Boric acid pyrolysis modulating secondary-shell boron coordination in iron single-atom catalysts for high-efficiency peracetic acid activation and bisphenol A degradation
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引用次数: 0
Abstract
In this study, we incorporated boric acid into the synthesis of single-atom catalysts (SACs), where it served dual roles by facilitating iron dispersion and introducing boron coordination. Our results show that boron oxide formed from molten boric acid acts as both an efficient high-temperature carbonization agent and a metal-blocking medium, effectively suppressing iron nanoparticle formation in the resulting iron SAC material (Fe@NBC). The material features predominantly nitrogen-coordinated single iron atoms, with boron atoms successfully incorporated into secondary coordination shells. Fe@NBC demonstrates excellent Fenton-like catalytic activity, completely removing 10 mg/L bisphenol A (BPA) within 30 min through peracetic acid (PAA) activation. Increasing the boron content from 2.78 % to 4.23 % improved BPA removal efficiency from 52.1 % to 100 %. Density functional theory (DFT) calculations reveal that electron-deficient boron atoms adjust the electronic structure of Fe-N4 active sites. As the boron coordination number in the second shell increases from 1 to 2, the central iron atom loses more electrons (1.20e- to 2.25e-). This strengthens the oxidant’s adsorption at the Fe site (−0.96 eV to −1.07 eV), boosts electron transfer between PAA and the Fe active center while reducing the energy barrier for hydroxyl radical formation. This work provides critical insights for designing boron-mediated Fenton-like catalysts to efficiently degrade organic pollutants in water.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.