Nuclear magnetic resonance method for distinguishing carbonaceous source of carbonaceous aerosol component

文档序号:1685950 发布日期:2020-01-03 浏览:33次 中文

阅读说明:本技术 一种区分碳质气溶胶组分的碳质来源的核磁共振方法 (Nuclear magnetic resonance method for distinguishing carbonaceous source of carbonaceous aerosol component ) 是由 张向云 李军 张干 于 2019-10-15 设计创作,主要内容包括:本发明公开了一种区分碳质气溶胶组分的碳质来源的核磁共振方法。采集碳质气溶胶主要来源的生物质源气溶胶、煤炭燃烧排放气溶胶和交通排放(化石源)气溶胶样品,利用固体核磁共振分析3类典型源气溶胶碳谱,进行数据分析,将官能团分为sp3-杂化的烷基C(0-60ppm),sp2-杂化的碳100-165ppm)和氧化碳(60-100ppm+165-220ppm)三类,以这三个类别作为端元,做出三元点图;将待测碳质气溶胶组分样品测定其固体核磁共振碳谱数据,根据以上所作三元点图数据,解析三元一次方程,即可以计算出该待测碳质气溶胶组分样品中的生物质源、煤炭燃烧排放和交通排放的各碳质来源占比。本发明能够区分碳质气溶胶组分的碳质来源,为防控碳质气溶胶组分提供了有利条件。(The invention discloses a nuclear magnetic resonance method for distinguishing a carbonaceous source of a carbonaceous aerosol component. Collecting biomass source aerosol, coal combustion emission aerosol and traffic emission (fossil source) aerosol samples which are main sources of carbonaceous aerosol, analyzing a 3-class typical source aerosol carbon spectrum by utilizing solid nuclear magnetic resonance, carrying out data analysis, dividing functional groups into three classes of sp 3-hybridized alkyl C (0-60ppm), sp 2-hybridized carbon 100-165ppm) and carbon oxide (60-100ppm +165-220ppm), and taking the three classes as end members to make a ternary diagram; and (3) measuring solid nuclear magnetic resonance carbon spectrum data of the carbonaceous aerosol component sample to be measured, and analyzing a ternary linear equation according to the ternary diagram data to calculate the carbon source proportion of the biomass source, the coal combustion emission and the traffic emission in the carbonaceous aerosol component sample to be measured. The invention can distinguish the carbon source of the carbon aerosol component and provides favorable conditions for preventing and controlling the carbon aerosol component.)

1. A nuclear magnetic resonance method of discriminating a carbonaceous source of a carbonaceous aerosol component, comprising the steps of:

collecting biomass source aerosol, coal combustion emission aerosol and traffic emission (fossil source) aerosol samples which are main sources of carbonaceous aerosol, analyzing a 3-class typical source aerosol carbon spectrum by utilizing solid nuclear magnetic resonance, carrying out data analysis, dividing functional groups into three classes of sp 3-hybridized alkyl C (0-60ppm), sp 2-hybridized carbon 100-165ppm) and carbon oxide (60-100ppm +165-220ppm), and taking the three classes as end members to make a ternary diagram;

and (3) measuring solid nuclear magnetic resonance carbon spectrum data of the carbonaceous aerosol component sample to be measured, and analyzing a ternary linear equation according to the ternary diagram data to calculate the carbon source proportion of the biomass source, the coal combustion emission and the traffic emission in the carbonaceous aerosol component sample to be measured.

2. The method of claim 1, wherein the solid-state nmr is 400MHz solid-state nmr.

3. The nmr method of claim 1 or 2, wherein the biomass-derived aerosol, coal combustion emissions aerosol, and traffic emissions (fossil-derived) aerosol samples are obtained by simulation of a live event.

Technical Field

The invention belongs to the field of geochemistry, and particularly relates to a nuclear magnetic resonance method for distinguishing a carbonaceous source of a carbonaceous aerosol component.

Background

The carbonaceous aerosol component is an important chemical component in the atmospheric aerosol, and the contribution rate of the carbonaceous aerosol component in atmospheric fine particles is 10-70 percent (Lim and Turpin, 2002; Lonati et al, 2007). It has significant contribution to air pollution and dust haze, and in addition, it contains a large amount of toxic substances, can directly harm human health, and is one of the leading topics of current atmospheric chemistry research (Highwood and Kinnersley, 2006; Nel, 2005). Carbonaceous aerosols comprise thousands of organic compounds, typically including polycyclic aromatic hydrocarbons, normal alkanes, aldones, and carboxylic acids. Only 10-40% of the organics in the aerosol can be qualitatively and quantitatively determined by gas chromatography-mass spectrometry (GC-MS) (Jacobson, 2001). Thus, the overall contamination level of the carbonaceous aerosol is generally expressed in terms of the mass concentration of the carbonaceous aerosol obtained by carbon content analysis.

