State Key Laboratory of Fine Chemicals, Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
Faculty of Natural Sciences, Institute of Chemistry, Materials for Innovative Energy Concepts, Chemnitz University of Technology, Chemnitz 09107, Germany.
ACS Appl Mater Interfaces. 2023 May 17;15(19):23276-23285. doi: 10.1021/acsami.3c02810. Epub 2023 May 6.
High-entropy alloys (HEAs), as new heterogeneous catalytic materials, possess remarkable catalytic performance in numerous reactions. However, rational and controllable synthesis of these complex structures remains a challenge. In this work, bulk and carbon nanotube (CNT)-supported ultrasmall PtFeCoNiCu HEA nanoparticles with an average particle size of 1.58 nm are prepared by lithium naphthalenide-driven reduction under mild conditions. The supported PtFeCoNiCu/CNT catalyst exhibits high catalytic activity in the aqueous-phase hydrogenation of maleic anhydride to succinic acid with a selectivity of 98% at full conversion of maleic acid (the hydrolysis product of maleic anhydride), a low apparent activation energy ( = 49 kJ mol), and excellent stability. Moreover, a much higher mass-specific activity of Pt in the catalyst is displayed over PtFeCoNiCu/CNT (1515.4 mmol g h) than that of 5 wt % Pt/CNT (388.0 mmol g h). This work provides a strong support for HEAs as advanced heterogeneous catalysts and will be of great significance for promoting the research and application of HEAs in the field of selective hydrogenation.
高熵合金（HEAs）作为新型多相催化材料，在许多反应中表现出卓越的催化性能。然而，对这些复杂结构的合理可控合成仍然是一个挑战。在这项工作中，通过在温和条件下使用锂萘基驱动还原，制备了具有平均粒径为 1.58nm 的块状和碳纳米管（CNT）负载的超小 PtFeCoNiCu HEA 纳米颗粒。负载的 PtFeCoNiCu/CNT 催化剂在马来酸酐水相氢化制琥珀酸反应中表现出高催化活性，在马来酸（马来酸酐的水解产物）完全转化的情况下，选择性为 98%，表观活化能低（=49kJ/mol），稳定性好。此外，催化剂中 Pt 的质量比活性（PtFeCoNiCu/CNT 为 1515.4mmolgh）远高于 5wt%Pt/CNT（388.0mmolgh）。这项工作为 HEAs 作为先进的多相催化剂提供了有力支持，对于推动 HEAs 在选择性氢化领域的研究和应用具有重要意义。
