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由钙钛矿型氧化物衍生的可再生 Ni 催化剂在水相氢化中的催化行为。

The catalytic behaviour in aqueous-phase hydrogenation over a renewable Ni catalyst derived from a perovskite-type oxide.

机构信息

Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Centre for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, P. R. China.

出版信息

Dalton Trans. 2018 Dec 28;47(48):17276-17284. doi: 10.1039/c8dt03907k. Epub 2018 Nov 14.

DOI:10.1039/c8dt03907k
PMID:30427348
Abstract

Water is inevitably associated with the production of bio-derived platform molecules, but most supported metallic catalysts have poor water compatibility. Although there have been a great number of investigations regarding the hydrogenation of bio-derived unsaturated compounds in the organic phase, the reactions that proceed in water are still quite challenging. Herein, we report the synthesis of a supported nickel catalyst (Ni-LN650) by the reduction of the perovskite-type oxide LaNiO precursor at 650 °C. The derived catalyst affords attractive activity in the hydrogenation of furfural by using water as the reaction medium, in which furfural is completely converted into tetrahydrofurfuryl alcohol with the highest productivity of 289.7 mmol g h at 120 °C and 1 MPa of H within 5 h of reaction. The Ni-LN650 catalyst also exhibits good stability and renewability in a cycle test, stemming from the self-regeneration peculiarity of the perovskite-type oxide precursor. Moreover, the catalyst can also demonstrate high activity in the aqueous-phase hydrogenation of various aldehydes, alkenes and carboxylic acids in a series of experiments. Due to the merits of usability in water, the renewability and wide application scope, the Ni-LN650 catalyst can be treated as a promising candidate for the catalytic conversion of bio-derived platform molecules into high value-added fuels and chemicals.

摘要

水不可避免地与生物衍生平台分子的生产有关,但大多数支持的金属催化剂的水兼容性较差。尽管已经有大量关于在有机相中生物衍生不饱和化合物的加氢反应的研究,但在水中进行的反应仍然具有很大的挑战性。在此,我们报道了通过在 650°C 下还原钙钛矿型氧化物 LaNiO 前体制备负载型镍催化剂(Ni-LN650)。该催化剂在水作为反应介质的糠醛加氢反应中表现出很高的活性,在 120°C 和 1 MPa H 的条件下,反应 5 小时内,糠醛完全转化为四氢糠醇,最高产率为 289.7 mmol g h。Ni-LN650 催化剂在循环测试中也表现出良好的稳定性和可再生性,这源于钙钛矿型氧化物前体的自再生特性。此外,该催化剂在一系列实验中还可以在各种醛、烯烃和羧酸的水相加氢反应中表现出很高的活性。由于在水中具有可用性、可再生性和广泛的应用范围,Ni-LN650 催化剂可以被视为将生物衍生平台分子转化为高附加值燃料和化学品的有前途的候选催化剂。

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