In this work, birnessite-type delta-MnO2 nanoflowers were uniformly deposited on 3D nickel foam (NF) by one-step hydrothermal route for high-efficient activation of peroxymonosulfate (PMS) towards degradation of acid orange 7 (AO7). High specific surface area, large pore volume and 3D hierarchical structure promotes the mass and electron transfer for great catalytic activity. Low reaction energy barrier (E-a = 2 7.5 kJ/mol) and outstanding reusability with extremely low manganese leaching during recycling (<0.06 mg/L) was achieved due to the 3D hierarchical structure which could effectively avoid the agglomeration of nano-sized MnO2 center dot SO4(center dot) was confirmed to be the predominant reactive species for AO7 decomposition by electron spin resonance and quenching tests. The synergistic catalytic mechanism of MnO2/NF and the role of inner-sphere complexation between the active sites of MnO2 and peroxymonosulfate were thoroughly investigated. Compared with traditional nano/micro-sized catalysts, 3D macroscopic MnO2/NF with facile recovery and high stability potentially facilitates fascinating applications as green heterogeneous catalysis approach. (C) 2020 Elsevier Inc. All rights reserved.