Reconstructing the coordination environment of single atomic Fe-catalysts for boosting the Fenton-like degradation activities

This study develops an advanced single-atomic iron-loaded graphitic carbon nitride (Fe 1 /CN) with unparalleled efficiency for converting peroxymonosulfate (PMS) to oxidants for water treatment. We found that acid-etching of Fe 1 /CN leads to the reconstruction of conventional Fe 1 –N 4 to Fe 1 –C 2 N 1 active sites. The acid-induced Fe 1 –C 2 N 1 sites are more favorable for PMS binding and have a lower energy barrier for 1 O 2 production. The precise tuning of the coordination environment bestows the acid-etched Fe 1 /CN with 29 times higher rate constants of bisphenol A degradation than its pristine counterparts. Further, the particulate catalysts were assembled into a self-supported catalytic membrane, which demonstrates excellent long-term durability throughout 170 h flow-through tests in both synthetic and real wastewater . This work provides pivotal insights into improving PMS activation activity by regulating the coordination environment around single atomic Fe sites. The engineering innovation laid the groundwork for new point-of-use water treatment devices.