Wen‐Kai Zhu, Ye Song, Du‐Juan Wu, Zhuo‐Xin Liao, Donggyun Kim, Jinhyeon Park, Jungmok You, Han Minsu, Song Li, Guang‐Yao Li, Chao‐Hai Wang, Jeonghun Kim
ABSTRACT Recently, cobalt/nitrogen co‐doped materials have emerged as heterogeneous catalysts to activate peroxymonosulfate (PMS) and have been applied to advanced oxidation processes for environmental remediation. However, their recyclability and reusability remain major barriers to practical application. In this work, we integrated cellulose nanofibrils (CNFs) as a binder with Co‐based zeolitic imidazolate framework‐67 (ZIF‐67) and carbonized, yielding a reusable Co/N co‐doped carbonaceous material. Briefly, a self‐assembly strategy was employed to construct two‐dimensional ZIF‐67@CNFs hybridized materials, followed by a straightforward pyrolysis process to fabricate Co/N co‐doped CNFs (CoNCNFs). Typical organic pollutants were selected as the target contaminants to investigate the catalytic performance of the CoNCNFs. The CoNCNFs achieved outstanding catalytic activity toward degrading the organic pollutants, with almost 100% degradation within 5 min. Additionally, the reaction parameters for the pollutants/PMS system were optimized. Furthermore, the CoNCNFs treated by an annealing process exhibited promising stability and reusability even after five consecutive reactions. Notably, scavenger experiments demonstrated that both SO 4 •− , • OH, O 2 •− , and 1 O 2 participated in the catalytic degradation process, whereas SO 4 •− played an important role. This work provides a new strategy to construct novel Co/N co‐doped carbonaceous material as efficient heterogeneous catalysts for environmental remediation.