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利用二氧化碳作为反应介质来减轻苯乙烯-丁二烯橡胶热分解过程中多环芳烃的生成。

Utilizing carbon dioxide as a reaction medium to mitigate production of polycyclic aromatic hydrocarbons from the thermal decomposition of styrene butadiene rubber.

机构信息

Department of Earth and Environmental Engineering [HKSM], Columbia University, New York, New York 10027, United States.

出版信息

Environ Sci Technol. 2012 Oct 2;46(19):10752-7. doi: 10.1021/es301933p. Epub 2012 Sep 18.

Abstract

The CO(2) cofeed impact on the pyrolysis of styrene butadiene rubber (SBR) was investigated using thermogravimetric analysis (TGA) coupled to online gas chromatography/mass spectroscopy (GC/MS). The direct comparison of the chemical species evolved from the thermal degradation of SBR in N(2) and CO(2) led to a preliminary mechanistic understanding of the formation and relationship of light hydrocarbons (C(1-4)), aromatic derivatives, and polycyclic aromatic hydrocarbons (PAHs), clarifying the role of CO(2) in the thermal degradation of SBR. The identification and quantification of over 50 major and minor chemical species from hydrogen and benzo[ghi]perylene were carried out experimentally in the temperature regime between 300 and 500 °C in N(2) and CO(2). The significant amounts of benzene derivatives from the direct bond dissociation of the backbone of SBR, induced by thermal degradation, provided favorable conditions for PAHs by the gas-phase addition reaction at a relatively low temperature compared to that with conventional fuels such as coal and petroleum-derived fuels. However, the formation of PAHs in a CO(2) atmosphere was decreased considerably (i.e., ∼50%) by the enhanced thermal cracking behavior, and the ultimate fates of these species were determined by different pathways in CO(2) and N(2) atmospheres. Consequently, this work has provided a new approach to mitigate PAHs by utilizing CO(2) as a reaction medium in thermochemical processes.

摘要

使用热重分析 (TGA) 与在线气相色谱/质谱联用 (GC/MS) 研究了 CO2 共进料对苯乙烯丁二烯橡胶 (SBR) 热解的影响。直接比较 SBR 在 N2 和 CO2 中热降解产生的化学物质,初步了解了轻烃 (C(1-4))、芳族衍生物和多环芳烃 (PAHs) 的形成和关系,阐明了 CO2 在 SBR 热降解中的作用。在 300 至 500°C 的温度范围内,在 N2 和 CO2 中进行了实验,鉴定和定量了超过 50 种主要和次要化学物质,包括氢和苯并[ghi]苝。SBR 主链的直接键断裂所产生的大量苯衍生物,通过热降解诱导,为在相对较低温度下通过气相加成反应形成 PAHs 提供了有利条件,与煤和石油衍生燃料等传统燃料相比。然而,在 CO2 气氛中,通过增强的热裂化行为,PAHs 的形成大大减少(即约 50%),这些物质的最终命运在 CO2 和 N2 气氛中通过不同途径确定。因此,这项工作为通过在热化学过程中利用 CO2 作为反应介质来减轻 PAHs 提供了一种新方法。

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