双单原子催化剂的锰-铈双中心可协同触发活性氧生成,从而高效臭氧氧化新污染物

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-07-29 DOI:10.1021/acsestengg.4c0018910.1021/acsestengg.4c00189
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

摘要

多种活性氧(ROS)的协同作用促进了难降解污染物的降解和矿化。然而,瓶颈问题包括如何合理设计具有多个活性位点的单原子催化剂,以便在异相催化臭氧氧化(HCO)过程中产生多种 ROS,以及如何详细解释其生成机制。在本研究中,我们通过简单、可扩展的一锅法制备了具有双活性位点的双单原子 Mn-(Nx-C)-Ce 催化剂,其中原子分散的活性 Mn-N4 和 Ce-N4 位点协同促进了 -OH 的生成。此外,密度泛函理论计算和分子动力学模拟阐明,催化剂表面的Mn-N4位点更倾向于生成-OH和-OHad,而Ce-N4位点更倾向于生成其他ROS(O2--、1O2和*Oad)。N,N-二乙基-3-甲基苯甲酰胺(DEET)的三种主要降解途径进一步揭示了多种 ROS 的协同作用。由于能够产生多种 ROS,Mn-(Nx-C)-Ce 催化剂在降解 DEET 和贝扎非贝特酯以及高级处理城市污水和焦化废水方面表现出卓越的活性和稳定性。这项研究为合理设计高效、稳定的臭氧催化剂开辟了一条新途径,并深入探讨了 Mn-Ce 双活性位点在 HCO 过程中的协同效应。
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Mn–Ce Bicenter of a Dual Single-Atom Catalyst Synergistically Triggers Reactive Oxygen Species Generation for Efficient Ozonation of Emerging Contaminants

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.

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ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
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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.
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