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Electrical Oligomerization of Small Hydrocarbons Activated by Collision with High Energy Electrons at Ambient Conditions
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2020-11-03 , DOI: 10.1021/acssuschemeng.0c05954
Kunpeng Wang 1 , David Staack 1
Affiliation  

Isomerization and polymerization are two essential chemical processes that produce valuable chemicals and high quality fuels. However, they hardly occur at ambient conditions due to the activation energy barrier of multiple chemical reactions. Thermal activation of those reactions by catalysts or high temperature and pressure or both are very costly and emits a vast amount of greenhouse gases (GHG). Here, we show a greener method that uses electricity and high energy electrons to efficiently activate small molecules at ambient conditions. Activated fragments and radicals cross-link and produce larger and more valuable compounds without use of any catalysts. One small hydrocarbon (C5H12) was irradiated by a high energy electron beam at the liquid state. About 5% conversion, iso-paraffin (85%) and n-paraffin (15%), in a C6–C15 range was observed using 400 kJ/kg energy input (0.8% of pentane’s energy content). We propose that collisions between high energy electrons and small molecules at the liquid state create radicals very efficiently by nonselective cleavage of carbon–carbon and carbon–hydrogen bonds. Radicals then undergo random pairing reactions and selectively produce large branched species. The energy cost of this method is comparable with thermal methods. This method is electrical and easily adaptable to renewable energy sources with potentially zero GHG emissions.

中文翻译:

在环境条件下与高能电子碰撞活化的小烃的电低聚

异构化和聚合是生产有价值的化学物质和高质量燃料的两个基本化学过程。然而,由于多种化学反应的活化能垒,它们在环境条件下几乎不发生。通过催化剂或高温高压或两者同时进行的这些反应的热活化非常昂贵,并且会散发大量的温室气体(GHG)。在这里,我们展示了一种更环保的方法,该方法利用电和高能电子在环境条件下有效激活小分子。活化的片段和自由基交联并产生更大,更有价值的化合物,而无需使用任何催化剂。一种小烃(C 5 H 12用高能电子束在液态照射)。使用400 kJ / kg的能量输入(戊烷能量含量的0.8%),在C 6 -C 15范围内观察到约5%的转化率,异链烷烃(85%)和链烷烃(15%)。我们提出,高能电子和液态小分子之间的碰撞通过碳-碳键和碳-氢键的非选择性裂解非常有效地产生了自由基。自由基然后经历随机的配对反应并选择性地产生大的分支物种。这种方法的能源成本与热法相当。这种方法是电动的,并且很容易适应潜在的零温室气体排放的可再生能源。
更新日期:2020-11-16
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