Microenvironment modulation of biocatalyst derived from natural cellulose of wheat straw for enhancing p-nitrophenol degradation via boosting peroxymonosulfate activation

Defect-rich nitrogen-doped biocatalyst (B-NC) was synthesized from natural cellulose of wheat straw using straightforward mechanical method and one-step pyrolysis approach. In contrast to the nitrogen-doped biocatalyst (NC), by leveraging the synergistic effects of nitrogen dopants and surface defects, the microenvironmentmodulated B-NC exhibited the enhanced mass transfer efficiency and a significant improvement in reactivity for p-nitrophenol degradation (111 %-196 %). The catalyst's exceptional performance primarily arose from graphitic N, pyridinic N and C--O active sites, which mainly derived from the cellulose structure of wheat straw and nitrogen dopants. Electron paramagnetic resonance and quenching tests confirmed that the B-NC/peroxymonosulfate system generated more reactive species (SO4 center dot- , center dot OH, O2 center dot- , and 1O2) during p-nitrophenol degradation, surpassing the NC/peroxymonosulfate system. Additionally, both density functional theory calculations and electrochemical experiments provided evidence of peroxymonosulfate strongly adsorbing onto B-NC's defect sites, facilitating the formation of catalyst/peroxymonosulfate* complexes and promoting electron transfer processes. This research provides valuable insights into the regulation of defects in nitrogen-doped biocatalyst derived from natural cellulose, presenting a promising solution for remediating refractory organic pollutants.