Boron-engineered interfacial electronic states orchestrate layered metal–π–carbon nitride coupling for intensified nonradical reactivity

Abstract

Aerospace propellant contaminants, such as monomethylhydrazine (MMH), present a significant environmental challenge, requiring advanced catalytic technologies for efficient water treatment. This study introduces a molecularly engineered heterostructure, layered double hydroxides@boron-doped graphitic carbon nitride (LDH@BCN), as a highly efficient peroxymonosulfate (PMS) activator. The LDH@BCN/PMS system achieves near-complete MMH degradation within 50 minutes, primarily driven by enhanced singlet oxygen (¹O₂) generation and an electron transfer pathway (ETP). Boron doping creates unique electronic synergy, optimizing charge transfer and PMS activation through –O–B–O– bridging and semi-metallic B–B bonds. Mechanistic insights from DFT and GC-MS analysis reveal non-covalent charge redistribution at the N–B interface, facilitating MMH degradation via hydroxylation and deamination. Polyethersulfone (PES)-supported LDH@BCN membranes exhibit long-term stability and anti-fouling properties, maintaining over 85% efficiency over 12 hours in continuous-flow systems. Life cycle assessment (LCA) further confirms the environmental sustainability of the LDH@BCN/PMS system, offering a low environmental impact and reduced resource consumption compared to traditional methods. This work presents LDH@BCN as a versatile and sustainable solution for the removal of ultra-trace pollutants in aerospace wastewater, advancing environmental catalysis in industrial applications.