B-Bridge Regulated Asymmetric Dual-Atomic Catalysts for Synergistically Enhanced Styrene Mineralization and CO₂...

Developing innovative resource utilization strategies to achieve sustainable recycling of waste-to-fuel is highly desirable, yet the design of cost-effective bifunctional catalysts with dual high-efficiency remains unexplored. While the Fenton-like reaction relies on enhancing peroxymonosulfate (PMS) adsorption and accelerating interfacial electron transfer to improve kinetic rates, CO₂ reduction is constrained by sluggish kinetics and competing hydrogen evolution reaction. Herein, we construct a bifunctional catalyst (NiFe-BNC) featuring dual-atomic active sites by introducing boron atoms into a biomass-derived chitosan substrate rich in functional groups, which optimizes atomic coordination environments. In situ experiments and density functional theory calculations reveal that B-atom modulation facilitates carbon substrate defect enrichment, while the charge-tuning effect between metal sites and "boron electron bridge" optimizes PMS adsorption configurations. This synergistic effect facilitates the interfacial electron transfer and enhances the CO₂ adsorption capacity of NiFe-BNC by 6 times that of NiFe-NC. The obtained NiFe-BNC exhibits significantly enhanced catalytic activity and selectivity, realizing 99% efficient degradation of volatile organic pollutants in the flowing phase within 2 h and stable mineralization exceeding 60%, while achieving a large current density of 1000 mA cm^-2 and CO Faraday efficiency of 98% in the flow electrolytic cell. This work innovatively paves a new way for the rational design of cost-effective functional catalysts to achieve carbon cycle utilization.