Effect of Support Functionalization on Catalytic Direct Hydrogenation and Catalytic Transfer Hydrogenation of Muconic Acid to Adipic Acid

Catalysts Pub Date : 2024-07-19 DOI:10.3390/catal14070465
Elisa Zanella, Stefano Franchi, Narmin Jabbarli, Ilaria Barlocco, M. Stucchi, Carlo Pirola
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Abstract

The liquid-phase hydrogenation of muconic acid (MA) to produce bio-adipic acid (AdA) is a prominent environmentally friendly chemical process, that can be achieved through two distinct methodologies: catalytic direct hydrogenation using molecular hydrogen (H2), or catalytic transfer hydrogenation utilizing a hydrogen donor. In this study, both approaches were explored, with formic acid (FA) selected as the hydrogen source for the latter method. Palladium-based catalysts were chosen for these processes. Metal’s nanoparticles (NPs) were supported on high-temperature heat-treated carbon nanofibers (HHT-CNFs) due to their known ability to enhance the stability of this metal catalyst. To assess the impact of support functionalization on catalyst stability, the HHT-CNFs were further functionalized with phosphorus and oxygen to obtain HHT-P and HHT-O, respectively. In the hydrogenation reaction, catalysts supported on functionalized supports exhibited higher catalytic activity and stability compared to Pd/HHT, reaching an AdA yield of about 80% in less than 2 h in batch reactor. The hydrogen-transfer process also yielded promising results, particularly with the 1%Pd/HHT-P catalyst. This work highlights the efficacy of support functionalization in improving catalyst performance, particularly when formic acid is used as a safer and more cost-effective hydrogen donor in the hydrogen-transfer process.
载体官能化对粘多酸催化直接加氢和催化转化加氢为己二酸的影响
通过液相氢化粘多酸(MA)来生产生物己二酸(AdA)是一种突出的环境友好型化学工艺,可通过两种不同的方法实现:使用分子氢(H2)进行催化直接氢化,或利用氢供体进行催化转移氢化。本研究对这两种方法进行了探讨,并选择甲酸(FA)作为后一种方法的氢源。这些过程选择了钯基催化剂。金属纳米颗粒(NPs)被支撑在高温热处理碳纳米纤维(HHT-CNFs)上,因为众所周知,高温热处理碳纳米纤维能够增强这种金属催化剂的稳定性。为了评估支撑物官能化对催化剂稳定性的影响,对 HHT-CNF 进一步进行了磷和氧官能化,分别得到了 HHT-P 和 HHT-O。在氢化反应中,与 Pd/HHT 相比,支撑在功能化支撑物上的催化剂表现出更高的催化活性和稳定性,在间歇反应器中,不到 2 小时就能达到约 80% 的 AdA 收率。氢转移过程也取得了可喜的结果,尤其是使用 1%Pd/HHT-P 催化剂时。这项工作凸显了载体功能化在提高催化剂性能方面的功效,尤其是在氢转移过程中使用甲酸作为更安全、更经济的氢供体时。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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