Metal-organic-framework derived Co-Pd bond is preferred over Fe-Pd for reductive upgrading of furfural to tetrahydrofurfuryl alcohol.
Metal-organic-framework derived Co-Pd bond is preferred over Fe-Pd for reductive upgrading of furfural to tetrahydrofurfuryl alcohol.
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DOI：
10.1039/c9dt01190k
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发表时间：
2019-06
影响因子：
4
通讯作者：
Saikiran Pendem;S. Bolla;D. Morgan;D. Shinde;Z. Lai;L. Nakka;J. Mondal
中科院分区：
文献类型：
--
作者：
Saikiran Pendem;S. Bolla;D. Morgan;D. Shinde;Z. Lai;L. Nakka;J. Mondal
结合贵过渡金属催化剂已被用于从生物质衍生的糠醛（作为平台分子）生产各种重要的非石油基化学品，并且由于对可持续和清洁燃料的迫切需求而引起了巨大的研究兴趣。在此，我们报告了钯改性的金属有机骨架（MOF）辅助制备的PdCo 3 O 4和PdFe 3 O 4纳米粒子封装在石墨N掺杂碳（NC）矩阵通过简易的原位Therapy。这为生物质衍生的糠醛（FA）的还原升级提供了具有上级催化活性的选择性变化。在优化的反应条件下，PdCo3O4@NC催化剂在糠醛加氢反应中表现出高效的催化性能，糠醛转化率达到100%，四氢糠醇（THFAL）收率达到95%。相比之下，所合成的Pd-Fe 3 O 4 @NC提供了70%的THFAL产率后，8小时的反应与四个连续的循环测试。基于不同的表征数据（XPS，H2-TPR）的纳米杂化物，我们可以得出结论，PdCo-Nx活性位的存在下，和Co 3 O 4和Pd（ii），Co 3 O 4和Pd 0之间的多重协同效应，以及在碳质基质中的N的存在下，负责上级催化活性和改善的催化剂稳定性。我们的策略提供了一个简单的设计和合成过程中的贵过渡金属合金作为一个上级生物质精炼，强大的催化剂，通过贵金属改性的MOFs作为前体。
Combined noble-transition metal catalysts have been used to produce a wide range of important non-petroleum-based chemicals from biomass-derived furfural (as a platform molecule) and have garnered colossal research interest due to the urgent demand for sustainable and clean fuels. Herein, we report the palladium-modified metal-organic-framework (MOF) assisted preparation of PdCo3O4 and PdFe3O4 nanoparticles encapsulated in a graphitic N-doped carbon (NC) matrix via facile in situ thermolysis. This provides a change in selectivity with superior catalytic activity for the reductive upgrading of biomass-derived furfural (FA). Under the optimized reaction conditions, the newly designed PdCo3O4@NC catalyst exhibited highly efficient catalytic performance in the hydrogenation of furfural, providing 100% furfural conversion with 95% yield of tetrahydrofurfuryl alcohol (THFAL). In contrast, the as-synthesized Pd-Fe3O4@NC afforded a THFAL yield of 70% after an 8 h reaction with four consecutive recycling tests. Based on different characterization data (XPS, H2-TPR) for nanohybrids, we can conclude that the presence of PdCo-Nx active sites, and the multiple synergistic effects between Co3O4 and Pd(ii), Co3O4 and Pd0, as well as the presence of N in the carbonaceous matrix, are responsible for the superior catalytic activity and improved catalyst stability. Our strategy provides a facile design and synthesis process for a noble-transition metal alloy as a superior biomass refining, robust catalyst via noble metal modified MOFs as precursors.