Highly dispersive Ru confined in porous ultrathin g-C3N4 nanosheets as an efficient peroxymonosulfate activator for removal of organic pollutants

Abstract

Ru species were loaded on a two-dimensional (2D) material of graphitic carbon nitride (2D g-C3N4) to serve as the efficient AOP catalysts. The catalytic activity was closely related to the dispersion degree of Ru, as determined by the inherent nanoarchitecture of the supporting material. Ultrathin g-C3N4 nanosheets with a unique porous structure were fabricated by further thermally oxidizing and etching bulk g-C3N4 (bCN) in air. Homogeneous dispersion of Ru species was successfully achieved on the porous few-layered g-C3N4 nanosheets (pCN) by stirring, washing, freeze drying and annealing processes to obtain Ru-pCN catalysts, whereas bCN or multilayered g-C3N4 (mCN) led to the aggregation of Ru nanoparticles in Ru-bCN and Ru-mCN materials. The conventional impregnation method also caused the resulting Ru-pCN-imp catalyst with undesirable Ru aggregation in spite of employing pCN. The optimal 4.4Ru-pCN removed 100% of 2,4,6-trichlorophenol (TCP) within only 3 min, superior to its counterpart samples, and exhibited remarkable degradation efficiencies for methyl orange, neutral red, 4-chlorophenol, tetracycline and oxytetracycline. Mechanistic studies suggested that four radicals, e.g., •OH, SO4• −, O2• − and 1O2 were generated during the peroxymonosulfate (PMS) activation, in which SO4• − and 1O2 played a major role.