Yuan Ruixia, Jiang Zhongqiu, Wang Zhaohui, Gao Simeng, Liu Zhanjian, Li Meiling, Boczkaj Grzegorz
College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, China.
College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, China.
J Colloid Interface Sci. 2020 Jul 1;571:142-154. doi: 10.1016/j.jcis.2020.03.041. Epub 2020 Mar 11.
In this work, birnessite-type δ-MnO 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 = 27.5 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 MnO. SO was confirmed to be the predominant reactive species for AO7 decomposition by electron spin resonance and quenching tests. The synergistic catalytic mechanism of MnO/NF and the role of inner-sphere complexation between the active sites of MnO and peroxymonosulfate were thoroughly investigated. Compared with traditional nano/micro-sized catalysts, 3D macroscopic MnO/NF with facile recovery and high stability potentially facilitates fascinating applications as green heterogeneous catalysis approach.
在本工作中,通过一步水热法将水钠锰矿型δ-MnO纳米花均匀沉积在三维泡沫镍(NF)上,用于高效活化过一硫酸盐(PMS)以降解酸性橙7(AO7)。高比表面积、大孔容和三维分级结构促进了传质和电子转移,具有很高的催化活性。由于三维分级结构能够有效避免纳米MnO团聚,实现了低反应能垒(E = 27.5 kJ/mol)以及回收过程中极低的锰浸出率(<0.06 mg/L)和出色的可重复使用性。通过电子自旋共振和猝灭试验证实SO为AO7分解的主要活性物种。深入研究了MnO/NF的协同催化机理以及MnO活性位点与过一硫酸盐之间的内球络合作用。与传统的纳米/微米尺寸催化剂相比,具有易于回收和高稳定性的三维宏观MnO/NF作为绿色多相催化方法可能具有迷人的应用前景。