In situ preparation of highly graphitized N-doped biochar geopolymer composites for efficient catalytic degradation of tetracycline in water by H2O2

Abstract

Advanced oxidation processes (AOPs) hold great prospects for the treatment of antibiotic wastewater. N-doped biochar (NB) has received increasing attention as a catalyst for AOPs because of its green nature, abundant biomass resources, and low cost. However, NB catalysts are complicated to prepare and difficult to recover, limiting their practical application. In this study, an N-doped biochar geopolymer composite (NBGC) was synthesized via in situ doping, simultaneous carbonization, and activation (ISCA) of lignin and urea in the porous geopolymer flake, without additional activators. The ISCA process used a low-cost geopolymer flake that not only served as a carrier to immobilize NB and facilitate the recovery, but also applied its inherent strong alkalinity to activate NB. The composite catalyst obtained at 600 °C (NBGC-600) exhibited excellent activity in activating H2O2 to degrade tetracycline (∼100%, 50 mg/L). The EPR results indicated that NBGC-600 had a strong ability to activate and decompose H2O2 to •OH, which could be attributed to its rich persistent radicals, graphitized N and CO groups, as well as the high degree of graphitization of biochar. The degradation pathway and intermediates of tetracycline in the NBGC-600-H2O2 system were also discussed according to the HPLC-MS results. Moreover, NBGC-600 had excellent reusability and showed great potential for continuous treatment of tetracycline in water. This work paves a new way for the synthesis of cost-effective N-doped biochar composite catalysts for AOPs.