Enhancing oxidants activation by transition metal-modified catalytic membranes for wastewater treatment

Yi, Qiuying; Li, Zhouyan; Li, Jiayi; Zhou, Jiahui; Li, Xuesong; Dai, Ruobin; Wang, Xueye

doi:10.1007/s11164-022-04895-3

Cited by 8 publications

(1 citation statement)

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“…Refractory organic pollutants pose a significant environmental challenge due to their resistance to degradation, which is primarily attributed to their complex and stable molecular structures. − Strategies to degrade these contaminants during wastewater treatment have focused on peroxymonosulfate (PMS)-based oxidation technologies. − Activation of PMS leads to the generation of reactive oxygen species (ROSs) that contribute to degradation, including hydroxyl radicals (HO • ), sulfate radicals (SO 4 •– ), singlet oxygen ( 1 O 2 ), , and high-valent metals. , Various materials have been employed to enhance the activation of PMS such as photocatalysts, electrocatalysts, cocatalysts, and advanced functional materials. , Furthermore, integrating catalysts into wastewater treatment membranes, known as catalytic membranes, has emerged as an effective method for rapid and efficient production of ROS in PMS oxidation processes. − …”

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confidence: 99%

Single-Atom Cobalt-Modified Catalytic Membrane for Pollutant Degradation with High Tolerance of Environmental Interferences

Yi,

Lv,

Yang

et al. 2023

ACS EST Eng.

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Peroxymonosulfate (PMS)-based catalytic oxidation processes represent promising means of degrading organic contaminants for wastewater treatment. However, these systems typically use dispersions of catalytic particles that require challenging recovery steps, and the radical-based oxidation processes are inefficient due to reactions with background species present in natural waters. Herein, we incorporate single-atom cobalt into a catalytic membrane (Co−C 3 N 4 ) for the selective production of high-valent cobalt-oxo species (Co (IV) =O). The generation of Co (IV) �O is confirmed by 18 O isotopic labeling and scavenger experiments. Furthermore, density functional theory calculations show that Co (IV) �O formation rather than radical formation is thermodynamically favorable in the Co−C 3 N 4 /PMS process. The Co−C 3 N 4 membrane activates PMS with a rate constant of k obs = 11.1540 min −1 , which is nearly 105 times greater than that for traditional heterogeneous catalytic dispersions (i.e., k obs = 0.1065 min −1 ). Additionally, the Co (IV) �O-mediated oxidation process degrades contaminants with low ionization potentials at accelerated rates (e.g., k obs = 17.2860 min −1 for guaiacol). The process also demonstrates improved resistance to background ions and humic acid, in comparison with conventional radical-based oxidation processes. Our study presents a facile approach to engineer singleatom catalytic membranes for high-valent metal-oxo-mediated PMS-based catalytic oxidation processes, providing promising opportunities for efficiently removing persistent pollutants while mitigating interference from background species.

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