Mn–Ce Bicenter of a Dual Single-Atom Catalyst Synergistically Triggers Reactive Oxygen Species Generation for Efficient Ozonation of Emerging Contaminants
Can He, Zhongguo Zhang*, Jianbing Wang*, Chunhui Zhang, Shizong Wang, Kefeng Zhang, Liangliang Wang, Junxing Han, Chenhao Gong and Kuixiao Li,
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引用次数: 0
Abstract
The synergistic effect of multiple reactive oxygen species (ROS) facilitates the degradation and mineralization of recalcitrant contaminants. However, bottlenecks include the rational design of single-atom catalysts with multiple active sites to produce multiple ROS in heterogeneous catalytic ozonation (HCO) processes and the detailed interpretation of the generation mechanisms. In this study, we prepared a dual single-atom Mn–(Nx–C)–Ce catalyst with dual active sites via a simple and scalable one-pot method in which atomically dispersed active Mn–N4 and Ce–N4 sites synergistically promoted the generation of •OH. Moreover, density functional theory calculations and molecular dynamics simulations elucidated that Mn–N4 sites on the catalyst surface preferred to generate •OH and •OHad, while Ce–N4 sites preferred to generate other ROS (O2•–, 1O2, and *Oad). The three main degradation pathways of N,N-diethyl-3-methylbenzamide (DEET) further revealed the synergistic effects of multiple ROS. Due to the ability for generation of multiple ROS, the Mn–(Nx–C)–Ce catalyst exhibited superior activity and excellent stability for the degradation of DEET and bezafibrate as well as advanced treatments of municipal sewage and coking wastewater. This study paves a new avenue for rationally designing a highly efficient and stabilized catalyst for ozone and provides an insight into the synergistic effect of Mn–Ce dual active sites in the HCO process.
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.