Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Atmospheric Chemistry and Physics Pub Date : 2024-07-04 DOI:10.5194/acp-24-7575-2024
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, Xinming Wang
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Abstract

Abstract. Humic-like substances (HULIS) are complex macromolecules in water-soluble organic compounds (WSOCs) containing multiple functional groups, and transition metal ions (TMs) are ubiquitous in atmospheric particles. In this study, potential physical and chemical interactions between HULIS and four TM species, including Cu2+, Mn2+, Ni2+, and Zn2+, were analyzed by optical method under acidic, weakly acidic, and neutral conditions. The results showed that Cu2+, Mn2+, and Zn2+ only slightly enhanced mass absorption efficiency (MAE365) of HULIS in winter and had indiscernible effects on the absorption Ångström exponent (AAE) of HULIS in both seasons under all acidity conditions. All four TMs had fluorescence quenching effects on winter HULIS, and only Cu2+ had similar effects on summer HULIS, with the highest quenching coefficients found under weakly acidic conditions in both seasons. The 1H-nuclear magnetic resonance (1H-NMR) and Fourier-transform infrared (FTIR) spectra revealed that Cu2+ mainly bound with aromatic species and tightened the molecule structures of HULIS. The parallel factor analysis (PARAFAC) results extracted four components of HULIS, including low-oxidized humic-like substances (C1), N-containing compounds (C2), highly oxidized humic-like substances (C3), and the mixing residuals (C4), from the fluorescence spectra in both winter and summer. The spectral characteristic of HULIS with Cu2+ additions under three acidity conditions indicated that electron-donating groups of HULIS mainly corresponded to C1 and C3, with Cu2+ binding with HULIS by replacing protons, while electron-withdrawing groups of HULIS could correspond to C2, with its connection with Cu2+ through electrostatic adsorption or colliding-induced energy transfer.
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测量报告:过渡金属离子对类腐殖质(HULIS)光学特性的影响揭示了一种结构偏好--中国北京 PM2.5 案例研究
摘要。类腐植酸物质(HULIS)是水溶性有机化合物(WSOCs)中含有多种官能团的复杂大分子,而过渡金属离子(TMs)在大气颗粒物中无处不在。本研究在酸性、弱酸性和中性条件下,采用光学方法分析了 HULIS 与四种过渡金属离子(包括 Cu2+、Mn2+、Ni2+ 和 Zn2+)之间潜在的物理和化学相互作用。结果表明,在所有酸度条件下,Cu2+、Mn2+和Zn2+仅在冬季略微提高了HULIS的质量吸收效率(MAE365),而在两个季节对HULIS的吸收Ångström指数(AAE)的影响不明显。所有四种 TM 对冬季的 HULIS 都有荧光淬灭效应,只有 Cu2+ 对夏季的 HULIS 有类似的效应,在两个季节的弱酸性条件下淬灭系数最高。1H-核磁共振(1H-NMR)和傅立叶变换红外光谱(FTIR)显示,Cu2+主要与芳香族物种结合,使HULIS的分子结构更加紧密。平行因子分析(PARAFAC)结果从冬夏两季的荧光光谱中提取了HULIS的四个组分,包括低氧化腐殖样物质(C1)、含N化合物(C2)、高氧化腐殖样物质(C3)和混合残余物(C4)。三种酸度条件下加入Cu2+的类腐殖质的光谱特征表明,类腐殖质中的供电子基团主要对应于C1和C3,Cu2+通过取代质子与类腐殖质结合;而类腐殖质中的取电子基团可能对应于C2,通过静电吸附或碰撞引起的能量转移与Cu2+结合。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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