氮掺杂还原氧化石墨烯泡沫吸附/活化过硫酸盐协同去除双酚A的研究

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摘要利用氧化石墨烯和氨水为原料，采用水热法-冷冻干燥技术制备了易回收氮掺杂还原氧化石墨烯泡沫（N-RGF）催化剂，通过SEM，XRD，XPS，FT-IR，BET和TG等手段对催化剂结构和表面物理化学性质进行表征和分析.利用N-RGF通过吸附/活化过二硫酸盐（PDS）降解协同去除双酚A （BPA），优化了其制备条件，并探讨去除机理.结果表明，N-RGF为网状三维结构，孔径约为1~5μm，最优条件为180℃水热反应20h，氮掺杂量为6%.制备的N-RGF降解BPA速率是RGF的4.88倍.活性物种捕获实验和电子顺磁共振（EPR）研究结果显示单线态氧（¹O₂）是N-RGF活化PDS降解BPA的主要活性物种.HPLC-MS检测了降解过程的中间体，并提出了可能的降解途径.MCF-7雌激素活性测试结果显示N-RGF通过吸附/活化PDS可有效消除母体的雌激素活性而不产生雌激素活性更强的中间体.

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	和丽金
	龙俊宏
	金华蕾
	左怡丹
	宋洁
	夏丽红
	石苗
	罗利军
	戴建辉

关键词 ：双酚A, 氮掺杂还原氧化石墨烯泡沫, 过二硫酸盐, 活化, 吸附

Abstract：The nitrogen doped reduced graphene oxide foam (N-RGF) was prepared by hydrothermal method followed freeze-drying treatment using graphene oxide and ammonia as starting materials. The structure and surface physical-chemical properties of as-prepared catalysts were investigated and analysed by SEM, XRD, XPS, FT-IR, BET and TG techniques. The N-RGF was used to activate peroxydisulfate (PDS) for BPA removal via adsorption/degradation synergistically. The results showed that the N-RGF catalyst was a three-dimensional structure with average pore size(1~5μm). Its optimal preparation conditions were 6% nitrogen doping amount and hydrothermal treatment at 180℃ for 20h. The degradation rate constant of BPA over N-RGF activated PDS was 4.88 times than that over RGF activated PDS. Active species capture experiment and electron paramagnetic resonance (EPR) results showed that singlet oxygen (¹O₂) was the main contributor for BPA abatement. The four possible degradation intermediates were confirmed by ultra-high-performance liquid chromatography-mass spectrometry, and possible degradation pathway was proposed. The estrogenic activity of treated solution was reduced by MCF-7cell viability evaluation.

Key words： bisphenol A nitrogen-doped reduced graphene oxide foam peroxydisulfate activation adsorption

收稿日期: 2022-08-25

PACS:

X703

基金资助:国家自然科学基金资助项目（22266036，22065036）；云南省中青年学术技术带头人后备人才项目（202105AC160055）；云南省教育厅科学研究基金项目（2022Y463）

通讯作者: 罗利军,教授,10501931@qq.com E-mail: 10501931@qq.com

作者简介: 和丽金(1998-),女,云南丽江人,云南民族大学硕士研究生,主要从事新污染物治理.

引用本文:

和丽金, 龙俊宏, 金华蕾, 左怡丹, 宋洁, 夏丽红, 石苗, 罗利军, 戴建辉. 氮掺杂还原氧化石墨烯泡沫吸附/活化过硫酸盐协同去除双酚A的研究[J]. 中国环境科学, 2023, 43(3): 1107-1121. HE Li-jin, LONG Jun-hong, JIN Hua-lei, ZUO Yi-dan, SONG Jie, XIA Li-hong, SHI Miao, LUO Li-jun, DAI Jian-hui. Removal of bisphenol A by nitrogen-doped reduced graphene oxide foam via adsorption/peroxydisulfate activation. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(3): 1107-1121.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I3/1107

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