High-flux alkane production from bio-derived fatty acid decarboxylation enabled by photothermal conversion effect

IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Fuel Processing Technology Pub Date : 2024-03-08 DOI:10.1016/j.fuproc.2024.108072
Chunlin Hao , Bin Li , Guibao Guo , Shengli An
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Abstract

Heating is the most straightforward means to achieve rapid, high-throughput production for thermal catalytic reactions, but photocatalysis reactions rarely use it because its intrinsic driving force depends on the effective separation of photogenerated charges, which generally shows little or sometimes negative dependence on temperature. Here we demonstrate that the heat generated by the photothermal conversion of Bi2O3 nanoparticles can be utilized to dramatically accelerate the photocatalytic decarboxylation of long-chain fatty acids to Cn-1 n-alkanes. Using high-boiling solvents to maximize reaction temperatures, Cn-1 n-alkane can therefore be obtained in very high concentrations (e.g., ∼0.5 M) in a single operation, 5 orders of magnitude higher than the previous both semiconductor photocatalytic and algal photoenzyme transformations limited in the range ∼ 1–102 μM. Comprehensive characterizations unveil that the heat from incident light enables the standing C-chain at low temperature down onto the surface of catalyst, which allows the photoinduced hole/electron to readily approach and react with the more strained C-COO bonds. This study manifests that the vast majority of incident light energy can be utilized in the form of heat to improve the reaction efficiency to as meet industrial output levels as possible.

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利用光热转换效应从生物衍生脂肪酸脱羧反应中生产高通量烷烃
加热是实现热催化反应快速、高通量生产的最直接手段,但光催化反应却很少使用加热,因为其内在驱动力取决于光生电荷的有效分离,而电荷的有效分离通常与温度关系不大,有时甚至呈负相关。在这里,我们证明了 Bi2O3 纳米粒子光热转换产生的热量可用于显著加速长链脂肪酸到 Cn-1 正构烷烃的光催化脱羧反应。利用高沸点溶剂最大限度地提高反应温度,可在一次操作中获得极高浓度(如 ∼ 0.5 M)的 Cn-1 正烷烃,比之前局限在 ∼ 1-102 μM 范围内的半导体光催化和藻类光酶转化高出 5 个数量级。全面的特性分析表明,入射光产生的热量能使低温下静止的 C 链下降到催化剂表面,从而使光诱导的空穴/电子容易接近并与更紧张的 C-COO- 键发生反应。这项研究表明,绝大部分入射光能可以热能形式加以利用,从而提高反应效率,尽可能达到工业产出水平。
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来源期刊
Fuel Processing Technology
Fuel Processing Technology 工程技术-工程:化工
CiteScore
13.20
自引率
9.30%
发文量
398
审稿时长
26 days
期刊介绍: Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.
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