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Title
Surface cleavage and electron donation mechanism of emerging contaminantsexcited by H2O2 assisted Cu-based catalyst
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作者
孙英涛林业泓蔡璇英张致泰张发根胡春吕来
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Author
SUN Yingtao;LIN Yehong;CAI Xuanying;ZHANG Zhitai;ZHANG Fagen;HU Chun;LYU Lai
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单位
广州大学大湾区环境研究院珠江三角洲水质安全与保护教育部重点实验室广州大学乡村振兴研究院广州大学环境科学与工程学院
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Organization
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education,Institute of Environmental Research at Greater Bay, Guangzhou University
Institute of Rural Revitalization, Guangzhou University
School ofEnvironmental Science and Engineering, Guangzhou University
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摘要
源头水中存在着有毒的新污染物(ECs)和无毒的溶解性有机质(DOM),如何低耗高效地优先去除 ECs 是源头水深度净化的关键。 为突破这一瓶颈,本研究将 Cu、Al 金属物种原位调控为具有表面贫富电子微区的双反应中心(DRCs) 催化剂(CA-CN),并将其应用于去除水中微量ECs。 研究表明:在微量 H2O2的协助下,CA-CN 对于多种微量新污染物都具有优异的降解性能,尤其是对于双酚 A,在 5 min 内就可实现超 80%的去除率;在配置了微量 ECs 的实际源头水体中实现了 ECs 的优先去除;一系列表征技术发现污染物作为电子供体通过 π-π 结构与催化剂表面的缺电子中心发生界面作用并传递电子,电子通过催化剂表面的 C—O—M(金属物种)键桥传递至富电子中心,并活化吸附在此的过氧化氢和溶解氧;过氧化氢在整个过程中更重要的作用是触发降解 ECs 的链式反应。 这些发现突破了传统源头水净化的瓶颈问题,为开发新型高效、低耗水净化工艺提供了方向。
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Abstract
Toxic emerging contaminants (ECs) and non-toxic dissolved organic matter (DOM) arepresent in the source water. The key to purification of source water is to realize low cost and efficientpriority removal of toxic emerging contaminants. To break this bottleneck, Cu and Al metal specieswere modulated in situ into a dual reaction centers (DRCs) catalyst (CA-CN) with surface electronrich / -poor microregions in this work, and the catalyst was applied to the removal of trace ECs in water.It showed that CA-CN had excellent degradation performance for various trace ECs with the assistanceof trace amounts of H2O2, especially for BPA, which could be removed over 80% within 5 minutes. Inaddition, preferential removal of ECs was achieved in the actual source waters configured with traceECs. Series of characterization techniques showed that ECs acted as electron donors, and interface in⁃teraction occurred through π - π structures with electron - poor centers on the catalyst surface andtransfer electrons, and then the electrons were transferred to electron - rich centers via C—O—M(metal species) bond bridges on the catalyst surface, activating H2O2 and dissolved oxygen adsorbedtherein. The more important role of H2O2 in the whole process was to trigger the chain reaction of degrad⁃ing ECs. This discovery breaks through the bottleneck of traditional source water purification and providesa direction for development of new high-efficiency and low-consumption water purification processes.
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关键词
双反应中心微量 H2O2协助优先去除 ECs污染物供电子效应溶解氧活化
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KeyWords
Dual-reaction-center; Trace H2O2 assistance; Preferential removal of ECs; Contaminantelectron donor effect; Dissolved oxygen activation
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基金项目(Foundation)
国家自然科学基金-优秀青年科学基金项目(52122009);国家自然科学基金-面上项目(52070046)
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文章目录
0 引 言
1 材料和方法
1.1 实验材料
1.2 催化剂的制备
1.3 催化剂表征技术
1.4 实验方法
1.5 分析方法
2 结果与分析
2.1 表面电子极化分布的表征
2.2 对微量新污染物的高效去除
2.3 对实际水源水中新污染物的优先去除
2.4 双反应中心催化体系净水机制
3 结 论
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DOI
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引用格式
孙英涛, 林业泓, 蔡璇英, 等. H2O2协助铜基催化剂激发新污染物表面裂解性能与供电子机制[J]. 能源环境保护, 2023, 37(2): 187-195.
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Citation
SUN Yingtao, LIN Yehong, CAI Xuanying, et al. Surface cleavage and electron donation mechanism of emergingcontaminants excited by H2O2 assisted Cu-based catalyst[J]. Energy Environmental Protection, 2023, 37(2):187-195.
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