Carbonaceous aerosols contain thousands of compounds, the composition of the components is highly complex, so knowledge of their origin, toxicity and component characteristics remains limited (Andreae, 2009; Chen et al, 2017; Goldstein and Galbally, 2007; Hallquist et al, 2009; Laskin et al, 2015). Carbonaceous aerosols are mainly derived from biomass combustion (non-fossil source), coal combustion and traffic emissions (fossil source) etc. (Huang et al, 2014; Zhang et al, 2015 b). In recent years, analysis techniques such as Nuclear Magnetic Resonance (NMR) have been developed to greatly improve the knowledge of the components of organic carbon aerosols, but the research and the knowledge of the organic carbon of the atmospheric aerosols have been insufficient.

The phenomenon of nuclear magnetic resonance was discovered independently in 1946 by american scientists Bloch (using induction) and Purcell (using absorption). In 1953, the first nmr was successfully developed, but the initial utility was limited to the hydrogen spectrum of liquid materials. In nature12The spin quantum number of the C-nucleus is zero, a nuclear magnetic resonance signal is not observed, and an isotope with a spin quantum number of 1/2 is capable of observing an NMR signal13C, but the abundance of the C is low in nature and only accounts for 1.1 percent of the total carbon content,13the observed sensitivity of the C NMR signal was only 1/5700 for protons.13The practical application of C NMR was the first pulse since 1971Starting from the advent of the Fourier transform NMR apparatus, which by means of a computer, through Fourier transformation, can accumulate NMR signals generated by a plurality of pulses so that13The sensitivity of C NMR is greatly improved. Nuclear Magnetic Resonance (NMR) technology can determine the carbon functional group distribution information of complex organic matters, and is a powerful tool for researching the detailed structure information of complex natural organic matters in atmospheric aerosol (Zhang-Toyun et al, 2015; Duarte et al, 2005; Sannigrahi et al, 2006).

Disclosure of Invention

It is an object of the present invention to provide a nuclear magnetic resonance method capable of discriminating carbonaceous sources of carbonaceous aerosol components.

The nuclear magnetic resonance method for distinguishing the carbonaceous source of the carbonaceous aerosol component is characterized by comprising the following steps of:

collecting biomass source aerosol, coal combustion emission aerosol and traffic emission (fossil source) aerosol samples which are main sources of carbonaceous aerosol, analyzing a 3-class typical source aerosol carbon spectrum by utilizing solid nuclear magnetic resonance, carrying out data analysis, dividing functional groups into three classes of sp 3-hybridized alkyl C (0-60ppm), sp 2-hybridized carbon 100-165ppm) and carbon oxide (60-100ppm +165-220ppm), and taking the three classes as end members to make a ternary diagram;

and (3) measuring solid nuclear magnetic resonance carbon spectrum data of the carbonaceous aerosol component sample to be measured, and analyzing a ternary linear equation according to the ternary diagram data to calculate the carbon source proportion of the biomass source, the coal combustion emission and the traffic emission in the carbonaceous aerosol component sample to be measured.

Preferably, the solid nuclear magnetic resonance is 400MHz solid nuclear magnetic resonance.

Preferably, the biomass source aerosol, coal combustion emission aerosol and traffic emission (fossil source) aerosol samples are obtained by simulating a live scene.

The method can distinguish the carbon sources of the carbon aerosol components, greatly improves the knowledge of the organic carbon aerosol components, and provides favorable conditions for preventing and controlling the carbon aerosol components.

Description of the drawings:

FIG. 1 is a sample of biomass-derived aerosol, coal combustion emissions aerosol, and traffic emissions (fossil-derived) aerosol13C-NMR spectrum;

FIG. 2 is a ternary plot of typical carbonaceous aerosol NMR data;

FIG. 3 is a sample of formulation P113C-NMR spectrum;

the specific implementation mode is as follows:

the following examples are further illustrative of the present invention and are not intended to be limiting thereof.

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