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中国北方高海拔地区大气类腐殖质(HULIS)的特征:丰度、分子组成和光学性质

Characterization of atmospheric humic-like substances (HULIS) at a high elevation in North China: Abundance, molecular composition and optical properties.

作者信息

Gong Chaofan, Liu Xinghui, Nie Xiaoling, Xu Xinmiao, Wang Xinfeng, Xue Likun, Wang Yan

机构信息

School of Environmental Science and Engineering, Shandong University, Qingdao 266237, China.

School of Environmental Science and Engineering, Shandong University, Qingdao 266237, China; School of Water Conservancy and Environment, University of Jinan, Jinan 250022, China.

出版信息

J Environ Sci (China). 2025 Sep;155:673-685. doi: 10.1016/j.jes.2024.11.028. Epub 2024 Dec 4.

Abstract

The optical absorption of large molecular compounds HULIS (humic-like substances) can significantly impact the aerosol light absorption and radiative forcing, influencing cloud condensation nuclei formation and thus the climate and atmospheric environment. This study collected aerosol (PM) samples from the summit of Mount Tai in North China to investigate the concentration, molecular composition, and optical properties of HULIS. The average concentration of HULIS in the PM in this study was 1.26 ± 0.54 µg/m, comprising for 56 % of the water-soluble organic carbon (WSOC), with levels lower than urban areas but higher than other mountainous regions. Mass spectrometry revealed that CHO and CHON components, with high aromaticity and phenolic groups, are major contributors to absorption and fluorescence. These results indicate that HULIS is mainly composed of lignin and proteins/amino sugars, derived from combustion and secondary formation, and possesses a high light absorption capacity (with MAE (mass absorption efficiency) and AAE (Ångström exponent) indices of 0.62 m/g and 4.99, respectively). Parallel factor analysis identified three fluorescence components of HULIS, with proportions of 60.8 % for less oxygen humic-like substances, 21.0 % for high oxygen humic-like substances, and 18.2 % for protein-like substances. Our study highlights the significance of the light-absorbing capacity and secondary formation of HULIS at Mount Tai, laying the groundwork for investigation into the climate effects, formation mechanisms, and sources of HULIS generation.

摘要

大分子化合物类腐殖质(HULIS)的光吸收会显著影响气溶胶的光吸收和辐射强迫,进而影响云凝结核的形成,从而对气候和大气环境产生影响。本研究采集了中国北方泰山山顶的气溶胶(PM)样本,以调查HULIS的浓度、分子组成和光学特性。本研究中PM中HULIS的平均浓度为1.26±0.54µg/m,占水溶性有机碳(WSOC)的56%,其水平低于城市地区,但高于其他山区。质谱分析表明,具有高芳香性和酚基的CHO和CHON成分是吸收和荧光的主要贡献者。这些结果表明,HULIS主要由木质素和蛋白质/氨基糖组成,来源于燃烧和二次形成,并且具有高光吸收能力(质量吸收效率(MAE)和埃斯特朗指数(AAE)分别为0.62 m/g和4.99)。平行因子分析确定了HULIS的三种荧光成分,其中低氧类腐殖质占60.8%,高氧类腐殖质占21.0%,类蛋白质物质占18.2%。我们的研究突出了泰山HULIS的光吸收能力和二次形成的重要性,为研究HULIS的气候效应、形成机制和产生来源奠定了基础。

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