Activation of Hydrogen Peroxide by a Titanium Oxide-Supported Iron Catalyst: Evidence for Surface Fe(IV) and Its Selectivity,Environmental Science & Technology

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Activation of Hydrogen Peroxide by a Titanium Oxide-Supported Iron Catalyst: Evidence for Surface Fe(IV) and Its Selectivity
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-11-12 , DOI: 10.1021/acs.est.0c04262
Hak-Hyeon Kim ₁ , Hongshin Lee ₂ , Donghyun Lee ₃ , Young-Jin Ko ₄ , Heesoo Woo ₅ , Jaesang Lee ₂ , Changha Lee ₃ , Anh Le-Tuan Pham ₁

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Iron immobilized on supports such as silica, alumina, titanium oxide, and zeolite can activate hydrogen peroxide (H₂O₂) into strong oxidants. However, the role of the support and the nature of the oxidants produced in this process remain elusive. This study investigated the activation of H₂O₂ by a TiO₂-supported catalyst (FeTi-ox). Characterizing the catalyst surface in situ using X-ray absorption spectroscopy (XAS), together with X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR), revealed that the interaction between H₂O₂ and the TiO₂ phase played a key role in the H₂O₂ activation. This interaction generated a stable peroxo–titania ≡Fe(III)–Ti–OOH complex, which reacted further with H₂O to produce a surface oxidant, likely ≡Fe[IV] ═ O²⁺. The oxidant effectively degraded acetaminophen, even in the presence of chloride, bicarbonate, and organic matter. Unexpectedly, contaminant oxidation continued after the H₂O₂ in the solution was depleted, owing to the decomposition of ≡Fe(III)–Ti–OOH by water. In addition, the FeTi-ox catalyst effectively degraded acetaminophen over five testing cycles. Overall, new insights gained in this study may provide a basis for designing more effective catalysts for H₂O₂ activation.

中文翻译：

氧化钛负载的铁催化剂对过氧化氢的活化作用：表面Fe（IV）及其选择性的证据

固定在二氧化硅，氧化铝，氧化钛和沸石等载体上的铁可将过氧化氢（H ₂ O ₂）活化为强氧化剂。然而，在该过程中载体的作用和氧化剂的性质仍然难以捉摸。本研究研究了TiO ₂负载的催化剂（FeTi-ox）对H ₂ O ₂的活化作用。使用X射线吸收光谱（XAS），X射线光电子能谱（XPS）和电子顺磁共振（EPR）来原位表征催化剂表面，表明H ₂ O ₂和TiO ₂相之间的相互作用起到了H ₂ O中的关键作用₂激活。这种相互作用产生了稳定的过氧-二氧化钛≡Fe（III）-Ti-OOH配合物，它与H ₂ O进一步反应生成表面氧化剂，可能是≡Fe[IV]═O2 ⁺。即使在存在氯化物，碳酸氢盐和有机物的情况下，氧化剂也能有效降解对乙酰氨基酚。出乎意料的是，由于水分解≡Fe（III）-Ti-OOH，溶液中的H ₂ O ₂耗尽后，污染物继续氧化。此外，FeTi-ox催化剂可在五个测试周期内有效降解对乙酰氨基酚。总体而言，在这项研究中获得的新见解可能为设计更有效的H ₂ O ₂活化催化剂提供基础。

更新日期：2020-12-01

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