Visible-light-driven coproduction of diesel precursors and hydrogen from lignocellulose-derived methylfurans
Visible-light-driven coproduction of diesel precursors and hydrogen from lignocellulose-derived methylfurans
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DOI：
10.1038/s41560-019-0403-5
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发表时间：
2019-07-01
期刊：
影响因子：
56.7
通讯作者：
Wang, Feng
中科院分区：
文献类型：
--
作者：
Luo, Nengchao;Montini, Tiziano;Wang, Feng
生物质光催化制氢是一种很有前途的水分解替代方案，这要归功于氧化半反应更容易，并且能够同时生产太阳能燃料和增值化学品。在这里，我们展示了从木质纤维素衍生的甲基呋喃通过无受体的双极性C-C偶联，使用Ru掺杂的ZnIn 2S 4催化剂和可见光驱动的共同生产H-2和柴油燃料前体。用这种化学方法，以高于96%的选择性产生高达1.04 g g（催化剂）（-1）h（-1）的柴油燃料前体（类似于其中41%是支链烷烃的前体），以及6.0 mmol g（催化剂）（-1）h（-1）的H-2。随后的加氢脱氧反应产生包含直链和支链烷烃的所需柴油燃料。我们建议，Ru掺杂剂，取代在ZnIn 2S 4矩阵中的铟离子的位置，提高电荷分离效率，从而加速C-H活化的共同生产的H-2和柴油燃料前体。
Photocatalytic hydrogen production from biomass is a promising alternative to water splitting thanks to the oxidation half-reaction being more facile and its ability to simultaneously produce solar fuels and value-added chemicals. Here, we demonstrate the coproduction of H-2 and diesel fuel precursors from lignocellulose-derived methylfurans via acceptorless dehydrogenative C-C coupling, using a Ru-doped ZnIn2S4 catalyst and driven by visible light. With this chemistry, up to 1.04 g g(catalyst)(-1)h(-1) of diesel fuel precursors (similar to 41% of which are precursors of branched-chain alkanes) are produced with selectivity higher than 96%, together with 6.0 mmol g(catalyst)(-1) h(-1) of H-2. Subsequent hydrodeoxygenation reactions yield the desired diesel fuels comprising straight- and branched-chain alkanes. We suggest that Ru dopants, substituted in the position of indium ions in the ZnIn2S4 matrix, improve charge separation efficiency, thereby accelerating C-H activation for the coproduction of H-2 and diesel fuel precursors.