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Lamellar Cluster-Like Grown FeCo Layered Double Hydroxides As Stable Peroxymonosulfate Activators at Wide Circumneutral Ph

Chemical engineering journal(2024)

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摘要
The development of effective and reliable Fenton-like catalytic systems in circumneutral pH is a longstanding interest. Metal-organic framework derivatives become promising catalyst candidates due to high catalytic accessibility and structural flexibility, but their stability remains in doubt. Herein, a MIL -88A self-templating strategy to synthesize structurally decentralized FeCo-layered-double hydroxide (FeCo-LDH, M-FCL) was proposed. The well-constructed M-FCL 3 presented superior peroxymonosulfate (PMS) activation for nearly 100 % sulfamethazine (SMT) degradation within 15 min, which was virtually wobble-slight in the pH = 2.5 - 10.5 range. The performance decrease at limiting pH was mainly ascribed to activity-blocked of M-FCL 3 by analyzing the involved reaction substrates and reactive oxygen species. In specific, the hydrolytic detachment or excessive aggregation of surface-active FeCo-LDH occurred at limiting pH with unbalanced hydrolysis-coprecipitation. Especially, theoretical calculations further exposed that the loss of dominated active Co site and the formation of inert SMT + dissociating species were detrimental to the catalytic process in acidic environments. Nevertheless, the well-founded resistance of the constructed M-FCL 3 /PMS system to interference and its ability to operate for a long period proved its potential for application in near-neutral environments. This work raised concern for the variations of Fenton-like catalysis at limiting pH, promoting the application of MOF-derived LDH for environmental remediation.
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关键词
Fenton-like reaction,Circumneutral pH,MOF derivatives,LDH,Wastewater treatment
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