Xiao Ge, Wenjing Li, Jie Wang, Yangfan Yuan, Hongxia Xu, Bin Gao, Shengsen Wang*, Xiaozhi Wang and Yuen Wu,
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引用次数: 0
Abstract
The ability of single-atom catalysts (SSCs) to degrade refractory organic pollutants in peroxymonosulfate (PMS)-based heterogeneous catalysis can be compromised due to less diversity in reactive species and unfavorable affinity with PMS. Herein, the as-prepared ternary atomic-scale site catalyst comprising single-atomic Fe/Ce sites and Fe cluster sites (Fe-Ce-BC-900) could completely remove concentrated 4-chlorophenol (4-CP, 40 mg L–1) in aqueous solution within 30 min, 1.20–1.35 times more efficient than Fe SSCs or Ce SSCs. The reactive oxygen species (ROSs) could be highly diversified on the ternary atomic-scale sites because of the Janus mechanisms: the production of nonradicals (1O2) through PMS oxidation and the generation of radicals (SO4•– and •OH) via PMS reduction on the ternary catalytic sites, which accounted for oxidative degradation of concentrated 4-CP. Density functional theory (DFT) calculations indicated that the ternary catalytic sites enhanced the uneven charge distribution and down-regulated the d-band center of Fe-Ce-BC-900 as compared to Fe-BC-900 and Ce-BC-900 catalysts, thereby optimizing the adsorption energy of PMS molecules and promoting electron transfer between metal sites and adjacent oxygen atoms. This study provides valuable insights into the configuration of multicatalytic sites for detoxification of organic-contaminants-polluted wastewater.
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.