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碳酸化废金属吸附树脂活化过硫酸盐降解2,4-二氯苯酚的机理研究

Insights into the mechanism of persulfate activation with carbonated waste metal adsorbed resin for the degradation of 2,4-dichlorophenol.

作者信息

Zhou Shuang, Hu Yonglian, Yang Minglei, Liu Yun, Li Qingke, Wang Yanhong, Gu Guohua, Gan Min

机构信息

School of Minerals Processing and Bioengineering, Key Laboratory of Biometallurgy of Ministry of Education, Central South University, Changsha, 410083, China; State Environmental Protection Key Laboratory of Mineral Metallurgical Resources Utilization and Pollution Control, Wuhan University of Science and Technology, Wuhan, 430081, China.

School of Minerals Processing and Bioengineering, Key Laboratory of Biometallurgy of Ministry of Education, Central South University, Changsha, 410083, China.

出版信息

Environ Res. 2023 Jun 1;226:115639. doi: 10.1016/j.envres.2023.115639. Epub 2023 Mar 10.

DOI:10.1016/j.envres.2023.115639
PMID:36907348
Abstract

Superabsorbent resin (SAR) saturated with heavy metals poses a threat to surrounding ecosystem. To promote the reutilization of waste, resins adsorbed by Fe and Cu were carbonized and used as catalysts (Fe@C/Cu@C) to activate persulfate (PS) for 2,4-dichlorophenol (2,4-DCP) degradation. The heterogeneous catalytic reaction was mainly responsible for 2,4-DCP removal. The synergistic effect of Fe@C and Cu@C was propitious to 2,4-DCP degradation. Fe@C/Cu@C with a ratio of 2:1 showed the highest performance of 2,4-DCP removal. 40 mg/L 2,4-DCP was completely removed within 90 min under reaction conditions of 5 mM PS, pH = 7.0 and T = 25 °C. The cooperation of Fe@C and Cu@C facilitated the redox cycling of Fe and Cu species to supply accessible PS activation sites, enhancing ROS generation for 2,4-DCP degradation. Carbon skeleton enhanced 2,4-DCP removal via radical/nonradical oxidation pathways and via its adsorption to 2,4-DCP. SO˙-, HO˙ and O were the dominate radical species involved in 2,4-DCP destruction. Meanwhile, the possible pathways of 2,4-DCP degradation were proposed based on GC-MS. Finally, recycling tests proved catalysts exhibited recyclable stability. Aiming to resource utilization, Fe@C/Cu@C with satisfactory catalysis and stability, is promising catalyst for contaminated water treatment.

摘要

饱和重金属的超吸水性树脂(SAR)对周围生态系统构成威胁。为了促进废物的再利用,将吸附了铁和铜的树脂碳化并用作催化剂(Fe@C/Cu@C),以活化过硫酸盐(PS)来降解2,4-二氯苯酚(2,4-DCP)。非均相催化反应是去除2,4-DCP的主要原因。Fe@C和Cu@C的协同作用有利于2,4-DCP的降解。比例为2:1的Fe@C/Cu@C表现出最高的2,4-DCP去除性能。在5 mM PS、pH = 7.0和T = 25°C的反应条件下,90分钟内可完全去除40 mg/L的2,4-DCP。Fe@C和Cu@C的协同作用促进了铁和铜物种的氧化还原循环,提供了可利用的PS活化位点,增强了用于2,4-DCP降解的ROS生成。碳骨架通过自由基/非自由基氧化途径以及通过其对2,4-DCP的吸附增强了2,4-DCP的去除。SO˙-、HO˙和O是参与2,4-DCP破坏的主要自由基物种。同时,基于气相色谱-质谱联用仪(GC-MS)提出了2,4-DCP降解的可能途径。最后,循环测试证明催化剂具有可循环使用的稳定性。为了实现资源利用,具有令人满意的催化性能和稳定性的Fe@C/Cu@C是用于污水处理的有前景的催化剂。

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