃.This outstanding performance can be attributed to the unique ERI structure and the increased acidity of SAPO-17.This work not only presents an effective method for synthesizing SAPO molecular sieves with enhanced acidity but also offers a new perspective for expanding the active temperature range of the ammonia selective catalytic reduction reaction.
