李绚,
李雪花^,,
陈景文
工业生态与环境工程教育部重点实验室, 大连理工大学环境学院, 大连 116024

作者简介: 李绚(1990),女,硕士生,研究方向为纳米毒理学,E-mail:lx_xuan@mail.dlut.edu.cn.

通讯作者: 李雪花,lixuehua@dlut.edu.cn ;

基金项目: 国家自然科学基金(21477016)；中央高校基本科研业务费专项资金(DUT16LK13)


中图分类号: X171.5

Synergistic Photogeneration of ¹O₂ and ·OH by Humid Acid and Carbon Nanomaterial in Aqueous Phase

Li Xuan,
Li Xuehua^,,
Chen Jingwen
Key Laboratory of Industrial Ecology and Environmental Engineering, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China

Corresponding author: Li Xuehua,lixuehua@dlut.edu.cn ;

CLC number: X171.5

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摘要:采用电子自旋共振光谱(EPR)技术，分析腐殖酸在光照下对4种典型碳纳米材料诱导产生单线态氧(¹O₂ )和羟基自由基(·OH)的影响。基于密度泛函理论计算4种典型碳纳米材料的前线轨道能，比较了它们分别经能量转移诱导产生¹O₂ 的能力以及经电子传递诱导产生·OH的能力。结果显示，4种不同形状的碳纳米材料(富勒烯、单壁碳纳米管、多壁碳纳米管以及石墨烯)悬浮液在紫外光照下均无¹O₂ 和·OH产生。与腐殖酸共同存在下，4种碳纳米材料均显著诱导¹O₂ 的产生，且富勒烯和石墨烯还能光致生成·OH。协同产生¹O₂ 的能力大小为：单壁碳纳米管 > 富勒烯 > 多壁碳纳米管 > 石墨烯，协同产生·OH的能力大小为：石墨烯 > 富勒烯。¹O₂ 的产生能力与碳纳米材料的能隙大小和颗粒聚集程度有关，而诱导产生·OH的能力主要取决于化学硬度。总之，我们的研究表明腐殖酸与碳纳米颗粒可协同产生活性氧物种。
关键词: 碳纳米材料/
腐殖酸/
活性氧物种/
EPR/
能带结构

Abstract:Effects of humic acid (HA) on photochemical production of singlet oxygen (¹O₂ ) and hydroxyl radical (·OH) induced by four typical carbon nanomaterials were investigated by using electron paramagnetic resonance (EPR). Based on the density functional theory, the frontier orbital energies of four typical carbon nanomaterials were calculated, and their ability of ¹O₂ generation by energy transfer and ·OH production by electron transform were compared, respectively. Results showed that C₆₀, single-walled carbon nanotubes (SWNT), multi-walled carbon nanotubes (MWNT) and graphene suspensions didn’t induce the production of ¹O₂ and ·OH under UV irradiation. When HA was present, four typical carbon nanomaterials significantly enhanced ¹O₂ production. In addition, C₆₀ and graphene in HA solutions also caused ·OH generation. The ability to produce ¹O₂ followed the order: SWNT > C₆₀ > MWNT > graphene, and to produce ·OH followed the order: graphene > C₆₀. The capacity of ¹O₂ production is attributed to the energy gap and particle aggregation degree of carbon nanomaterials, and the ability to induce ·OH mainly depended on the chemical hardness. In conclusion, our results indicated the synergistic photogeneration of ¹O₂ and ·OH by HA and carbon nanomaterials.
Key words:carbon nanomaterial/
humic acid/
reactive oxygen species/
EPR/
band structure.