Exploring water-soluble organic aerosols structures in urban atmosphere using advanced solid-state 13C NMR spectroscopy
Exploring water-soluble organic aerosols structures in urban atmosphere using advanced solid-state 13C NMR spectroscopy
复制标题
使用先进的固态 13C NMR 光谱探索城市大气中的水溶性有机气溶胶结构
DOI：
10.1016/j.atmosenv.2020.117503
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发表时间：
2020
影响因子：
5
通讯作者：
Schmidt-Rohr, Klaus
中科院分区：
文献类型：
--
作者：
Duarte, Regina M.B.O.;Duan, Pu;Mao, Jingdong;Chu, Wenying;Duarte, Armando C.;Schmidt-Rohr, Klaus
大气颗粒物中的水溶性有机物(WSOM)对气候和人类健康有着深远的影响。WSOM的这种环境意义的核心是一组复杂的化合物，其中大部分仍然经常是未破译的。然而，并不是所有的环境问题都需要深入研究WSOM成分的分子水平识别。了解不同官能团对整个气溶胶WSOM组成的贡献提供了一个非常重要的结构数据集，使WSOM能够在气候研究中得到更好的代表。首次应用先进的固体~(13)C核磁共振技术，包括近定量的~(13)C多交叉极化/魔角旋转(MULTI CP/MAS)、偶极退相多CP/MAS、带~(13)C化学位移各向异性滤光片的~(13)C/MAS和二维~1H-~(13)C异核相关(2D HETCOR)技术，对城市大气中采集的整个气溶胶WSOM进行了精确的定量结构描述。在不同冬季天气条件下，对两个短时间内采集的两个城市气溶胶WSOM样品进行了调查。核磁共振数据成功地精确定位了整个气溶胶WSOM成分的可变性，使得能够在两个短时间内为每个样品提出来源特定的结构特征。基于这些组成数据建立了一个新的城市气溶胶WSOM的结构模型，表明在短时间内存在三类独立的化合物，它们的含量和分子多样性都不同：富杂原子的脂肪族(链状或支链)、碳水化合物部分和高度取代的芳香族单元。这些发现确立了先进的固体核磁共振作为一种有希望的工具，用于在快速变化的大气条件下探测不均匀气溶胶WSOM的化学结构，从而能够解决模拟和测量的气溶胶WSOM之间的差异。
Water-soluble organic matter (WSOM) in air particles has profound effects on climate and human health. At the heart of this environmental significance of WSOM lies a complex set of compounds, of which a major fraction still often remains undeciphered. Yet, not all environmental problems require delving into the molecular-level identification of WSOM constituents. Understanding the contribution of different functional groups to whole aerosol WSOM composition offers a highly important structural dataset that enables a better representation of WSOM in climate studies. For the first time, advanced solid-state13C nuclear magnetic resonance (NMR) techniques, including nearly quantitative13C multiple cross polarization/magic angle spinning (multiCP/MAS), multiCP/MAS with dipolar dephasing, multiCP/MAS with13C chemical shift anisotropy filter, and two-dimensional1H–13C heteronuclear correlation (2D HETCOR), are applied to acquire an accurate quantitative structural description of whole aerosol WSOM collected in an urban atmosphere. Two urban aerosol WSOM samples collected in two short periods of time, under different wintry weather conditions, were investigated. NMR data successfully pinpointed the variability of whole aerosol WSOM composition, allowing to suggest source-specific structural characteristics for each sample in two short periods of time. A new structural model of urban aerosol WSOM was build based on this compositional data, showing the presence of three independent classes of compounds that vary both in content and molecular diversity within short periods of time: heteroatom-rich aliphatic (either chain or branched), carbohydrate-like moieties, and highly substituted aromatic units. These findings establish advanced solid-state NMR as a promising tool for probing the chemical structures of inhomogeneous aerosol WSOM in rapidly changing atmospheric conditions, allowing to resolve discrepancies between modeled and measured aerosol WSOM.
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影响因子：
4.6
作者：
Labrousse S;Sallée JB;Fraser AD;Massom RA;Reid P;Hobbs W;Guinet C;Harcourt R;McMahon C;Authier M;Bailleul F;Hindell MA;Charrassin JB
通讯作者：
Charrassin JB
影响因子：
11.4
作者：
Gehui Wang;K. Kawamura
通讯作者：
Gehui Wang;K. Kawamura
来自二维 1H-13C 相关固态核磁共振的腐殖酸新结构信息。
影响因子：
11.4
作者：
J. Mao;B. Xing;K. Schmidt
通讯作者：
K. Schmidt
城市环境中的二次有机气溶胶起源：生物和燃料燃烧前体的影响。
影响因子：
3.4
作者：
M. Minguillón;Noemí Pérez;Nicolas Marchand;A. Bertrand;B. Temime;Konstantinos Agrios;S. Szidat;B. L. Drooge;Alexandre Sylvestre;A. Alastuey;C. Reche;A. Ripoll;Esther Marco;J. Grimalt;X. Querol
通讯作者：
X. Querol