Yi Shen, Mingzheng Yang, Chao Zhu, Haizhong Zhang, Renlan Liu, Jun Wang, Qile Fang, Shuang Song, Baoliang Chen
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引用次数: 0
Abstract
The activation of peroxymonosulfate (PMS) to generate singlet oxygen (1O2) for the removal of emerging organic pollutants (EOPs) from complex aqueous environments has garnered widespread attention. However, the low efficiency and selectivity of current PMS activation for 1O2 generation result in suboptimal EOP degradation. To enhance the selectivity of PMS activation and promote the non-radical pathway, non-metal heteroatoms with varying electronegativities were introduced to disrupt the symmetrical coordination structure of Fe active sites in Fe single-atom catalysts. The results showed that, in the B-Fe1/GLCNs/PMS system, the pseudo-first-order kinetic rate for bisphenol A (BPA) degradation reached 4.435 min–1, which is 7.4 times higher than that of the unmodified control group. Experimental and theoretical calculations demonstrated that the doping of non-metal heteroatoms altered the electron density and distribution at the Fe active sites, thereby modulating the adsorption configuration of HSO5– and increasing the selectivity for PMS activation to generate 1O2. Additionally, the degradation of EOPs by 1O2 produced intermediate products with lower biological toxicity, and 1O2 demonstrated strong anti-interference capability. The change in HSO5– morphology improved the rate of 1O2 generation. This study provides deep insights into designing high-performance PMS activation catalysts via non-metal doping to regulate the electronic structure of active sites for a selective non-radical pathway.
期刊介绍:
ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources.
The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope.
Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.