research-article
Xiaoben Yang,
Qianglin Li,
Ling Wu,
Binghua Zhou,
Zhipeng Wang,
Zhenghong Huang,
Mingxi Wang
Nitrophenols (NPs), classified as priority pollutantsdue to their significant toxicity, persistence, and bioaccumulation potential,pose severe threats to ecosystems and human health. Catalytic reduction,particularly the conversion of NPs like 4-nitrophenol (4-NP) to less toxicaminophenols using sodium borohydride (NaBH4), represents apromising remediation strategy. While conventional metal-based catalysts facelimitations including high cost, poor durability, and potential metal leaching,carbon-based metal-free catalysts (C-MFCs) have emerged as highly efficient,sustainable, and cost-effective alternatives. However, the precise reactionmechanisms governing NP reduction over C-MFCs remain ambiguous, and significantdebate surrounds the nature of the active sites and the structure-activityrelationships dictating performance. This review systematically elucidates thecatalytic sites and associated reduction mechanisms in C-MFCs. Wecomprehensively summarize design principles centered on defect engineeringstrategies, encompassing single-atom (N, S, B, P, O), dual-atom (B,N; N,S;N,P), and tri-atom (B,N,F; N,P,F) doping, alongside non-doping defects such asedge and pore defects. The critical structure-performance relationships linkingthese engineered active sites to catalytic activity (e.g., turnover frequency,TOF) are analyzed, integrating experimental evidence and theoretical insights.Furthermore, strategies for constructing three-dimensional architectures toenhance active site accessibility and catalyst stability are highlighted. Thiswork provides fundamental insights to guide the rational design ofnext-generation high-performance C-MFCs for sustainable nitrophenol pollutioncontrol.