A unique Co@CoO catalyst for hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran.
A unique Co@CoO catalyst for hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran.
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一种独特的Co@CoO催化剂，用于生物质衍生的5-羟甲基糠醛氢解为2,5-二甲基呋喃。
DOI：
10.1038/s41467-022-31362-9
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发表时间：
2022-06-27
影响因子：
16.6
通讯作者：
中科院分区：
文献类型：
--
作者：
开发无贵金属催化剂以促进生物质燃料和化学品的可持续生产仍然是一个重要而具有挑战性的目标。在这里，我们报道了通过一种独特的核壳结构催化剂Co@CoO将生物质衍生的5-羟甲基糠醛有效地氢解为2,5-二甲基呋喃，该催化剂在所有催化剂中，包括迄今为止报道的贵金属基催化剂，提供了最高的生产率。令人惊讶的是，我们发现催化活性位点位于含氧空位的CoO壳层上，而不是金属Co上。各种光谱实验和计算模型的结合表明，含氧空位的CoO壳层不仅驱动H2的异裂裂解，而且还驱动H2的均裂裂解，产生更活跃的Hδ−，从而产生异常的催化活性。Co@CoO对木质素模型化合物的直接加氢脱氧也表现出优异的活性。这项研究首次揭示了基于简单金属氧化物的催化剂将可再生生物质加氢脱氧为化学原料的潜力。开发无贵金属催化剂以促进生物质燃料和化学品的可持续生产具有挑战性。本文作者报道了一种独特的核壳结构Co@CoO催化剂，该催化剂在生物质衍生化合物的氢解中表现出优异的性能。
The development of precious-metal-free catalysts to promote the sustainable production of fuels and chemicals from biomass remains an important and challenging target. Here, we report the efficient hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran over a unique core-shell structured catalyst, Co@CoO that affords the highest productivity among all catalysts, including noble-metal-based catalysts, reported to date. Surprisingly, we find that the catalytically active sites reside on the shell of CoO with oxygen vacancies rather than the metallic Co. The combination of various spectroscopic experiments and computational modelling reveals that the CoO shell incorporating oxygen vacancies not only drives the heterolytic cleavage, but also the homolytic cleavage of H2 to yield more active Hδ− species, resulting in the exceptional catalytic activity. Co@CoO also exhibits excellent activity toward the direct hydrodeoxygenation of lignin model compounds. This study unlocks, for the first time, the potential of simple metal-oxide-based catalysts for the hydrodeoxygenation of renewable biomass to chemical feedstocks. The development of precious-metal-free catalysts to promote the sustainable production of fuels and chemicals from biomass challenging. Here the authors report a unique core-shell structured Co@CoO catalyst which exhibits excellent performance in the hydrogenolysis of biomass-derived compounds.
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