氧化铌负载铱催化木质素衍生酚选择性加氢脱氧制芳烃
Selective Hydrodeoxygenation of Lignin-Derived Phenols to Aromatics Catalyzed by NbO-Supported Iridium.
作者信息
Jeantelot Gabriel, Følkner Simen P, Manegold Johanna I S, Ingebrigtsen Morten G, Jensen Vidar R, Le Roux Erwan
机构信息
Department of Chemistry, University of Bergen, Allégaten 41, N-5007 Bergen, Norway.
出版信息
ACS Omega. 2022 Aug 23;7(35):31561-31566. doi: 10.1021/acsomega.2c04314. eCollection 2022 Sep 6.
The dominating catalytic approach to aromatic hydrocarbons from renewables, deoxygenation of phenol-rich depolymerized lignin bio-oils, is hard to achieve: hydrodeoxygenation (HDO) of phenols typically leads to the loss of aromaticity and to non-negligible fractions of cyclohexanones and cyclohexanols. Here, we report a catalyst, niobia-supported iridium nanoparticles (Ir@NbO), which combines full conversion in the HDO of lignin-derived phenols with appreciable and tunable selectivity for aromatics (25-95%) under mild conditions (200-300 °C, 2.5-10 bar of H). A simple approach to the removal of Brønsted-acidic sites via Hünig's base prevents coking and allows reaction conditions ( > 225 °C, 2.5 bar of H), promoting high yields of aromatic hydrocarbons.
从可再生资源中获取芳烃的主要催化方法，即对富含苯酚的解聚木质素生物油进行脱氧，很难实现：酚类的加氢脱氧（HDO）通常会导致芳香性丧失，并产生不可忽视的环己酮和环己醇馏分。在此，我们报道了一种催化剂，即铌负载的铱纳米颗粒（Ir@NbO），它在温和条件（200 - 300 °C，2.5 - 10 bar氢气）下，能使木质素衍生酚类的HDO实现完全转化，并对芳烃具有可观且可调节的选择性（25 - 95%）。通过亨尼希碱去除布朗斯台德酸性位点的简单方法可防止结焦，并允许在更高的反应条件（> 225 °C，2.5 bar氢气）下促进芳烃的高产率。
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