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解析富铁污泥水热炭在介导三氯生类芬顿氧化中关键作用。

Unraveling the critical role of iron-enriched sludge hydrochar in mediating the Fenton-like oxidation of triclosan.

机构信息

School of Energy and Environmental Engineering, Hebei University of Technology, Tianjin, 300401, China.

MOE Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Science and Engineering, Nankai University, Tianjin 300071, China.

出版信息

Environ Pollut. 2023 Mar 15;321:121205. doi: 10.1016/j.envpol.2023.121205. Epub 2023 Feb 2.

Abstract

The traditional Fenton system is subject to the low efficiency of the Fe(III)/Fe(II) conversion cycle, with significant attempts made to improve the oxidation efficiency by overcoming this hurdle. In support of this goal, iron-enriched sludge-derived hydrochar was prepared as a high-efficiency catalyst by one-step hydrothermal carbonization and its performance and mechanisms in mediating the oxidation of triclosan were explored in the present study. The hydrochar prepared at 240 °C for 4 h (HC) had the highest removal of triclosan (97.0%). The removal of triclosan in the HC/HO system was greater than 90% in both acidic and near-neutral environments and remained as high as 83.5% after three cycles, indicating the broad pH applicability and great recycling stability of sludge-derived hydrochar in Fenton-like systems. HO was activated by both persistent free radicals (PFRs; 19.7%) and iron (80.3%). The binding of Fe(III) to carboxyl decreased the electron transfer energy from HO to Fe(III), making its degradation efficiency 2.6 times greater than that of the conventional Fenton reaction. The study provides a way for iron-enriched sludge utilization and reveals a role for hydrochar in promoting iron cycling and electron transfer in the Fenton reaction.

摘要

传统的芬顿体系受到 Fe(III)/Fe(II)转化循环效率低的限制,为了克服这一障碍,人们做了大量尝试来提高氧化效率。为了支持这一目标,本研究采用一步水热碳化法制备了富铁污泥衍生水热炭作为高效催化剂,探索了其在介导三氯生氧化中的性能和机制。在 240°C 下反应 4 小时制备的水热炭(HC)对三氯生的去除率最高(97.0%)。在酸性和近中性环境中,HC/HO 体系对三氯生的去除率均大于 90%,经过三次循环后仍高达 83.5%,表明富铁污泥衍生水热炭在类芬顿体系中具有广泛的 pH 适用性和良好的循环稳定性。HO 被持久自由基(PFRs;19.7%)和铁(80.3%)共同活化。Fe(III)与羧基的结合降低了 HO 向 Fe(III)转移的电子转移能量,使其降解效率比传统芬顿反应高 2.6 倍。该研究为富铁污泥的利用提供了一种方法,并揭示了水热炭在促进芬顿反应中铁循环和电子转移中的作用。

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