Ring defects-rich and pyridinic N-doped graphene aerogel as floating adsorbent for efficient removal of tetracycline: Evidence from NEXAFS measurements and theoretical calculations

Abstract

The rational design of carbon-based adsorbents with a high uptake efficiency for polar organic molecules is a key challenge in water purification research. Herein, we report a graphene aerogel that is doped with pyridinic-N and has abundant ring defects (denoted by DNGA). The aerogel sample exhibits a high adsorption capacity of 607.1 mg/g toward tetracycline (TC), a fast adsorption process (20 min), and good reusability (with a declining efficiency < 10.0% after five cycles), while being easy to recycle. C/N K-edge X-ray absorption near-edge structure (XANES) measurements demonstrate that the efficient adsorption capacity of the DNGA sample is related to the presence of ring defects and the pyridinic-N species. Density functional theory (DFT) calculations demonstrate that ring defects of type 5–8–5 and the pyridinic-N species at the edge location are primarily responsible for TC removal. In this study, we resolve a controversial issue regarding the origin of the adsorption performance origin of N-doped carbon-based adsorbents. The findings of this study can guide the development of novel and improved N-doped carbon-based adsorbents for the removal of target contaminants.