Transition Metal and Metal–Nx Codoped MOF‐Derived Fenton‐Like Catalysts: A Comparative Study on Single Atoms and Nanoparticles. Issue 50 (23rd November 2020) - Gao, Yun
Abstract: To deal with the ever‐growing toxic benzene‐derived compounds in the water system, extensive efforts have been dedicated for catalytic degradation of pollutants. However, the activities and efficiencies of the transition metal‐based nanoparticles or single‐atom sites are still ambiguous in Fenton‐like reactions. Herein, to compare the Fenton‐like catalytic efficiencies of the nanoparticles and single atoms, the free‐standing nanofibrous catalyst comprising Co nanocrystals and Co–N x codoped carbon nanotubes (CNTs) or bare Co–N x doped CNTs is fabricated. It is noteworthy that all these nanofibrous catalysts exhibit efficient activities, mesoporous structures, and conductive carbon networks, which allow a feasible validation of the catalytic effects. Benefiting from the maximized atomic utilization, the atomic Co–N x centers exhibit much higher reaction kinetic constant (κ = 0.157 min −1 ) and mass activity toward the degradation of bisphenol A, far exceeding the Co nanocrystals (κ = 0.082 min −1 ). However, for the volume activities, the single‐atom catalyst does not show apparent advantages compared to the nanocrystal‐based catalyst. Overall, this work not only provides a viable pathway for comparing Fenton‐like catalytic effects of transition metal‐based nanoparticles or single atoms but also opens up a new avenue for developing prominent catalysts for organic pollutants' degradation. Abstract : The Fenton‐like catalytic activities and efficiencies of Co‐based nanoparticles and single‐atom structures are investigated and compared systematically via engineering catalysts comprising Co‐nanocrystals and atomic Co–N x codoped carbon nanotubes. Benefiting from the maximized atomic utilization, the atomic Co–N x centers exhibit much higher reaction kinetic constant and mass activity toward the degradation of bisphenol A, far exceeding the Co nanoparticles.