Catalytic oxidation of clofibric acid by peroxydisulfate activated with wood-based biochar: Effect of biochar pyrolysis temperature, performance and mechanism

Catalytic oxidation of clofibric acid by peroxydisulfate activated with wood-based biochar: Effect of biochar pyrolysis temperature, performance and mechanism
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木基生物炭活化过二硫酸盐催化氧化氯贝酸:生物炭热解温度、性能和机理的影响

DOI:
10.1016/j.cej.2019.06.006
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发表时间:
2019-10
影响因子:
15.1
通讯作者:
Zhang Hui
Zhang Hui
中科院分区:
工程技术1区
文献类型:
--
作者:
Zhu Kangmeng;Wang Xisong;Geng Mengzi;Chen Dong;Lin Heng;Zhang Hui

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木质生物炭在 400-700°C 的不同热解温度下制备,并用于激活过二硫酸盐 (PDS) 以降解氯贝酸 (CA)。与其他 BC 相比,在 700°C 下热解的生物炭 (BC700) 显示出更优异的 CA 去除催化性能(60 分钟反应 97.8%)。 BC700/PDS 过程在 4.0–9.0 的初始 pH 范围内高效运行。还检查了 PDS 浓度和 BC700 剂量对 CA 去除的影响。应用自由基猝灭实验和电子顺磁共振 (EPR) 谱来识别 BC700/PDS 系统中产生的反应自由基。探讨了 BC700 芳环中持久自由基 (PFR)、氧官能团和 π-π* 过渡对 PDS 活化的作用。通过液相色谱-质谱法(LC-MS)鉴定了CA的反应中间体,并提出了相应的降解途径。这项研究有助于开发用于可持续修复水中有机污染物的绿色材料,并为进一步的研究提供支持。
Wood-based biochars were fabricated at different pyrolysis temperatures of 400–700 °C and used to activate peroxydisulfate (PDS) for the degradation of clofibric acid (CA). Biochar pyrolyzed at 700 °C (BC700) showed more excellent catalytic performance toward CA removal (97.8% in a 60 min reaction) than other BCs. The BC700/PDS process performed efficiently at initial pH range of 4.0–9.0. The effects of PDS concentration and BC700 dosage on CA removal were also examined. Radical quenching experiments and electron paramagnetic resonance (EPR) spectra were applied to identify the reactive radicals generated in the BC700/PDS system. The role of persistent free radicals (PFRs), oxygen functional groups and π-π*transitions in aromatic rings of BC700 for the PDS activation was explored. The reaction intermediates of CA were identified by liquid chromatography–mass spectrometry (LC–MS) and the corresponding degradation pathway was proposed. This study contributes to the development of green materials for sustainable remediation of organic contaminants in water and provides support for further studies.
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