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采用单颗粒分析法研究上海大气中铁质颗粒的来源与混合态。

Source and mixing state of iron-containing particles in Shanghai by individual particle analysis.

机构信息

State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China; Graduate University of Chinese Academy of Sciences, Beijing 100049, PR China.

出版信息

Chemosphere. 2014 Jan;95:9-16. doi: 10.1016/j.chemosphere.2013.04.046. Epub 2013 May 26.

Abstract

Bioavailable iron (Fe) is an essential nutrient that can control oceanic productivity, thereby impacting the global carbon budget and climate. Therefore it is of vital importance to identify chemical species and mixing state of Fe-containing particles in the air, which are demonstrated to pose substantial impact on bioavailability of Fe. Using a single particle aerosol mass spectrometer (SPAMS), ~2,000,000 individual particles with mass spectra were collected in Shanghai for nearly 22d during the winter of 2011. Number fraction of Fe-containing particles (NfFe) varied in a wide range (<1-15%) throughout the measurement. Fe-containing particles were mainly clustered into four chemical groups, comprising of Fe-rich, K-rich, Dust and V-containing particle types. Analysis of mass spectra and mixing state suggests that Fe-containing particles correspond to various sources in Shanghai, especially anthropogenic sources iron/steel industrial activities, and fly ashes from both biomass burning and coal combustion, accounting for ~55% and ~18%, respectively. However, invasion of dust from northern desert areas is suspected to be more responsible for the spikes of NfFe (>10%), when Dust particle type contributed to >50% of Fe-containing particles. It is also revealed that Fe-containing particles were internally mixed with secondary species (e.g., sulfate and nitrate). Anthropogenic K-rich and Fe-rich particles tended to associate with both sulfate and nitrate, and thus might lead to more fraction of soluble Fe, compared to Dust particles. These results imply that atmospheric processing of Fe-containing particles from various sources might vary and thus would change the bioavailability of atmospheric Fe.

摘要

可利用铁(Fe)是一种必需的营养物质,它可以控制海洋生产力,从而影响全球碳预算和气候。因此,确定空气中含铁颗粒的化学物质和混合状态至关重要,这已被证明对 Fe 的可利用性有重大影响。利用单颗粒气溶胶质谱仪(SPAMS),在 2011 年冬季的近 22 天内,我们在上海收集了约 200 万个具有质谱的单个颗粒。含 Fe 颗粒的数分数(NfFe)在整个测量过程中变化范围很广(<1-15%)。含 Fe 颗粒主要分为四个化学组,包括富 Fe、富 K、尘埃和含 V 颗粒类型。对质谱和混合状态的分析表明,含 Fe 颗粒对应于上海的各种来源,特别是人为源钢铁工业活动和生物质燃烧和煤燃烧的飞灰,分别占约 55%和 18%。然而,来自北方沙漠地区的沙尘入侵可能更导致 NfFe(>10%)的飙升,此时尘埃颗粒类型占含 Fe 颗粒的>50%。研究还表明,含 Fe 颗粒与二次物质(如硫酸盐和硝酸盐)内部混合。人为富 K 和富 Fe 颗粒往往与硫酸盐和硝酸盐结合,因此与尘埃颗粒相比,可能导致更多的可溶性 Fe 分率。这些结果表明,来自各种来源的含 Fe 颗粒的大气处理可能会有所不同,从而改变大气 Fe 的生物利用度。

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