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Enhanced photocatalytic alkane production from fatty acid decarboxylation via inhibition of radical oligomerization
Nature Catalysis ( IF 37.8 ) Pub Date : 2020-02-19 , DOI: 10.1038/s41929-020-0423-3
Zhipeng Huang , Zhitong Zhao , Chaofeng Zhang , Jianmin Lu , Huifang Liu , Nengchao Luo , Jian Zhang , Feng Wang

The decarboxylation of bio-derived fatty acids provides a sustainable pathway for the production of alkane products under mild conditions; however, products are generally obtained in low selectivity due to the uncontrollable reactivity of radical intermediates. Here we demonstrate that photogenerated radicals can be rapidly terminated by surface hydrogen species during photocatalytic decarboxylation of fatty acids on a hydrogen-rich surface that is constructed by the interactions between H2 and Pt/TiO2 catalyst, thereby greatly inhibiting oligomerization; Cn1 alkanes can therefore be obtained from bio-derived C12–C18 fatty acids in high yields (≥90%) under mild conditions (30 °C, H2 pressure ≤0.2 MPa) and 365 nm light-emitting dode irradiation. Industrial low-value fatty acid mixtures (namely, soybean and tall oil fatty acids) can be transformed into alkane products in high yields (up to 95%). Our research introduces an efficient biomass-upgrading approach that is enabled by subtle control of the radical intermediate conversion on a heterogeneous surface.



中文翻译:

通过抑制自由基低聚反应增强脂肪酸脱羧反应产生的光催化烷烃

生物衍生脂肪酸的脱羧为在温和条件下生产烷烃产品提供了可持续的途径;然而,由于自由基中间体的不可控制的反应性,通常以低选择性获得产物。在这里,我们证明了在H 2和Pt / TiO 2催化剂之间的相互作用所构成的富氢表面上,脂肪酸在光催化脱羧过程中,表面氢物种可以迅速终止光生自由基,从而极大地抑制了低聚反应。因此,在温和的条件下(30°C,H),可以高产率(≥90%)从生物来源的C 12 – C 18脂肪酸获得C n1烷烃2个压力≤0.2MPa)和365 nm的发光二极管照射。工业低价值的脂肪酸混合物(即大豆和妥尔油脂肪酸)可以高产率(高达95%)转化为烷烃产品。我们的研究引入了一种有效的生物质提升方法,该方法可通过对异质表面上自由基中间转化的精细控制来实现。

更新日期:2020-02-19
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