Cerium-based nanohydrolase for fast catalytic hydrolysis of β-lactam antibiotics in wastewater effluents

To defuse risks of antibiotic residues in effluent to achieve safe wastewater reuse, direct hydrolysis of the functional group responsible for the antibacterial activity, such as the of β-lactam ring in β-lactam antibiotics, has been recognized as an efficient and cost-effective strategy. However, the instability of natural hydrolases limits their use in treating antibiotic-containing wastewater. Herein, inspired by the active site of natural hydrolase, a Ce-based nanohydrolase was created for rapid hydrolysis of β-lactam antibiotics. The typical β-lactam antibiotic, penicillin G (PG), could be totally removed by the nanohydrolase within 2 min with a hydrolysis efficiency of 44%, and the hydrolysis efficiency could reach 98% within 10 min. It revealed that Ce(IV) in the nanohydrolase adsorbed PG via Lewis acid-Lewis base interaction to activate the β-lactam ring, while the -OH on Ce(III) served as nucleophile to attack the β-lactam ring, thereby promoting the hydrolysis of PG. The Ce-based nanohydrolase also showed good catalytic hydrolysis performance towards other commonly used β-lactam antibiotics and structurally related chemicals, implying its substrate universality. In addition to having high hydrolytic activity similar to that of natural hydrolases, this nanohydrolase exhibited extraordinary reusability and potential for practical applications that natural hydrolases do not possess. This work offers an innovative strategy to eliminate the risks of hydrolysable micropollutants in wastewater effluents and also provides reference for designing better nanohydrolase. © 2024 Elsevier B.V.