Highly-open nanoframe structures consisting of interconnected and exposed ridges are highly desirable for achieving efficient catalysis,but preparing them by a facile etching-free methodology is still a very daunting ...Highly-open nanoframe structures consisting of interconnected and exposed ridges are highly desirable for achieving efficient catalysis,but preparing them by a facile etching-free methodology is still a very daunting task.Herein,we propose a novel metal-organic framework(MOF)-assisted and etching-free strategy for the construction of Co/N-doped carbon nanoframes with highly-open and precisely-controllable structures.This strategy is based on the face-selective epitaxial growth of ZIF-67 on the 36{110}facets of 72-facet ZIF-8 to form an unprecedented anisotropic ZIF-67-on-ZIF-8 heterostructure,which is subsequently pyrolyzed under Ar atmosphere to realize a solid-to-frame transformation.The highly-open nanoframe structure enables the substrates to readily penetrate into the catalyst interior and thereby create additional exposed active sites,which together with the good mass transport,high atomic utilization and increased surface area are responsible for its remarkably enhanced catalytic activity for the biomass valorisation when compared with its solid and closed hollow counterparts.This study could shed valuable insights into the design and preparation of various highly-open nanoframes with abundant exposed active species by using an etching-free strategy for efficient catalysis and beyond.展开更多
基金supported by Guangdong Natural Science Funds for Distinguished Young Scholar(2018B030306050)the National Natural Science Foundation of China(22138003,21825802)the Natural Science Foundation of Guangdong Province(2017A030312005).
文摘Highly-open nanoframe structures consisting of interconnected and exposed ridges are highly desirable for achieving efficient catalysis,but preparing them by a facile etching-free methodology is still a very daunting task.Herein,we propose a novel metal-organic framework(MOF)-assisted and etching-free strategy for the construction of Co/N-doped carbon nanoframes with highly-open and precisely-controllable structures.This strategy is based on the face-selective epitaxial growth of ZIF-67 on the 36{110}facets of 72-facet ZIF-8 to form an unprecedented anisotropic ZIF-67-on-ZIF-8 heterostructure,which is subsequently pyrolyzed under Ar atmosphere to realize a solid-to-frame transformation.The highly-open nanoframe structure enables the substrates to readily penetrate into the catalyst interior and thereby create additional exposed active sites,which together with the good mass transport,high atomic utilization and increased surface area are responsible for its remarkably enhanced catalytic activity for the biomass valorisation when compared with its solid and closed hollow counterparts.This study could shed valuable insights into the design and preparation of various highly-open nanoframes with abundant exposed active species by using an etching-free strategy for efficient catalysis and beyond.